Articles | Volume 7, issue 6
Geosci. Model Dev., 7, 3153–3172, 2014
https://doi.org/10.5194/gmd-7-3153-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Special issue: The Modular Earth Submodel System (MESSy) (ACP/GMD inter-journal...
Geosci. Model Dev., 7, 3153–3172, 2014
https://doi.org/10.5194/gmd-7-3153-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Model description paper 21 Dec 2014
Model description paper | 21 Dec 2014
ORACLE (v1.0): module to simulate the organic aerosol composition and evolution in the atmosphere
A. P. Tsimpidi et al.
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Vlassis A. Karydis, Alexandra P. Tsimpidi, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 21, 14983–15001, https://doi.org/10.5194/acp-21-14983-2021, https://doi.org/10.5194/acp-21-14983-2021, 2021
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Aerosol particle pH is well-buffered by alkaline compounds, notably NH3 and crustal elements. NH3 is found to supply remarkable buffering capacity on a global scale, from the polluted continents to the remote oceans. Potential future changes in agricultural NH3 must be accompanied by strong reductions of SO2 and NOx to avoid particles becoming highly acidic, with implications for human health (aerosol toxicity), ecosystems (acid deposition), clouds, and climate (aerosol hygroscopicity).
Andrea Pozzer, Simon Reifenberg, Vinod Kumar, Bruno Franco, Domenico Taraborrelli, Sergy Gromov, Sebastian Ehrhart, Patrick Jöckel, Rolf Sander, Veronica Fall, Simon Rosanka, Vlassis Karydis, Dimitris Akritidis, Tamara Emmerichs, Monica Crippa, Diego Guizzardi, Johannes W. Kaiser, Lieven Clarisse, Astrid Kiendler-Scharr, Holger Tost, and Alexandra Tsimpidi
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-295, https://doi.org/10.5194/gmd-2021-295, 2021
Revised manuscript under review for GMD
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A newly developed set-up of the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) is here evaluated; a comprehensive organic degradation mechanism is used and coupled with a volatility base model. The results show that the model is reproducing most of the tracer and aerosols satisfactorily, although with discrepancies for oxygenated organic gases and that this model configuration can be used for further research in atmospheric chemistry.
Erin Evoy, Adrian M. Maclean, Grazia Rovelli, Ying Li, Alexandra P. Tsimpidi, Vlassis A. Karydis, Saeid Kamal, Jos Lelieveld, Manabu Shiraiwa, Jonathan P. Reid, and Allan K. Bertram
Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, https://doi.org/10.5194/acp-19-10073-2019, 2019
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We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Andrea Pozzer, Spyros N. Pandis, and Jos Lelieveld
Geosci. Model Dev., 11, 3369–3389, https://doi.org/10.5194/gmd-11-3369-2018, https://doi.org/10.5194/gmd-11-3369-2018, 2018
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A new module, ORACLE 2-D, that calculates the concentrations of surrogate organic species in two-dimensional space defined by volatility and oxygen-to-carbon ratio has been developed and evaluated. ORACLE 2-D uses a simple photochemical aging scheme that efficiently simulates the net effects of fragmentation and functionalization. ORACLE 2-D can be used to compute the ability of organic particles to act as cloud condensation nuclei and serves as a tool to quantify their climatic impact.
Huisheng Bian, Mian Chin, Didier A. Hauglustaine, Michael Schulz, Gunnar Myhre, Susanne E. Bauer, Marianne T. Lund, Vlassis A. Karydis, Tom L. Kucsera, Xiaohua Pan, Andrea Pozzer, Ragnhild B. Skeie, Stephen D. Steenrod, Kengo Sudo, Kostas Tsigaridis, Alexandra P. Tsimpidi, and Svetlana G. Tsyro
Atmos. Chem. Phys., 17, 12911–12940, https://doi.org/10.5194/acp-17-12911-2017, https://doi.org/10.5194/acp-17-12911-2017, 2017
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Atmospheric nitrate contributes notably to total aerosol mass in the present day and is likely to be more important over the next century, with a projected decline in SO2 and NOx emissions and increase in NH3 emissions. This paper investigates atmospheric nitrate using multiple global models and measurements. The study is part of the AeroCom phase III activity. The study is the first attempt to look at global atmospheric nitrate simulation at physical and chemical process levels.
Andrea Pozzer, Alexandra P. Tsimpidi, Vlassis A. Karydis, Alexander de Meij, and Jos Lelieveld
Atmos. Chem. Phys., 17, 12813–12826, https://doi.org/10.5194/acp-17-12813-2017, https://doi.org/10.5194/acp-17-12813-2017, 2017
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This study shows that agricultural emissions are important for air quality and their reduction can effectively reduce the concentration of fine particles and their associated premature mortality. Therefore, emission control policies, especially in North America and Europe, should also involve strong ammonia emission decreases to optimally reduce fine-particle concentration.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 7345–7364, https://doi.org/10.5194/acp-17-7345-2017, https://doi.org/10.5194/acp-17-7345-2017, 2017
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We analyzed the sensitivity of model-predicted global-scale OA to parameters and assumptions that control primary emissions, photochemical aging, and the scavenging efficiency of LVOCs, SVOCs, and IVOCs. The simulated OA concentrations were evaluated against a global dataset of AMS measurements. According to our analysis, a combination of increased IVOCs and decreased hygroscopicity of the freshly emitted IVOCs can help reduce discrepancies between simulated SOA and observed OOA concentrations.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 16, 8939–8962, https://doi.org/10.5194/acp-16-8939-2016, https://doi.org/10.5194/acp-16-8939-2016, 2016
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In this work we use a global chemistry climate model together with a comprehensive global AMS data set in order to provide valuable insights into the temporal and geographical variability of the contribution of the emitted particles and the chemically processed organic material from combustion sources to total OA. This study reveals the high importance of SOA from anthropogenic sources on global OA concentrations and identifies plausible sources of discrepancy between models and measurements.
V. A. Karydis, A. P. Tsimpidi, A. Pozzer, M. Astitha, and J. Lelieveld
Atmos. Chem. Phys., 16, 1491–1509, https://doi.org/10.5194/acp-16-1491-2016, https://doi.org/10.5194/acp-16-1491-2016, 2016
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We provide an assessment of the chemical composition and global aerosol load of aerosol nitrate and determine the effect of mineral dust on its formation due to thermodynamical interactions. For this purpose we used an explicit geographical representation of the emitted soil particle size distribution and chemical composition. We conclude mineral dust aerosol chemistry is important for nitrate aerosol formation and significantly affects its global distribution, especially in the coarse mode.
Ovid Oktavian Krüger, Bruna A. Holanda, Sourangsu Chowdhury, Andrea Pozzer, David Walter, Christopher Pöhlker, Maria Dolores Andrés Hernández, John Phillip Burrows, Christiane Voigt, Jos Lelieveld, Johannes Quaas, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1100, https://doi.org/10.5194/acp-2021-1100, 2022
Preprint under review for ACP
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The abrupt reduction in human activities during the first COVID-19 lockdown created unprecedented atmospheric conditions. We took the opportunity to quantify changes in black carbon (BC) as a major anthropogenic air pollutant. Therefore, we measured BC onboard a research aircraft over Europe during the lockdown and compared the results to measurements from 2017. With model simulations we account for different weather conditions and find a lockdown-related decrease in BC of 40 %.
Guangjie Zheng, Hang Su, Siwen Wang, Andrea Pozzer, and Yafang Cheng
Atmos. Chem. Phys., 22, 47–63, https://doi.org/10.5194/acp-22-47-2022, https://doi.org/10.5194/acp-22-47-2022, 2022
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The recently proposed multiphase buffer theory provides a framework to reconstruct long-term trends and spatial variations in aerosol pH, while non-ideality is a major limitation for its broad applications. Here we proposed a parameterization method to estimate the impact of non-ideality and validated it against long-term observations and global simulations. With this method, the multiphase buffer theory can reproduce well aerosol pH variations estimated by comprehensive thermodynamic models.
Dimitris Akritidis, Andrea Pozzer, Johannes Flemming, Antje Inness, Philippe Nédélec, and Prodromos Zanis
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-998, https://doi.org/10.5194/acp-2021-998, 2021
Preprint under review for ACP
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We perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 over Europe, using WOUDC (World Ozone and Ultraviolet Radiation Data Centre) ozonesondes and IAGOS (In-service Aircraft for a Global Observing System) aircraft measurements. Chemical data assimilation assists CAMSRA to reproduce the observed O3 increases in the troposphere during the examined folding events, yet it mostly results in O3 overestimation in the upper troposphere.
Clara M. Nussbaumer, Andrea Pozzer, Ivan Tadic, Lenard Röder, Florian Obersteiner, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1028, https://doi.org/10.5194/acp-2021-1028, 2021
Preprint under review for ACP
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The European COVID-19 lockdowns have significantly reduced the emission of primary pollutants such as NOx which impacts the tropospheric photochemical processes and the abundance of O3. In this study, we present how the lockdowns have affected tropospheric trace gases and ozone production based on in situ observations and modeling simulations. We additionally show that the chemical regime shifted from a transition point to a NOx limitation in the upper troposphere.
Clara M. Nussbaumer, John N. Crowley, Jan Schuladen, Jonathan Williams, Sascha Hafermann, Andreas Reiffs, Raoul Axinte, Hartwig Harder, Cheryl Ernest, Anna Novelli, Katrin Sala, Monica Martinez, Chinmay Mallik, Laura Tomsche, Christian Plass-Dülmer, Birger Bohn, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 18413–18432, https://doi.org/10.5194/acp-21-18413-2021, https://doi.org/10.5194/acp-21-18413-2021, 2021
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HCHO is an important atmospheric trace gas influencing the photochemical processes in the Earth’s atmosphere, including the budget of HOx and the abundance of tropospheric O3. This research presents the photochemical calculations of HCHO and O3 based on three field campaigns across Europe. We show that HCHO production via the oxidation of only four volatile organic compound precursors, i.e., CH4, CH3CHO, C5H8 and CH3OH, can balance the observed loss at all sites well.
Simon Felix Reifenberg, Anna Martin, Matthias Kohl, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna Holanda, Ovid O. Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1005, https://doi.org/10.5194/acp-2021-1005, 2021
Preprint under review for ACP
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissionsare located in the upper troposphere, around the aircraft cruise altitude, while largest absolute changes are present at the surface.
Dirk Dienhart, John N. Crowley, Efstratios Bourtsoukidis, Achim Edtbauer, Philipp G. Eger, Lisa Ernle, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Eva Y. Pfannerstill, Roland Rohloff, Jan Schuladen, Christof Stönner, Ivan Tadic, Sebastian Tauer, Nijing Wang, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 17373–17388, https://doi.org/10.5194/acp-21-17373-2021, https://doi.org/10.5194/acp-21-17373-2021, 2021
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We present the first ship-based in situ measurements of formaldehyde (HCHO), hydroxyl radicals (OH) and the OH reactivity around the Arabian Peninsula. Regression analysis of the HCHO production rate and the related OH chemistry revealed the regional HCHO yield αeff, which represents the different chemical regimes encountered. Highest values were found for the Arabian Gulf (also known as the Persian Gulf), which highlights this region as a hotspot of photochemical air pollution.
Ksakousti Skyllakou, Pablo Garcia Rivera, Brian Dinkelacker, Eleni Karnezi, Ioannis Kioutsioukis, Carlos Hernandez, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 17115–17132, https://doi.org/10.5194/acp-21-17115-2021, https://doi.org/10.5194/acp-21-17115-2021, 2021
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Significant reductions in pollutant emissions took place in the US from 1990 to 2010. The reductions in sulfur dioxide emissions from electric-generating units have dominated the reductions in fine particle mass. The reductions in transportation emissions have led to a 30 % reduction of elemental concentrations and of organic particulate matter by a factor of 3. On the other hand, changes in biomass burning and biogenic secondary organic aerosol have been modest.
Clara M. Nussbaumer, Uwe Parchatka, Ivan Tadic, Birger Bohn, Daniel Marno, Monica Martinez, Roland Rohloff, Hartwig Harder, Flora Kluge, Klaus Pfeilsticker, Florian Obersteiner, Martin Zöger, Raphael Doerich, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 14, 6759–6776, https://doi.org/10.5194/amt-14-6759-2021, https://doi.org/10.5194/amt-14-6759-2021, 2021
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NO2 plays a central role in atmospheric photochemical processes and requires accurate measurements. This research presents NO2 data obtained via chemiluminescence using a photolytic converter from airborne studies around Cabo Verde and laboratory investigations. We show the limits and error-proneness of a conventional blue light converter in aircraft measurements affected by humidity and NO levels and suggest the use of an alternative quartz converter for more reliable results.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 21, 14983–15001, https://doi.org/10.5194/acp-21-14983-2021, https://doi.org/10.5194/acp-21-14983-2021, 2021
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Aerosol particle pH is well-buffered by alkaline compounds, notably NH3 and crustal elements. NH3 is found to supply remarkable buffering capacity on a global scale, from the polluted continents to the remote oceans. Potential future changes in agricultural NH3 must be accompanied by strong reductions of SO2 and NOx to avoid particles becoming highly acidic, with implications for human health (aerosol toxicity), ecosystems (acid deposition), clouds, and climate (aerosol hygroscopicity).
Spiro D. Jorga, Kalliopi Florou, Christos Kaltsonoudis, John K. Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 15337–15349, https://doi.org/10.5194/acp-21-15337-2021, https://doi.org/10.5194/acp-21-15337-2021, 2021
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We test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through the oxidation of the emitted organic vapors by the nitrate radicals produced during the reaction of ozone and nitrogen oxides. Our experiments, using as a starting point the ambient air of an urban area with high biomass burning activity, demonstrate that, even with sunlight, there is 20 %–70 % additional organic aerosol formed in a few hours.
Andrea Pozzer
Geosci. Commun., 4, 453–460, https://doi.org/10.5194/gc-4-453-2021, https://doi.org/10.5194/gc-4-453-2021, 2021
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In this paper we investigate the numbers of pages, references and references per page in open-access EGU journals. We showed that, while the number of references and number of pages have been constantly increasing in the period 2010–2020, the number of references per page did not change in the same period. Furthermore, all the journals showed a similar number of references per page, i.e. ~ 3.8 references per page.
Andrea Pozzer, Simon Reifenberg, Vinod Kumar, Bruno Franco, Domenico Taraborrelli, Sergy Gromov, Sebastian Ehrhart, Patrick Jöckel, Rolf Sander, Veronica Fall, Simon Rosanka, Vlassis Karydis, Dimitris Akritidis, Tamara Emmerichs, Monica Crippa, Diego Guizzardi, Johannes W. Kaiser, Lieven Clarisse, Astrid Kiendler-Scharr, Holger Tost, and Alexandra Tsimpidi
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-295, https://doi.org/10.5194/gmd-2021-295, 2021
Revised manuscript under review for GMD
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A newly developed set-up of the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) is here evaluated; a comprehensive organic degradation mechanism is used and coupled with a volatility base model. The results show that the model is reproducing most of the tracer and aerosols satisfactorily, although with discrepancies for oxygenated organic gases and that this model configuration can be used for further research in atmospheric chemistry.
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
Aristeidis Voliotis, Yu Wang, Yunqi Shao, Mao Du, Thomas J. Bannan, Carl J. Percival, Spyros N. Pandis, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 14251–14273, https://doi.org/10.5194/acp-21-14251-2021, https://doi.org/10.5194/acp-21-14251-2021, 2021
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Secondary organic aerosol (SOA) formation from mixtures of volatile precursors can be affected by the molecular interactions of the products. Composition and volatility measurements of SOA formed from mixtures of anthropogenic and biogenic precursors reveal processes that can increase or decrease the SOA volatility. The unique products of the mixture were more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
Mengze Li, Andrea Pozzer, Jos Lelieveld, and Jonathan Williams
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2021-246, https://doi.org/10.5194/essd-2021-246, 2021
Preprint under review for ESSD
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We present a global airborne measurement dataset of atmospheric ethane, propane and methane and temporal trends for the time period 2006-2016 in the UTLS. The Copernicus CAMS-GLOB ethane emission inventory coupled with atmospheric model EMAC was optimized by the observational data with 12 ethane sectoral emission sources distinguished. The global ethane emission budget is estimated to be 19.28 Tg/yr for 2006–2016.
Jean-Daniel Paris, Aurélie Riandet, Efstratios Bourtsoukidis, Marc Delmotte, Antoine Berchet, Jonathan Williams, Lisa Ernle, Ivan Tadic, Hartwig Harder, and Jos Lelieveld
Atmos. Chem. Phys., 21, 12443–12462, https://doi.org/10.5194/acp-21-12443-2021, https://doi.org/10.5194/acp-21-12443-2021, 2021
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We measured atmospheric methane and CO2 by ship in the Middle East. We probe the origin of methane with a combination of light alkane measurements and modeling. We find strong influence from nearby oil and gas production over the Arabian Gulf. Comparing our data to inventories indicates that inventories overestimate sources from the upstream gas industry but underestimate emissions from oil extraction and processing. The Red Sea was under a complex mixture of sources due to human activity.
Jennifer Schallock, Christoph Brühl, Christine Bingen, Michael Höpfner, Landon Rieger, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-654, https://doi.org/10.5194/acp-2021-654, 2021
Preprint under review for ACP
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This paper presents model simulations of stratospheric aerosols with a focus on explosive volcanic eruptions. Using occulation and limb-based satellite instruments with vertical profiles of sulfur dioxide and aerosol extinction, we characterised the influence of volcanic aerosols for the period between 1990–2019. We established a volcanic sulfur emission inventory that includes more than 500 eruptions. Our results show that also smaller eruptions can contribute to the stratospheric aerosol layer.
Patrick Dewald, Raphael Dörich, Jan Schuladen, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5501–5519, https://doi.org/10.5194/amt-14-5501-2021, https://doi.org/10.5194/amt-14-5501-2021, 2021
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Organic nitrates generated from the reaction between isoprene and the nitrate radical (ISOP-NITs) were detected via their thermal dissociation in heated quartz inlets to nitrogen dioxide monitored by cavity ring-down spectroscopy. The temperature-dependent dissociation profiles of ISOP-NITs in the presence of ozone (O3) are broad in contrast to narrow profiles of common reference compounds. We demonstrate that this broadening is caused by O3-assisted reactions of ISOP-NITs on quartz surfaces.
David Patoulias and Spyros N. Pandis
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-655, https://doi.org/10.5194/acp-2021-655, 2021
Revised manuscript accepted for ACP
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Our simulations indicate that the recently identified production and subsequent condensation effect of extremely low volatility organic compounds has a smaller than expected effect on the total concentration of atmospheric particles. On the other hand, the oxidation of intermediate volatility organic compounds leads to decreases of the ultrafine particle concentrations. These results improve our understanding of the links between secondary organic aerosol formation and ultrafine particles.
Raphael Dörich, Philipp Eger, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5319–5332, https://doi.org/10.5194/amt-14-5319-2021, https://doi.org/10.5194/amt-14-5319-2021, 2021
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We demonstrate in laboratory experiments that the formation of IOx anions (formed in reactions of I− with O3) or acetate anions (formed e.g. by the reaction of I− with peracetic acid) results in unexpected sensitivity of an iodide chemical ionisation mass spectrometer (I-CIMS) to HNO3 at a mass-to-charge ratio of 62. This helps explain observations of apparent high daytime levels of N2O5. Airborne measurements using I-CIMS confirm these conclusions.
Pablo Garcia Rivera, Brian T. Dinkelacker, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-568, https://doi.org/10.5194/acp-2021-568, 2021
Revised manuscript accepted for ACP
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The contribution of various pollution sources to the variability of fine PM in an urban area was examined using as an example the city of Pittsburgh. Biomass burning aerosol shows the largest variability during the winter with local maxima within the city and in the suburbs. During both periods the largest contributing source to the average PM2.5 is particles from outside the modeling domain. The average population weighted PM2.5 concentration does not change significantly with resolution.
Vinod Kumar, Julia Remmers, Steffen Beirle, Joachim Fallmann, Astrid Kerkweg, Jos Lelieveld, Mariano Mertens, Andrea Pozzer, Benedikt Steil, Marc Barra, Holger Tost, and Thomas Wagner
Atmos. Meas. Tech., 14, 5241–5269, https://doi.org/10.5194/amt-14-5241-2021, https://doi.org/10.5194/amt-14-5241-2021, 2021
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We present high-resolution regional atmospheric chemistry model simulations focused around Germany. We highlight the importance of spatial resolution of the model itself as well as the input emissions inventory and short-scale temporal variability of emissions for simulations. We propose a consistent approach for evaluating the simulated vertical distribution of NO2 using MAX-DOAS measurements while also considering its spatial sensitivity volume and change in sensitivity within this volume.
Simon Rosanka, Bruno Franco, Lieven Clarisse, Pierre-François Coheur, Andrea Pozzer, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 11257–11288, https://doi.org/10.5194/acp-21-11257-2021, https://doi.org/10.5194/acp-21-11257-2021, 2021
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The strong El Niño in 2015 led to a particular dry season in Indonesia and favoured severe peatland fires. The smouldering conditions of these fires and the high carbon content of peat resulted in high volatile organic compound (VOC) emissions. By using a comprehensive atmospheric model, we show that these emissions have a significant impact on the tropospheric composition and oxidation capacity. These emissions are transported into to the lower stratosphere, resulting in a depletion of ozone.
Miska Olin, David Patoulias, Heino Kuuluvainen, Jarkko V. Niemi, Topi Rönkkö, Spyros N. Pandis, Ilona Riipinen, and Miikka Dal Maso
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-466, https://doi.org/10.5194/acp-2021-466, 2021
Revised manuscript accepted for ACP
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An emission factor particle size distribution was determined from the measurements at an urban traffic site. It was used in updating a pre-existing emission inventory and regional modelling was performed after the update. Emission inventories typically underestimate nanoparticle emissions due to challenges in determining them with high certainty. This update reveals that the simulated aerosol levels have previously been underestimated especially for urban areas and for sub-50 nm-sized particles.
Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev., 14, 4429–4441, https://doi.org/10.5194/gmd-14-4429-2021, https://doi.org/10.5194/gmd-14-4429-2021, 2021
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Soil moisture is of great importance for weather and climate. We present a machine learning model that produces accurate predictions of satellite-observed surface soil moisture, based on meteorological data from a climate model. It can be used as soil moisture parametrisation in climate models and to produce comprehensive global soil moisture datasets. Moreover, it may motivate similar applications of machine learning in climate science.
Tamara Emmerichs, Bruno Franco, Catherine Wespes, Vinod Kumar, Andrea Pozzer, Simon Rosanka, and Domenico Taraborrelli
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-584, https://doi.org/10.5194/acp-2021-584, 2021
Revised manuscript not accepted
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Near-surface ozone is a harmful air pollutant and it is strongly affected by radical reactions and surface-atmosphere exchanges which in turn are modulated, directly and indirectly, by weather. Understanding the impact of weather on ozone, and air quality, is thus important also in view of weather extremes. The inclusion of additional ozone-weather links in the global model yields a 2-fold reduction of the ozone bias towards satellite observations.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
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Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
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Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
Nils Friedrich, Philipp Eger, Justin Shenolikar, Nicolas Sobanski, Jan Schuladen, Dirk Dienhart, Bettina Hottmann, Ivan Tadic, Horst Fischer, Monica Martinez, Roland Rohloff, Sebastian Tauer, Hartwig Harder, Eva Y. Pfannerstill, Nijing Wang, Jonathan Williams, James Brooks, Frank Drewnick, Hang Su, Guo Li, Yafang Cheng, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 21, 7473–7498, https://doi.org/10.5194/acp-21-7473-2021, https://doi.org/10.5194/acp-21-7473-2021, 2021
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This paper uses NOx and NOz measurements from the 2017 AQABA ship campaign in the Mediterranean Sea and around the Arabian Peninsula to examine the influence e.g. of emissions from shipping and oil and gas production. Night-time losses of NOx dominated in the Arabian Gulf and in the Red Sea, whereas daytime losses were more important in the Mediterranean Sea. Nitric acid and organic nitrates were the most prevalent components of NOz.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
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Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Georgia N. Theodoritsi, Giancarlo Ciarelli, and Spyros N. Pandis
Geosci. Model Dev., 14, 2041–2055, https://doi.org/10.5194/gmd-14-2041-2021, https://doi.org/10.5194/gmd-14-2041-2021, 2021
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Two schemes based on the volatility basis set were used for the simulation of biomass burning organic aerosol (bbOA) in the continental US. The first is the default scheme of the PMCAMx-SR model, and the second is a recently developed scheme based on laboratory experiments. The alternative bbOA scheme predicts much higher concentrations. The default scheme performed better during summer and fall, while the alternative scheme was a little better during spring.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Jaydeep Singh, Narendra Singh, Narendra Ojha, Amit Sharma, Andrea Pozzer, Nadimpally Kiran Kumar, Kunjukrishnapillai Rajeev, Sachin S. Gunthe, and V. Rao Kotamarthi
Geosci. Model Dev., 14, 1427–1443, https://doi.org/10.5194/gmd-14-1427-2021, https://doi.org/10.5194/gmd-14-1427-2021, 2021
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Atmospheric models often have limitations in simulating the geographically complex and climatically important central Himalayan region. In this direction, we have performed regional modeling at high resolutions to improve the simulation of meteorology and dynamics through a better representation of the topography. The study has implications for further model applications to investigate the effects of anthropogenic pressure over the Himalaya.
Chaim I. Garfinkel, Ohad Harari, Shlomi Ziskin Ziv, Jian Rao, Olaf Morgenstern, Guang Zeng, Simone Tilmes, Douglas Kinnison, Fiona M. O'Connor, Neal Butchart, Makoto Deushi, Patrick Jöckel, Andrea Pozzer, and Sean Davis
Atmos. Chem. Phys., 21, 3725–3740, https://doi.org/10.5194/acp-21-3725-2021, https://doi.org/10.5194/acp-21-3725-2021, 2021
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Water vapor is the dominant greenhouse gas in the atmosphere, and El Niño is the dominant mode of variability in the ocean–atmosphere system. The connection between El Niño and water vapor above ~ 17 km is unclear, with single-model studies reaching a range of conclusions. This study examines this connection in 12 different models. While there are substantial differences among the models, all models appear to capture the fundamental physical processes correctly.
Einar Karu, Mengze Li, Lisa Ernle, Carl A. M. Brenninkmeijer, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 14, 1817–1831, https://doi.org/10.5194/amt-14-1817-2021, https://doi.org/10.5194/amt-14-1817-2021, 2021
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A gas measurement device was developed to measure trace gases (ppt level) in the air based on an atomic emission detector. It combines a cryogenic pre-concentrator (CryoTrap), a gas chromatograph (GC), and a new high-resolution atomic emission detector (AED). The CryoTrap–GC–AED instrumental setup, limits of detection, and elemental performance are presented and discussed. Two measurement case studies are reported: one in a Finnish boreal forest and the other based on an aircraft campaign.
Domenico Taraborrelli, David Cabrera-Perez, Sara Bacer, Sergey Gromov, Jos Lelieveld, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 21, 2615–2636, https://doi.org/10.5194/acp-21-2615-2021, https://doi.org/10.5194/acp-21-2615-2021, 2021
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Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as ozone precursors. Monocyclic aromatics are no exception. Calculations with a comprehensive atmospheric model are consistent with this view but only for air masses close to pollution source regions. However, the same model predicts that aromatics, when transported to remote areas, may effectively destroy ozone. This loss of tropospheric ozone rivals the one attributed to bromine.
Sara Bacer, Sylvia C. Sullivan, Odran Sourdeval, Holger Tost, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 21, 1485–1505, https://doi.org/10.5194/acp-21-1485-2021, https://doi.org/10.5194/acp-21-1485-2021, 2021
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We investigate the relative importance of the rates of both microphysical processes and unphysical correction terms that act as sources or sinks of ice crystals in cold clouds. By means of numerical simulations performed with a global chemistry–climate model, we assess the relevance of these rates at global and regional scales. This estimation is of fundamental importance to assign priority to the development of microphysics parameterizations and compare model output with observations.
Stylianos Kakavas, David Patoulias, Maria Zakoura, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 799–811, https://doi.org/10.5194/acp-21-799-2021, https://doi.org/10.5194/acp-21-799-2021, 2021
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The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles in northern and southern Europe. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 pH units decrease over 2.5 km). The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol.
Klaus Klingmüller, Vlassis A. Karydis, Sara Bacer, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 20, 15285–15295, https://doi.org/10.5194/acp-20-15285-2020, https://doi.org/10.5194/acp-20-15285-2020, 2020
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Particulate air pollution cools the climate and partially masks the greenhouse warming by reflecting sunlight and enhancing the reflection by clouds. The intensity of this cooling depends on interactions between pollution and desert dust within the atmosphere. Our simulations with a global atmospheric chemistry-climate model indicate that these interactions significantly weaken the cooling.
Matias Berasategui, Damien Amedro, Luc Vereecken, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 13541–13555, https://doi.org/10.5194/acp-20-13541-2020, https://doi.org/10.5194/acp-20-13541-2020, 2020
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Peracetic acid is one of the most abundant organic peroxides in the atmosphere. We combine experiments and theory to show that peracetic acid reacts orders of magnitude more slowly with OH than presently accepted, which results in a significant extension of its atmospheric lifetime.
Bettina Hottmann, Sascha Hafermann, Laura Tomsche, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Marco Neumaier, Andreas Zahn, Birger Bohn, Greta Stratmann, Helmut Ziereis, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 12655–12673, https://doi.org/10.5194/acp-20-12655-2020, https://doi.org/10.5194/acp-20-12655-2020, 2020
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During OMO we observed enhanced mixing ratios of hydroperoxides (ROOH) in the Asian monsoon anticyclone (AMA) relative to the background. The observed mixing ratios are higher than steady-state calculations and EMAC simulations, especially in the AMA, indicating atmospheric transport of ROOH. Uncertainties in the scavenging efficiencies likely cause deviations from EMAC. Longitudinal gradients indicate a pool of ROOH towards the center of the AMA associated with upwind convection over India.
Nils Friedrich, Ivan Tadic, Jan Schuladen, James Brooks, Eoghan Darbyshire, Frank Drewnick, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 13, 5739–5761, https://doi.org/10.5194/amt-13-5739-2020, https://doi.org/10.5194/amt-13-5739-2020, 2020
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We present a new instrument for the measurement of NOx and NOy based on a combination of the thermal dissociation of NOy to NOx and cavity ring-down spectroscopic detection of NO2. It features a denuder to separate the contributions of gas-phase and particulate nitrates to NOy. We provide a detailed characterization of the instrument and briefly outline results from first deployments.
Antonios Tasoglou, Evangelos Louvaris, Kalliopi Florou, Aikaterini Liangou, Eleni Karnezi, Christos Kaltsonoudis, Ningxin Wang, and Spyros N. Pandis
Atmos. Chem. Phys., 20, 11625–11637, https://doi.org/10.5194/acp-20-11625-2020, https://doi.org/10.5194/acp-20-11625-2020, 2020
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A month-long set of summertime measurements in a remote area in the Mediterranean is used to quantify aerosol absorption. The measured light absorption was two or more times higher than that of fresh black carbon. The absorption enhancement due to the coating of black carbon cores by other aerosol components could explain only part of this absorption enhancement. The rest was due to brown carbon, mostly in the form of extremely low volatility organic compounds.
Nijing Wang, Achim Edtbauer, Christof Stönner, Andrea Pozzer, Efstratios Bourtsoukidis, Lisa Ernle, Dirk Dienhart, Bettina Hottmann, Horst Fischer, Jan Schuladen, John N. Crowley, Jean-Daniel Paris, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 10807–10829, https://doi.org/10.5194/acp-20-10807-2020, https://doi.org/10.5194/acp-20-10807-2020, 2020
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Carbonyl compounds were measured on a ship travelling around the Arabian Peninsula in summer 2017, crossing both highly polluted and extremely clean regions of the marine boundary layer. We investigated the sources and sinks of carbonyls. The results from a global model showed a significant model underestimation for acetaldehyde, a molecule that can influence regional air chemistry. By adding a diurnal oceanic source, the model estimation was highly improved.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Ivan Tadic, John N. Crowley, Dirk Dienhart, Philipp Eger, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Justin Shenolikar, Sebastian Tauer, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 6769–6787, https://doi.org/10.5194/acp-20-6769-2020, https://doi.org/10.5194/acp-20-6769-2020, 2020
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We present shipborne observations of NO, NO2, O3, HCHO, OH, HO2, H2O and the actinic flux obtained in the marine boundary layer (MBL) around the Arabian Peninsula during the summer 2017 AQABA ship campaign. NOx (NO+NO2) and O3 observations clearly showed anthropogenic influence in the MBL around the Arabian Peninsula. The observations were also used to calculate net O3 production in the MBL around the Arabian Peninsula, which was greatest over the northern Red Sea, Oman Gulf and Arabian Gulf.
Daniel Marno, Cheryl Ernest, Korbinian Hens, Umar Javed, Thomas Klimach, Monica Martinez, Markus Rudolf, Jos Lelieveld, and Hartwig Harder
Atmos. Meas. Tech., 13, 2711–2731, https://doi.org/10.5194/amt-13-2711-2020, https://doi.org/10.5194/amt-13-2711-2020, 2020
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In this study, a calibration device for OH and HO2 instruments is characterized at pressures of 275 to 1000 mbar, allowing instrument pressure sensitivity to be quantified to an accuracy of 22 % (1σ). Computational fluid dynamic simulations supporting the understanding of interactions between generated HOx and the instrument inlet led to enhanced determination of factors affecting instrument sensitivity.
Achim Edtbauer, Christof Stönner, Eva Y. Pfannerstill, Matias Berasategui, David Walter, John N. Crowley, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 6081–6094, https://doi.org/10.5194/acp-20-6081-2020, https://doi.org/10.5194/acp-20-6081-2020, 2020
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Marine regions where deep nutrient-rich water is pushed towards the surface are called upwelling regions. In these nutrient-rich waters large algal blooms form which are the basis of the marine food web. We measured methane sulfonamide, a molecule containing sulfur and nitrogen, for the first time in ambient air and could show that the origin of this emission is an algal bloom near the Somalia upwelling. Sulfur-containing compounds from algae can promote particle formation over the oceans.
Peter H. Zimmermann, Carl A. M. Brenninkmeijer, Andrea Pozzer, Patrick Jöckel, Franziska Winterstein, Andreas Zahn, Sander Houweling, and Jos Lelieveld
Atmos. Chem. Phys., 20, 5787–5809, https://doi.org/10.5194/acp-20-5787-2020, https://doi.org/10.5194/acp-20-5787-2020, 2020
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The atmospheric abundance of the greenhouse gas methane is determined by interacting emission sources and sinks in a dynamic global environment. In this study, its global budget from 1997 to 2016 is simulated with a general circulation model using emission estimates of 11 source categories. The model results are evaluated against 17 ground station and 320 intercontinental flight observation series. Deviations are used to re-scale the emission quantities with the aim of matching observations.
Philipp G. Eger, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Matthieu Riva, Qiaozhi Zha, Mikael Ehn, Lauriane L. J. Quéléver, Simon Schallhart, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 3697–3711, https://doi.org/10.5194/acp-20-3697-2020, https://doi.org/10.5194/acp-20-3697-2020, 2020
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Pyruvic acid, CH3C(O)C(O)OH, is an organic acid of biogenic origin that plays a crucial role in plant metabolism, is present in tropospheric air in both gas-phase and aerosol-phase, and is implicated in the formation of secondary organic aerosols. From the first gas-phase measurements of pyruvic acid in the Finnish boreal forest in September 2016 we derive its source strength and discuss potential sources and sinks, with a focus on the relevance of gas-phase pyruvic acid for radical chemistry.
Matthew Forrest, Holger Tost, Jos Lelieveld, and Thomas Hickler
Geosci. Model Dev., 13, 1285–1309, https://doi.org/10.5194/gmd-13-1285-2020, https://doi.org/10.5194/gmd-13-1285-2020, 2020
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We have integrated the LPJ-GUESS dynamic global vegetation model into the EMAC atmospheric chemistry-enabled GCM (general circulation model). This combined framework will enable the investigation of many land–atmosphere interactions and feedbacks with state-of-the-art simulation models. Initial results show that using the climate produced by EMAC together with LPJ-GUESS produces an acceptable representation of the global vegetation.
Athanasios Nenes, Spyros N. Pandis, Rodney J. Weber, and Armistead Russell
Atmos. Chem. Phys., 20, 3249–3258, https://doi.org/10.5194/acp-20-3249-2020, https://doi.org/10.5194/acp-20-3249-2020, 2020
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We show that aerosol acidity (pH) and liquid water content naturally emerge as previously ignored parameters that drive particulate matter formation in the atmosphere, and its sensitivity to emissions of ammonia and nitric acid. The simple framework presented is easily applied to ambient measurements or model output, and it provides the
chemical regimeof PM sensitivity to ammonia and nitric acid availability.
Damien Amedro, Matias Berasategui, Arne J. C. Bunkan, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 3091–3105, https://doi.org/10.5194/acp-20-3091-2020, https://doi.org/10.5194/acp-20-3091-2020, 2020
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Our laboratory experiments show that the rate coefficient for the termolecular reaction between OH and NO2 is enhanced in the presence of water vapour. Using a chemistry transport model we show that our new parameterization of the temperature, pressure, and bath-gas dependence of this reaction has a significant impact on, for example, NOx and the HNO2 / NO2 ratio when compared to present recommendations.
Matias Berasategui, Damien Amedro, Achim Edtbauer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 2695–2707, https://doi.org/10.5194/acp-20-2695-2020, https://doi.org/10.5194/acp-20-2695-2020, 2020
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We have determined the rate coefficient and mechanism for the reaction of the OH radical with methane sulphonamide, a trace gas which has recently been found in the atmosphere. The rate coefficient is 1.4 × 10−13 cm3 molec.−1 s−1, which indicates a tropospheric lifetime of > 2 months. The observation of CO, CO2, SO2, HNO3, HCOOH, and N2O products enabled us to derive a detailed reaction mechanism for the reaction, which proceeds predominantly by H abstraction from the CH3 group.
Julie M. Nicely, Bryan N. Duncan, Thomas F. Hanisco, Glenn M. Wolfe, Ross J. Salawitch, Makoto Deushi, Amund S. Haslerud, Patrick Jöckel, Béatrice Josse, Douglas E. Kinnison, Andrew Klekociuk, Michael E. Manyin, Virginie Marécal, Olaf Morgenstern, Lee T. Murray, Gunnar Myhre, Luke D. Oman, Giovanni Pitari, Andrea Pozzer, Ilaria Quaglia, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Kane Stone, Susan Strahan, Simone Tilmes, Holger Tost, Daniel M. Westervelt, and Guang Zeng
Atmos. Chem. Phys., 20, 1341–1361, https://doi.org/10.5194/acp-20-1341-2020, https://doi.org/10.5194/acp-20-1341-2020, 2020
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Differences in methane lifetime among global models are large and poorly understood. We use a neural network method and simulations from the Chemistry Climate Model Initiative to quantify the factors influencing methane lifetime spread among models and variations over time. UV photolysis, tropospheric ozone, and nitrogen oxides drive large model differences, while the same factors plus specific humidity contribute to a decreasing trend in methane lifetime between 1980 and 2015.
Ying Chen, Yafang Cheng, Nan Ma, Chao Wei, Liang Ran, Ralf Wolke, Johannes Größ, Qiaoqiao Wang, Andrea Pozzer, Hugo A. C. Denier van der Gon, Gerald Spindler, Jos Lelieveld, Ina Tegen, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 20, 771–786, https://doi.org/10.5194/acp-20-771-2020, https://doi.org/10.5194/acp-20-771-2020, 2020
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Particulate nitrate is one of the most important climate cooling agents. Our results show that interaction with sea-salt aerosol can shift nitrate to larger sized particles (redistribution effect), weakening its direct cooling effect. The modelling results indicate strong redistribution over coastal and offshore regions worldwide as well as continental Europe. Improving the consideration of the redistribution effect in global models fosters a better understanding of climate change.
Dimitris Akritidis, Andrea Pozzer, and Prodromos Zanis
Atmos. Chem. Phys., 19, 14387–14401, https://doi.org/10.5194/acp-19-14387-2019, https://doi.org/10.5194/acp-19-14387-2019, 2019
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We investigate the impact of future climate change under the RCP6.0 scenario on tropopause folds and tropospheric ozone, using a transient EMAC simulation and a tropopause fold detection algorithm. A strengthening of ozone stratosphere-to-troposphere transport (STT) is projected for the future, resulting in an increase in upper- and middle-tropospheric ozone. The maxima of future ozone STT increases are mainly projected for regions where tropopause folds are expected to occur more frequently.
Philipp G. Eger, Nils Friedrich, Jan Schuladen, Justin Shenolikar, Horst Fischer, Ivan Tadic, Hartwig Harder, Monica Martinez, Roland Rohloff, Sebastian Tauer, Frank Drewnick, Friederike Fachinger, James Brooks, Eoghan Darbyshire, Jean Sciare, Michael Pikridas, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 12121–12140, https://doi.org/10.5194/acp-19-12121-2019, https://doi.org/10.5194/acp-19-12121-2019, 2019
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Shipborne measurements of nitryl chloride (ClNO2) were made during the AQABA (Air Quality and climate change in the Arabian BAsin) ship campaign in summer 2017. The dataset includes measurements over the Mediterranean Sea and around the Arabian Peninsula with observed mixing ratios ranging from the limit of detection to 600 pptv. We examined the regional variability in the generation of ClNO2 and its importance for Cl atom generation in a marine boundary layer influenced by ships and industry.
Horst Fischer, Raoul Axinte, Heiko Bozem, John N. Crowley, Cheryl Ernest, Stefan Gilge, Sascha Hafermann, Hartwig Harder, Korbinian Hens, Ruud H. H. Janssen, Rainer Königstedt, Dagmar Kubistin, Chinmay Mallik, Monica Martinez, Anna Novelli, Uwe Parchatka, Christian Plass-Dülmer, Andrea Pozzer, Eric Regelin, Andreas Reiffs, Torsten Schmidt, Jan Schuladen, and Jos Lelieveld
Atmos. Chem. Phys., 19, 11953–11968, https://doi.org/10.5194/acp-19-11953-2019, https://doi.org/10.5194/acp-19-11953-2019, 2019
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We use in situ observations of H2O2 to study the interplay between photochemistry, transport and deposition processes. The data were obtained during five ground-based field campaigns across Europe. A budget calculation indicates that the photochemical production rate was much larger than photochemical loss and that dry deposition is the dominant loss process. To reproduce the change in H2O2 mixing ratios after sunrise, a variable contribution of entrainment from the residual layer is required.
Matthias Kippenberger, Gerhard Schuster, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 11939–11951, https://doi.org/10.5194/acp-19-11939-2019, https://doi.org/10.5194/acp-19-11939-2019, 2019
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We investigated the uptake of several trace gases to growing ice surfaces at temperatures relevant to cirrus clouds. HCl, a strong inorganic acid that ionises at the surface, was efficiently trapped in the growing ice, whereas oxidised organic trace gases, which attach to ice by hydrogen bonding, were not. HCl can be efficiently and rapidly removed from the gas phase in supersaturated ice clouds.
Jianzhong Ma, Christoph Brühl, Qianshan He, Benedikt Steil, Vlassis A. Karydis, Klaus Klingmüller, Holger Tost, Bin Chen, Yufang Jin, Ningwei Liu, Xiangde Xu, Peng Yan, Xiuji Zhou, Kamal Abdelrahman, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 19, 11587–11612, https://doi.org/10.5194/acp-19-11587-2019, https://doi.org/10.5194/acp-19-11587-2019, 2019
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We find a pronounced maximum in aerosol extinction in the upper troposphere and lower stratosphere over the Tibetan Plateau during the Asian summer monsoon, caused mainly by mineral dust emitted from the northern Tibetan Plateau and slope area, lofted to and accumulating within the anticyclonic circulation. Mineral dust, water-soluble compounds, such as nitrate and sulfate, and associated liquid water dominate aerosol extinction around the tropopause within the Asian summer monsoon anticyclone.
Eva Y. Pfannerstill, Nijing Wang, Achim Edtbauer, Efstratios Bourtsoukidis, John N. Crowley, Dirk Dienhart, Philipp G. Eger, Lisa Ernle, Horst Fischer, Bettina Hottmann, Jean-Daniel Paris, Christof Stönner, Ivan Tadic, David Walter, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 19, 11501–11523, https://doi.org/10.5194/acp-19-11501-2019, https://doi.org/10.5194/acp-19-11501-2019, 2019
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The Arabian Peninsula is a global hot spot of ozone pollution. Our measurements, made on a ship in summer 2017, indicate underlying reasons. Despite being at sea, we observed ozone-forming reactive trace gases (measured as so-called total OH reactivity) comparable to highly populated urban regions in amount and composition. This is due to strong emissions from oil extraction and ship traffic. These emissions were quickly converted to ozone due to intense solar irradiation and high temperatures.
Jonathan Liebmann, Nicolas Sobanski, Jan Schuladen, Einar Karu, Heidi Hellén, Hannele Hakola, Qiaozhi Zha, Mikael Ehn, Matthieu Riva, Liine Heikkinen, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 10391–10403, https://doi.org/10.5194/acp-19-10391-2019, https://doi.org/10.5194/acp-19-10391-2019, 2019
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The formation of alkyl nitrates in the boreal forest was dominated by reactions of the NO3 radical with terpenes, both during the day and the night, with fewer contributions from OH and ozone. The alkyl nitrates formed had lifetimes on the order of 2 h, reflecting efficient loss via uptake to aerosol and deposition.
Weiqi Xu, Conghui Xie, Eleni Karnezi, Qi Zhang, Junfeng Wang, Spyros N. Pandis, Xinlei Ge, Jingwei Zhang, Junling An, Qingqing Wang, Jian Zhao, Wei Du, Yanmei Qiu, Wei Zhou, Yao He, Ying Li, Jie Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 19, 10205–10216, https://doi.org/10.5194/acp-19-10205-2019, https://doi.org/10.5194/acp-19-10205-2019, 2019
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We present the first aerosol volatility measurements in Beijing in summer using a thermodenuder coupled with aerosol mass spectrometers. Our results showed that organic aerosol (OA) comprised mainly semi-volatile organic compounds in summer, and the freshly oxidized secondary OA was the most volatile component. We also found quite different volatility distributions in black-carbon-containing primary and secondary OA, ambient OA, ambient secondary OA and the WRF-Chem model.
Erin Evoy, Adrian M. Maclean, Grazia Rovelli, Ying Li, Alexandra P. Tsimpidi, Vlassis A. Karydis, Saeid Kamal, Jos Lelieveld, Manabu Shiraiwa, Jonathan P. Reid, and Allan K. Bertram
Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, https://doi.org/10.5194/acp-19-10073-2019, 2019
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We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
Ohad Harari, Chaim I. Garfinkel, Shlomi Ziskin Ziv, Olaf Morgenstern, Guang Zeng, Simone Tilmes, Douglas Kinnison, Makoto Deushi, Patrick Jöckel, Andrea Pozzer, Fiona M. O'Connor, and Sean Davis
Atmos. Chem. Phys., 19, 9253–9268, https://doi.org/10.5194/acp-19-9253-2019, https://doi.org/10.5194/acp-19-9253-2019, 2019
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Ozone depletion in the Antarctic has been shown to influence surface conditions, but the effects of ozone depletion in the Arctic on surface climate are unclear. We show that Arctic ozone does influence surface climate in both polar regions and tropical regions, though the proximate cause of these surface impacts is not yet clear.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Klaus Klingmüller, Jos Lelieveld, Vlassis A. Karydis, and Georgiy L. Stenchikov
Atmos. Chem. Phys., 19, 7397–7408, https://doi.org/10.5194/acp-19-7397-2019, https://doi.org/10.5194/acp-19-7397-2019, 2019
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Within the atmosphere, desert dust and anthropogenic pollution are mixed and interact, which affects the abundance and optical properties of the particulate matter. This results in an anthropogenic climate forcing associated with mineral dust notwithstanding the natural origin of most aeolian dust. With a global chemistry–climate model, we estimate this forcing to represent a considerable fraction of the total dust forcing.
Efstratios Bourtsoukidis, Lisa Ernle, John N. Crowley, Jos Lelieveld, Jean-Daniel Paris, Andrea Pozzer, David Walter, and Jonathan Williams
Atmos. Chem. Phys., 19, 7209–7232, https://doi.org/10.5194/acp-19-7209-2019, https://doi.org/10.5194/acp-19-7209-2019, 2019
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We report on results that demonstrate the utility of non-methane hydrocarbons as source/sink identification tracers while providing their mixing ratios around the Arabian Peninsula. By introducing novel data-analysis approaches, we establish a new method for separating associated and non-associated (with liquids) gases. We formulate a relationship between hydrocarbon oxidative pairs that can be used to evaluate the relative abundance of the hydroxyl and chlorine radicals in the troposphere.
Christos Kaltsonoudis, Spiro D. Jorga, Evangelos Louvaris, Kalliopi Florou, and Spyros N. Pandis
Atmos. Meas. Tech., 12, 2733–2743, https://doi.org/10.5194/amt-12-2733-2019, https://doi.org/10.5194/amt-12-2733-2019, 2019
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A portable dual-smog-chamber system was developed using two identical pillow-shaped smog chambers surrounded by UV lamps. The system has been designed to use ambient air as the starting point of the experiments. It can be easily disassembled and transported, enabling the study of various atmospheric environments and it can be used with natural sunlight. The results of test experiments using ambient air are discussed as examples of applications of this system.
Vincent Huijnen, Andrea Pozzer, Joaquim Arteta, Guy Brasseur, Idir Bouarar, Simon Chabrillat, Yves Christophe, Thierno Doumbia, Johannes Flemming, Jonathan Guth, Béatrice Josse, Vlassis A. Karydis, Virginie Marécal, and Sophie Pelletier
Geosci. Model Dev., 12, 1725–1752, https://doi.org/10.5194/gmd-12-1725-2019, https://doi.org/10.5194/gmd-12-1725-2019, 2019
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We report on an evaluation of tropospheric ozone and its precursor gases in three atmospheric chemistry versions as implemented in ECMWF’s Integrated Forecasting System (IFS), referred to as IFS(CB05BASCOE), IFS(MOZART) and IFS(MOCAGE). This configuration of having various chemistry versions within IFS provides a quantification of uncertainties in CAMS trace gas products that are induced by chemistry modelling.
Katerina S. Karadima, Vlasis G. Mavrantzas, and Spyros N. Pandis
Atmos. Chem. Phys., 19, 5571–5587, https://doi.org/10.5194/acp-19-5571-2019, https://doi.org/10.5194/acp-19-5571-2019, 2019
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We explore the morphologies of multicomponent nanoparticles through atomistic molecular dynamics simulations under atmospherically relevant conditions. Phase separation is predicted for almost all simulated nanoparticles either between organics and inorganics or between hydrophobic and hydrophilic constituents. Three main particle types were identified: organic islands at the surface, inorganic core-organic shell morphologies and complex structures with hydrophobic and hydrophilic domains.
Georgia N. Theodoritsi and Spyros N. Pandis
Atmos. Chem. Phys., 19, 5403–5415, https://doi.org/10.5194/acp-19-5403-2019, https://doi.org/10.5194/acp-19-5403-2019, 2019
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The chemical transport model PMCAMx was extended to investigate the effects of partitioning and photochemical aging of biomass burning emissions on organic aerosol (OA) concentrations and was applied in Europe. During the summer, the contribution of biomass burning to total OA levels over continental Europe was 16 % and during winter 47 %. Intermediate volatility organic compounds are predicted to be important precursors of secondary OA from biomass burning.
Meryem Tanarhte, Sara Bacer, Susannah M. Burrows, J. Alex Huffman, Kyle M. Pierce, Andrea Pozzer, Roland Sarda-Estève, Nicole J. Savage, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-251, https://doi.org/10.5194/acp-2019-251, 2019
Publication in ACP not foreseen
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Bioaerosols have been an important topic in atmospheric science in the last two decades. This paper compares different emission parametrizations used in fungal spores modeling and compare their results to two sets of new observational datasets. It emphasises their uncertainties in order to improve their modeling in the future. This comparison is addressed primarily to the scientific community (publishing in ACP) interested in this type of modeling and the related experimental work in this field.
Rolf Sander, Andreas Baumgaertner, David Cabrera-Perez, Franziska Frank, Sergey Gromov, Jens-Uwe Grooß, Hartwig Harder, Vincent Huijnen, Patrick Jöckel, Vlassis A. Karydis, Kyle E. Niemeyer, Andrea Pozzer, Hella Riede, Martin G. Schultz, Domenico Taraborrelli, and Sebastian Tauer
Geosci. Model Dev., 12, 1365–1385, https://doi.org/10.5194/gmd-12-1365-2019, https://doi.org/10.5194/gmd-12-1365-2019, 2019
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We present the atmospheric chemistry box model CAABA/MECCA which
now includes a number of new features: skeletal mechanism
reduction, the MOM chemical mechanism for volatile organic
compounds, an option to include reactions from the Master
Chemical Mechanism (MCM) and other chemical mechanisms, updated
isotope tagging, improved and new photolysis modules, and the new
feature of coexisting multiple chemistry mechanisms.
CAABA/MECCA is a community model published under the GPL.
Philipp G. Eger, Frank Helleis, Gerhard Schuster, Gavin J. Phillips, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 12, 1935–1954, https://doi.org/10.5194/amt-12-1935-2019, https://doi.org/10.5194/amt-12-1935-2019, 2019
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We present a chemical ionization quadrupole mass spectrometer (CI-QMS) with a novel discharge ion source. In addition to the expected detection of PAN, peracetic acid and ClNO2, the instrument is also sensitive to SO2, HCl and acetic acid through ion chemistry unique for our ion source. We present ionization schemes along with illustrative datasets from field campaigns underlining the potential of the CI-QMS as an alternative to polonium, especially for application in the marine boundary layer.
Laura Tomsche, Andrea Pozzer, Narendra Ojha, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 19, 1915–1939, https://doi.org/10.5194/acp-19-1915-2019, https://doi.org/10.5194/acp-19-1915-2019, 2019
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The Asian monsoon anticyclone (AMA) is an annual phenomenon in the northern hemispheric upper troposphere (UT) and lower stratosphere. We performed in situ measurements of carbon monoxide (CO) and methane (CH4) in the monsoon outflow region and in background air in the UT (Mediterranean, Arabian Peninsula, Arabian Sea) using airborne optical absorption spectroscopy during the Oxidation Mechanism Observations mission (summer 2015). The trace gases increased within the AMA, particularly CH4.
Anthoula D. Drosatou, Ksakousti Skyllakou, Georgia N. Theodoritsi, and Spyros N. Pandis
Atmos. Chem. Phys., 19, 973–986, https://doi.org/10.5194/acp-19-973-2019, https://doi.org/10.5194/acp-19-973-2019, 2019
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The ability of positive matrix factorization (PMF) factor analysis to identify and quantify the organic aerosol (OA) sources accurately is tested in this modeling study. The estimated uncertainty of the contribution of fresh biomass burning is less than 30 % and of the other primary sources is less than 40 %, when these sources contribute more than 20 % to the OA. Τhe first oxygenated OA factor includes mainly highly aged OA, while the second oxygenated OA factor contains fresher secondary OA.
Yingying Yan, David Cabrera-Perez, Jintai Lin, Andrea Pozzer, Lu Hu, Dylan B. Millet, William C. Porter, and Jos Lelieveld
Geosci. Model Dev., 12, 111–130, https://doi.org/10.5194/gmd-12-111-2019, https://doi.org/10.5194/gmd-12-111-2019, 2019
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The GEOS-Chem model has been updated with the SAPRC-11 aromatics chemical mechanism to evaluate global and regional effects of aromatics on tropospheric oxidation capacity. Our results reveal relatively slight changes in ozone, hydroxyl radical, and nitrogen oxides on a global mean basis (1–4 %), although remarkable regional differences (5–20 %) exist near the source regions. Improved representation of aromatics is important to simulate the tropospheric oxidation.
Ningxin Wang, Spiro D. Jorga, Jeffery R. Pierce, Neil M. Donahue, and Spyros N. Pandis
Atmos. Meas. Tech., 11, 6577–6588, https://doi.org/10.5194/amt-11-6577-2018, https://doi.org/10.5194/amt-11-6577-2018, 2018
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The interaction of particles with the chamber walls has been a significant source of uncertainty when analyzing results of secondary organic aerosol formation experiments performed in Teflon chambers. We evaluated the performance of several particle wall-loss correction methods for aging experiments of α-pinene ozonolysis products. Experimental procedures are proposed for the characterization of particle losses during different stages of these experiments.
Sebastian Ehrhart, Eimear M. Dunne, Hanna E. Manninen, Tuomo Nieminen, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4987–5001, https://doi.org/10.5194/gmd-11-4987-2018, https://doi.org/10.5194/gmd-11-4987-2018, 2018
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
David Patoulias, Christos Fountoukis, Ilona Riipinen, Ari Asmi, Markku Kulmala, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 13639–13654, https://doi.org/10.5194/acp-18-13639-2018, https://doi.org/10.5194/acp-18-13639-2018, 2018
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PMCAMx-UF, a 3-D chemical transport model focusing on the simulation of ultrafine particles, has been extended with the addition of the volatility basis set (VBS) approach for the simulation of organic aerosol. The model was applied in Europe and its predictions were evaluated against field observations collected during the PEGASOS 2012 campaign. The condensation of organics led to an increase (50–120 %) in the larger particles but the total number concentration decreased by 10–30 %.
John N. Crowley, Nicolas Pouvesle, Gavin J. Phillips, Raoul Axinte, Horst Fischer, Tuukka Petäjä, Anke Nölscher, Jonathan Williams, Korbinian Hens, Hartwig Harder, Monica Martinez-Harder, Anna Novelli, Dagmar Kubistin, Birger Bohn, and Jos Lelieveld
Atmos. Chem. Phys., 18, 13457–13479, https://doi.org/10.5194/acp-18-13457-2018, https://doi.org/10.5194/acp-18-13457-2018, 2018
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Simultaneous observations of PAA, PAN and H2O2 are used to provide insight into processes influencing the HOx chemistry of the boreal forest, including two biomass-burning-impacted periods. A significant contribution from photolytic HOx sources was included in a box model analysis to align model predictions with measurements. The model predicts high levels of organic peroxy radicals, also at night-time.
Jonathan M. Liebmann, Jennifer B. A. Muller, Dagmar Kubistin, Anja Claude, Robert Holla, Christian Plass-Dülmer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 12045–12059, https://doi.org/10.5194/acp-18-12045-2018, https://doi.org/10.5194/acp-18-12045-2018, 2018
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We present direct measurements of the summertime total reactivity (inverse lifetime) of NO3 towards organic trace gases at a rural mountain site. High daytime and low night-time values were found. The reactivity was dominated by reaction with monoterpenes and sufficiently high to compete with photolysis and reaction with NO during daytime. NO3 radical measurements from one night are presented. For the first time, direct measurements of OH and NO3 reactivity are compared.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Andrea Pozzer, Spyros N. Pandis, and Jos Lelieveld
Geosci. Model Dev., 11, 3369–3389, https://doi.org/10.5194/gmd-11-3369-2018, https://doi.org/10.5194/gmd-11-3369-2018, 2018
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A new module, ORACLE 2-D, that calculates the concentrations of surrogate organic species in two-dimensional space defined by volatility and oxygen-to-carbon ratio has been developed and evaluated. ORACLE 2-D uses a simple photochemical aging scheme that efficiently simulates the net effects of fragmentation and functionalization. ORACLE 2-D can be used to compute the ability of organic particles to act as cloud condensation nuclei and serves as a tool to quantify their climatic impact.
Zacharias Marinou Nikolaou, Jyh-Yuan Chen, Yiannis Proestos, Jos Lelieveld, and Rolf Sander
Geosci. Model Dev., 11, 3391–3407, https://doi.org/10.5194/gmd-11-3391-2018, https://doi.org/10.5194/gmd-11-3391-2018, 2018
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Chemistry is an important component of the atmosphere that describes many important physical processes. However, atmospheric chemical mechanisms include hundreds of species and reactions, posing a significant computational load. In this work, we use a powerful reduction method in order to develop a computationally faster chemical mechanism from a detailed mechanism. This enables accelerated simulations, which can be used to examine a wider range of processes in increased detail.
Maarten Krol, Marco de Bruine, Lars Killaars, Huug Ouwersloot, Andrea Pozzer, Yi Yin, Frederic Chevallier, Philippe Bousquet, Prabir Patra, Dmitry Belikov, Shamil Maksyutov, Sandip Dhomse, Wuhu Feng, and Martyn P. Chipperfield
Geosci. Model Dev., 11, 3109–3130, https://doi.org/10.5194/gmd-11-3109-2018, https://doi.org/10.5194/gmd-11-3109-2018, 2018
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The TransCom inter-comparison project regularly carries out studies to quantify errors in simulated atmospheric transport. This paper presents the first results of an age of air (AoA) inter-comparison of six global transport models. Following a protocol, six models simulated five tracers from which atmospheric transport times can easily be deduced. Results highlight that inter-model differences associated with atmospheric transport are still large and require further analysis.
Chinmay Mallik, Laura Tomsche, Efstratios Bourtsoukidis, John N. Crowley, Bettina Derstroff, Horst Fischer, Sascha Hafermann, Imke Hüser, Umar Javed, Stephan Keßel, Jos Lelieveld, Monica Martinez, Hannah Meusel, Anna Novelli, Gavin J. Phillips, Andrea Pozzer, Andreas Reiffs, Rolf Sander, Domenico Taraborrelli, Carina Sauvage, Jan Schuladen, Hang Su, Jonathan Williams, and Hartwig Harder
Atmos. Chem. Phys., 18, 10825–10847, https://doi.org/10.5194/acp-18-10825-2018, https://doi.org/10.5194/acp-18-10825-2018, 2018
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OH and HO2 control the transformation of air pollutants and O3 formation. Their implication for air quality over the climatically sensitive Mediterranean region was studied during a field campaign in Cyprus. Production of OH, HO2, and recycled OH was lower in aged marine air masses. Box model simulations of OH and HO2 agreed with measurements except at high terpene concentrations when model RO2 due to terpenes caused large HO2 loss. Autoxidation schemes for RO2 improved the agreement.
Eleni Karnezi, Benjamin N. Murphy, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Florian Rubach, Astrid Kiendler-Scharr, Thomas F. Mentel, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 10759–10772, https://doi.org/10.5194/acp-18-10759-2018, https://doi.org/10.5194/acp-18-10759-2018, 2018
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Different parameterizations of the organic aerosol (OA) formation and evolution are evaluated using ground and airborne measurements collected in the 2012 PEGASOS field campaign in the Po Valley (Italy). Total OA concentration and O : C ratios were reproduced within experimental error by a number of schemes. Anthropogenic secondary OA (SOA) contributed 15–25 % of the total OA, 20–35 % of SOA from intermediate volatility compounds oxidation, and 15–45 % of biogenic SOA depending on the scheme.
Aristeidis K. Georgoulias, Athanasios Tsikerdekis, Vassilis Amiridis, Eleni Marinou, Angela Benedetti, Prodromos Zanis, Georgia Alexandri, Lucia Mona, Konstantinos A. Kourtidis, and Jos Lelieveld
Atmos. Chem. Phys., 18, 8601–8620, https://doi.org/10.5194/acp-18-8601-2018, https://doi.org/10.5194/acp-18-8601-2018, 2018
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In this work, the MACC reanalysis dust product is evaluated over Europe, Northern Africa and the Middle East using the EARLINET-optimized CALIOP/CALIPSO pure dust satellite-based product LIVAS (2007–2012). As dust plays a determinant role in processes related to weather and climate, human healt, and the economy, it is obvious that adequately simulating the amount of dust and its optical properties is essential. Our results could be used as a reference in future climate model evaluations.
Meryem Tanarhte, Sara Bacer, Susannah M. Burrows, J. Alex Huffman, Kyle M. Pierce, Andrea Pozzer, Roland Sarda-Estève, Nicole J. Savage, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-361, https://doi.org/10.5194/acp-2018-361, 2018
Revised manuscript not accepted
Evangelia Kostenidou, Eleni Karnezi, James R. Hite Jr., Aikaterini Bougiatioti, Kate Cerully, Lu Xu, Nga L. Ng, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 5799–5819, https://doi.org/10.5194/acp-18-5799-2018, https://doi.org/10.5194/acp-18-5799-2018, 2018
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The volatility distribution of organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS) was estimated. The volatility distribution of all components covered a wide range including both semi-volatile and low-volatility components. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.
Yingying Yan, Andrea Pozzer, Narendra Ojha, Jintai Lin, and Jos Lelieveld
Atmos. Chem. Phys., 18, 5589–5605, https://doi.org/10.5194/acp-18-5589-2018, https://doi.org/10.5194/acp-18-5589-2018, 2018
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Surface-based measurements from the EMEP network and EMAC model simulations are used to estimate the European surface ozone changes over 1995–2014. It shows a significantly decreasing trend in the 95th percentile ozone concentrations, while increasing in the 5th percentile ozone. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels.
Klaus Klingmüller, Swen Metzger, Mohamed Abdelkader, Vlassis A. Karydis, Georgiy L. Stenchikov, Andrea Pozzer, and Jos Lelieveld
Geosci. Model Dev., 11, 989–1008, https://doi.org/10.5194/gmd-11-989-2018, https://doi.org/10.5194/gmd-11-989-2018, 2018
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More than 1 billion tons of mineral dust particles are raised into the atmosphere every year, which has a significant impact on climate, society and ecosystems. The location, time and amount of dust emissions depend on surface and wind conditions. In the atmospheric chemistry–climate model EMAC, we have updated the relevant surface data and equations. Our validation shows that the updates substantially improve the agreement of model results and observations.
Jonathan Liebmann, Einar Karu, Nicolas Sobanski, Jan Schuladen, Mikael Ehn, Simon Schallhart, Lauriane Quéléver, Heidi Hellen, Hannele Hakola, Thorsten Hoffmann, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 3799–3815, https://doi.org/10.5194/acp-18-3799-2018, https://doi.org/10.5194/acp-18-3799-2018, 2018
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Using a newly developed experimental setup, we have made the first direct measurements (during autumn 2016) of NO3 reactivity in the Finnish boreal forest. The NO3 reactivity was generally very high (maximum value of 0.94/s) so that daytime reaction with organics was a substantial fraction of the NO3 loss. Observations of biogenic hydrocarbons (BVOCs) suggested a dominant role for monoterpenes in determining the NO3 reactivity, which displayed a strong vertical gradient between 8.5 and 25 m.
Ningxin Wang, Evangelia Kostenidou, Neil M. Donahue, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 3589–3601, https://doi.org/10.5194/acp-18-3589-2018, https://doi.org/10.5194/acp-18-3589-2018, 2018
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This study investigates aging in the α-pinene ozonolysis system with hydroxyl radicals (OH) through smog chamber experiments. After an equivalent of 2–4 days of typical atmospheric oxidation conditions, homogeneous OH oxidation of the α-pinene ozonolysis products resulted in a 20–40 % net increase in the organic aerosol concentration and an increase in aerosol O : C by up to 0.04. The relative humidity in the 5–50 % range had a minimum effect on aging.
Katrin Dulitz, Damien Amedro, Terry J. Dillon, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 18, 2381–2394, https://doi.org/10.5194/acp-18-2381-2018, https://doi.org/10.5194/acp-18-2381-2018, 2018
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The reaction between the OH radical and HNO3 represents an important route for the release of NOx (NO and NO2) from HNO3, the most important NOx reservoir in many parts of the atmosphere. In our laboratory study, we have generated an extensive, high-quality set of rate coefficients for this reaction at different temperatures and pressures and used these to derive a new parameterisation of the rate coefficient for atmospheric modelling.
Hannah Meusel, Alexandra Tamm, Uwe Kuhn, Dianming Wu, Anna Lena Leifke, Sabine Fiedler, Nina Ruckteschler, Petya Yordanova, Naama Lang-Yona, Mira Pöhlker, Jos Lelieveld, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Bettina Weber, and Yafang Cheng
Atmos. Chem. Phys., 18, 799–813, https://doi.org/10.5194/acp-18-799-2018, https://doi.org/10.5194/acp-18-799-2018, 2018
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The photolysis of nitrous acid (HONO) forms the OH radical. However, not all sources are known. Recent studies showed that HONO can be emitted from soil but they did not evaluate the importance to the HONO budget. In this work HONO emissions from 43 soil and biological soil crust samples from Cyprus were measured in a dynamic chamber and extrapolated to the real atmosphere. A large fraction of the local missing source (published earlier; Meusel et al., 2016) could be assigned to soil emissions.
Efstratios Bourtsoukidis, Frank Helleis, Laura Tomsche, Horst Fischer, Rolf Hofmann, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 10, 5089–5105, https://doi.org/10.5194/amt-10-5089-2017, https://doi.org/10.5194/amt-10-5089-2017, 2017
Kerrigan P. Cain and Spyros N. Pandis
Atmos. Meas. Tech., 10, 4865–4876, https://doi.org/10.5194/amt-10-4865-2017, https://doi.org/10.5194/amt-10-4865-2017, 2017
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Hygroscopicity, oxidation level, and volatility of organic pollutants are three crucial properties that determine their fate in the atmosphere. This study assesses the feasibility of a novel measurement and analysis technique to determine these properties of organic aerosol
components at the same time and to establish their relationship.
Amit Sharma, Narendra Ojha, Andrea Pozzer, Kathleen A. Mar, Gufran Beig, Jos Lelieveld, and Sachin S. Gunthe
Atmos. Chem. Phys., 17, 14393–14413, https://doi.org/10.5194/acp-17-14393-2017, https://doi.org/10.5194/acp-17-14393-2017, 2017
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We evaluate the numerical simulations of surface ozone during pre-monsoon season against a network of stations including clean, rural and polluted urban environments in the south Asian region. Significant effects of the employed emission inventory and chemical mechanism on the simulated ozone are found during the noon hours of intense photochemistry. The presented evaluation on the diurnal timescale would have implications for assessing ozone buildup and impacts on human health and crop yields.
Huisheng Bian, Mian Chin, Didier A. Hauglustaine, Michael Schulz, Gunnar Myhre, Susanne E. Bauer, Marianne T. Lund, Vlassis A. Karydis, Tom L. Kucsera, Xiaohua Pan, Andrea Pozzer, Ragnhild B. Skeie, Stephen D. Steenrod, Kengo Sudo, Kostas Tsigaridis, Alexandra P. Tsimpidi, and Svetlana G. Tsyro
Atmos. Chem. Phys., 17, 12911–12940, https://doi.org/10.5194/acp-17-12911-2017, https://doi.org/10.5194/acp-17-12911-2017, 2017
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Atmospheric nitrate contributes notably to total aerosol mass in the present day and is likely to be more important over the next century, with a projected decline in SO2 and NOx emissions and increase in NH3 emissions. This paper investigates atmospheric nitrate using multiple global models and measurements. The study is part of the AeroCom phase III activity. The study is the first attempt to look at global atmospheric nitrate simulation at physical and chemical process levels.
Andrea Pozzer, Alexandra P. Tsimpidi, Vlassis A. Karydis, Alexander de Meij, and Jos Lelieveld
Atmos. Chem. Phys., 17, 12813–12826, https://doi.org/10.5194/acp-17-12813-2017, https://doi.org/10.5194/acp-17-12813-2017, 2017
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This study shows that agricultural emissions are important for air quality and their reduction can effectively reduce the concentration of fine particles and their associated premature mortality. Therefore, emission control policies, especially in North America and Europe, should also involve strong ammonia emission decreases to optimally reduce fine-particle concentration.
David Cabrera-Perez, Domenico Taraborrelli, Jos Lelieveld, Thorsten Hoffmann, and Andrea Pozzer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-928, https://doi.org/10.5194/acp-2017-928, 2017
Revised manuscript not accepted
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Aromatic compounds are present in rural and urban atmospheres. The aim of this work is to disentangle the impacts of these compounds in different important atmospheric chemical species with the help of a numerical model. Aromatics have low impact OH, NOx and Ozone concentrations in the global scale (below 4 %). The impact however is larger in the regional scale (up to 10 %). The largest impact is in glyoxal and NO3 concentrations, with changes up to 10 % globally and 40 % regionally.
Evangelos E. Louvaris, Eleni Karnezi, Evangelia Kostenidou, Christos Kaltsonoudis, and Spyros N. Pandis
Atmos. Meas. Tech., 10, 3909–3918, https://doi.org/10.5194/amt-10-3909-2017, https://doi.org/10.5194/amt-10-3909-2017, 2017
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A method for the determination of the organic aerosol volatility distribution combining thermodenuder and isothermal dilution measurements is developed. The approach was tested in experiments that were conducted in a smog chamber using organic aerosol produced during meat charbroiling. Addition of the dilution measurements to the thermodenuder data results in a lower uncertainty of the estimated vaporization enthalpy as well as the semivolatile content of the aerosol.
Heiko Bozem, Andrea Pozzer, Hartwig Harder, Monica Martinez, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 11835–11848, https://doi.org/10.5194/acp-17-11835-2017, https://doi.org/10.5194/acp-17-11835-2017, 2017
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We present a case study of deep convection over Germany in July 2007 within the framework of the HOOVER II project. Airborne in situ measurements within the in- and outflow regions of an isolated thunderstorm provide a unique data set to study the influence of deep convection on the transport efficiency of soluble and insoluble trace gases. Despite their high solubility HCHO and H2O2 show enhanced concentrations in the outflow presumably due to degassing from cloud droplets during freezing.
Hannah Meusel, Yasin Elshorbany, Uwe Kuhn, Thorsten Bartels-Rausch, Kathrin Reinmuth-Selzle, Christopher J. Kampf, Guo Li, Xiaoxiang Wang, Jos Lelieveld, Ulrich Pöschl, Thorsten Hoffmann, Hang Su, Markus Ammann, and Yafang Cheng
Atmos. Chem. Phys., 17, 11819–11833, https://doi.org/10.5194/acp-17-11819-2017, https://doi.org/10.5194/acp-17-11819-2017, 2017
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In this study we investigated protein nitration and decomposition by light in the presence of NO2 via flow tube measurements. Nitrated proteins have an enhanced allergenic potential but so far nitration was only studied in dark conditions. Under irradiated conditions we found that proteins predominantly decompose while forming nitrous acid (HONO) an important precursor of the OH radical. Unlike other studies on heterogeneous NO2 conversion we found a stable HONO formation over a long period.
Heiko Bozem, Tim M. Butler, Mark G. Lawrence, Hartwig Harder, Monica Martinez, Dagmar Kubistin, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 10565–10582, https://doi.org/10.5194/acp-17-10565-2017, https://doi.org/10.5194/acp-17-10565-2017, 2017
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We present airborne measurements and model simulations in the tropics and mid-latitudes during GABRIEL and HOOVER, respectively. Based only on in situ data net ozone formation/destruction tendencies (NOPR) are calculated and compared to a 3-D chemistry transport model. The NOPR is positive in the continental boundary layer and the upper troposphere above 6 km. In the marine boundary layer and the middle troposphere ozone destruction prevails. Fresh convection shows strong net ozone formation.
Bettina Derstroff, Imke Hüser, Efstratios Bourtsoukidis, John N. Crowley, Horst Fischer, Sergey Gromov, Hartwig Harder, Ruud H. H. Janssen, Jürgen Kesselmeier, Jos Lelieveld, Chinmay Mallik, Monica Martinez, Anna Novelli, Uwe Parchatka, Gavin J. Phillips, Rolf Sander, Carina Sauvage, Jan Schuladen, Christof Stönner, Laura Tomsche, and Jonathan Williams
Atmos. Chem. Phys., 17, 9547–9566, https://doi.org/10.5194/acp-17-9547-2017, https://doi.org/10.5194/acp-17-9547-2017, 2017
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The aim of the study was to examine aged air masses being transported from the European continent towards Cyprus. Longer-lived oxygenated volatile organic compounds (OVOCs) such as methanol were mainly impacted by long-distance transport and showed higher values in air masses from eastern Europe than in a flow regime from the west. The impact of the transport through the marine boundary layer as well as the influence of the residual layer/free troposphere on OVOCs were studied.
Stephan Keßel, David Cabrera-Perez, Abraham Horowitz, Patrick R. Veres, Rolf Sander, Domenico Taraborrelli, Maria Tucceri, John N. Crowley, Andrea Pozzer, Christof Stönner, Luc Vereecken, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 17, 8789–8804, https://doi.org/10.5194/acp-17-8789-2017, https://doi.org/10.5194/acp-17-8789-2017, 2017
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In this study we identify an often overlooked stable oxide of carbon, namely carbon suboxide (C3O2), in ambient air. We have made C3O2 and in the laboratory determined its absorption cross section data and the rate of reaction with two important atmospheric oxidants, OH and O3. By incorporating known sources and sinks in a global model we have generated a first global picture of the distribution of this species in the atmosphere.
Anna Novelli, Korbinian Hens, Cheryl Tatum Ernest, Monica Martinez, Anke C. Nölscher, Vinayak Sinha, Pauli Paasonen, Tuukka Petäjä, Mikko Sipilä, Thomas Elste, Christian Plass-Dülmer, Gavin J. Phillips, Dagmar Kubistin, Jonathan Williams, Luc Vereecken, Jos Lelieveld, and Hartwig Harder
Atmos. Chem. Phys., 17, 7807–7826, https://doi.org/10.5194/acp-17-7807-2017, https://doi.org/10.5194/acp-17-7807-2017, 2017
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The ambient concentration of stabilised Criegee intermediates (SCIs) was estimated for two
environments using field data. The low concentrations predicted indicate that SCIs are
unlikely to have a large impact on atmospheric chemistry. Concurrent measurements of an OH background signal using the Mainz IPI-LIF-FAGE instrument were found to be consistent with the chemistry of SCIs during the measurement campaigns.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 7345–7364, https://doi.org/10.5194/acp-17-7345-2017, https://doi.org/10.5194/acp-17-7345-2017, 2017
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We analyzed the sensitivity of model-predicted global-scale OA to parameters and assumptions that control primary emissions, photochemical aging, and the scavenging efficiency of LVOCs, SVOCs, and IVOCs. The simulated OA concentrations were evaluated against a global dataset of AMS measurements. According to our analysis, a combination of increased IVOCs and decreased hygroscopicity of the freshly emitted IVOCs can help reduce discrepancies between simulated SOA and observed OOA concentrations.
Christos Kaltsonoudis, Evangelia Kostenidou, Evangelos Louvaris, Magda Psichoudaki, Epameinondas Tsiligiannis, Kalliopi Florou, Aikaterini Liangou, and Spyros N. Pandis
Atmos. Chem. Phys., 17, 7143–7155, https://doi.org/10.5194/acp-17-7143-2017, https://doi.org/10.5194/acp-17-7143-2017, 2017
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Cooking emissions can be a significant source of particulate matter in urban areas. In this study the aerosol- and gas-phase emissions from meat charbroiling were characterized. More than 99% of the aerosol emitted was composed of organic compounds. The fresh particles were similar to the cooking organic aerosol over Greek cities during the winter, while the reacted particles were similar to those found in the atmosphere during the summer.
Narendra Ojha, Andrea Pozzer, Dimitris Akritidis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 6743–6757, https://doi.org/10.5194/acp-17-6743-2017, https://doi.org/10.5194/acp-17-6743-2017, 2017
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We investigate the processes, frequency of occurrence and seasonality, and effects of strongly enhanced ozone layers in the middle–upper troposphere (SOPs) over the Himalayas using a global model (EMAC). Rapid transport of stratospheric air masses is found as a key underlying process. Model predicts more frequent SOP events during the pre-monsoon. SOPs are found to significantly enhance the tropospheric ozone column over the Himalayas.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Jonathan M. Liebmann, Gerhard Schuster, Jan B. Schuladen, Nicolas Sobanski, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 10, 1241–1258, https://doi.org/10.5194/amt-10-1241-2017, https://doi.org/10.5194/amt-10-1241-2017, 2017
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We describe the first instrument for measurement of the rate constant for reactive loss (i.e. the total reactivity) of NO3 in ambient air. This is essentially a measureement of the lifetime of NO3 and will help assess the role of NO3 and N2O5 in conversion of reactive nitrogen oxides to reservoir species in the troposphere.
Nicolas Sobanski, Jim Thieser, Jan Schuladen, Carina Sauvage, Wei Song, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 17, 4115–4130, https://doi.org/10.5194/acp-17-4115-2017, https://doi.org/10.5194/acp-17-4115-2017, 2017
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We investigated the formation of gas-phase organic nitrates at a forested semi-urban site. This work constitutes the first detailed analysis of the sum of organic nitrate mixing ratios measured by thermal dissociation cavity ring-down spectroscopy in continental Europe. Day (OH-initiated) and night-time (NO3-initiated) production of alkyl nitrates proceed at similar rates.
Mohamed Abdelkader, Swen Metzger, Benedikt Steil, Klaus Klingmüller, Holger Tost, Andrea Pozzer, Georgiy Stenchikov, Leonard Barrie, and Jos Lelieveld
Atmos. Chem. Phys., 17, 3799–3821, https://doi.org/10.5194/acp-17-3799-2017, https://doi.org/10.5194/acp-17-3799-2017, 2017
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We present a modeling study on the impacts of the key processes (dust emission flux, convection and dust aging parameterizations) that control the transatlantic dust transport using an advanced version of the EMAC atmospheric chemistry general circulation model. We define the
direct effect of dust agingas an increase in the AOD as a result of hygroscopic growth. We define the
indirect effectas a reduction in the dust AOD due to the higher removal of the aged dust particles.
Kalliopi Florou, Dimitrios K. Papanastasiou, Michael Pikridas, Christos Kaltsonoudis, Evangelos Louvaris, Georgios I. Gkatzelis, David Patoulias, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Chem. Phys., 17, 3145–3163, https://doi.org/10.5194/acp-17-3145-2017, https://doi.org/10.5194/acp-17-3145-2017, 2017
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The composition of fine particulate matter (PM) in two major Greek cities (Athens and Patras) was measured during two wintertime campaigns in 2012 and 2013. Residential wood burning has dramatically increased due to the Greek financial crisis, contributing around 50 % of the fine PM on average and more than 80 % during nighttime. Cooking is also an important source during both midday and evening, while transportation dominates only during the morning rush hour.
Sinikka T. Lennartz, Christa A. Marandino, Marc von Hobe, Pau Cortes, Birgit Quack, Rafel Simo, Dennis Booge, Andrea Pozzer, Tobias Steinhoff, Damian L. Arevalo-Martinez, Corinna Kloss, Astrid Bracher, Rüdiger Röttgers, Elliot Atlas, and Kirstin Krüger
Atmos. Chem. Phys., 17, 385–402, https://doi.org/10.5194/acp-17-385-2017, https://doi.org/10.5194/acp-17-385-2017, 2017
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We present new sea surface and marine boundary layer measurements of carbonyl sulfide, the most abundant sulfur gas in the atmosphere, and calculate an oceanic emission estimate. Our results imply that oceanic emissions are very unlikely to account for the missing source in the atmospheric budget that is currently discussed for OCS.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Andrea Pozzer, Yogesh K. Tiwari, K. Ravi Kumar, and Jos Lelieveld
Atmos. Chem. Phys., 17, 257–275, https://doi.org/10.5194/acp-17-257-2017, https://doi.org/10.5194/acp-17-257-2017, 2017
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This study presents first ship-borne measurements of trace gases over the Bay of Bengal during summer monsoon. The observed variations in trace gases are shown to be due to dynamics/transport and en route photochemistry. Analysis of meteorological and chemical fields shows that significantly lower ozone during rainfall is associated with the downdrafts. A regional model reproduces the observed variations and revealed the rapid transport of ozone across the Bay of Bengal during an event.
Sara Bacer, Theodoros Christoudias, and Andrea Pozzer
Atmos. Chem. Phys., 16, 15581–15592, https://doi.org/10.5194/acp-16-15581-2016, https://doi.org/10.5194/acp-16-15581-2016, 2016
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We investigate the influence of the North Atlantic Oscillation on atmospheric pollutant transport in the 21st century under a global climate-change scenario, using a coupled atmosphere–chemistry–ocean general circulation model. We find that, at the end of the century, the south-western Mediterranean and northern Africa will see higher pollutant concentrations during positive NAO phases with respect to the past, while a wider part of north Europe will see lower pollutant concentrations.
Christos Kaltsonoudis, Evangelia Kostenidou, Kalliopi Florou, Magda Psichoudaki, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 14825–14842, https://doi.org/10.5194/acp-16-14825-2016, https://doi.org/10.5194/acp-16-14825-2016, 2016
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Volatile organic compounds (VOCs) were monitored in urban backgrounds sites, in Athens and Patras in Greece. In summer most of the measured VOCs were due to biogenic and traffic emissions. Winter measurements in Athens revealed that biomass burning used for residential heating was the dominant VOC source. The biomass burning VOC emission ratios and emission factors were estimated.
Antigoni Panagiotopoulou, Panagiotis Charalampidis, Christos Fountoukis, Christodoulos Pilinis, and Spyros N. Pandis
Geosci. Model Dev., 9, 4257–4272, https://doi.org/10.5194/gmd-9-4257-2016, https://doi.org/10.5194/gmd-9-4257-2016, 2016
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The ability of chemical transport model PMCAMx to reproduce ground and satellite aerosol optical depth (AOD) measurements over Europe is evaluated. PMCAMx reproduces AOD values over Spain, the UK, central Europe, and Russia with a fractional bias of less than 15 % and a fractional error of less than 30 %. The model overestimates the AOD over northern Europe probably due to an overestimation of organic aerosol and sulfates, and underestimates over the Balkans due to an underestimation of sulfates.
Hannah Meusel, Uwe Kuhn, Andreas Reiffs, Chinmay Mallik, Hartwig Harder, Monica Martinez, Jan Schuladen, Birger Bohn, Uwe Parchatka, John N. Crowley, Horst Fischer, Laura Tomsche, Anna Novelli, Thorsten Hoffmann, Ruud H. H. Janssen, Oscar Hartogensis, Michael Pikridas, Mihalis Vrekoussis, Efstratios Bourtsoukidis, Bettina Weber, Jos Lelieveld, Jonathan Williams, Ulrich Pöschl, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 16, 14475–14493, https://doi.org/10.5194/acp-16-14475-2016, https://doi.org/10.5194/acp-16-14475-2016, 2016
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There are many studies which show discrepancies between modeled and measured nitrous acid (HONO, precursor of OH radical) in the troposphere but with no satisfactory explanation. Ideal conditions to study the unknown sources of HONO were found on Cyprus, a remote Mediterranean island. Budget analysis of trace gas measurements indicates a common source of NO and HONO, which is not related to anthropogenic activity and is most likely derived from biologic activity in soils and subsequent emission.
Dimitris Akritidis, Andrea Pozzer, Prodromos Zanis, Evangelos Tyrlis, Bojan Škerlak, Michael Sprenger, and Jos Lelieveld
Atmos. Chem. Phys., 16, 14025–14039, https://doi.org/10.5194/acp-16-14025-2016, https://doi.org/10.5194/acp-16-14025-2016, 2016
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We investigate the contribution of tropopause folds in the summertime tropospheric ozone pool over the eastern Mediterranean and the Middle East. For this purpose we use the EMAC atmospheric chemistry–climate model and a fold identification algorithm. A clear increase of ozone is found in the middle troposphere due to fold activity. The interannual variability of near-surface ozone over the eastern Mediterranean is related to that of both tropopause folds and ozone in the free troposphere.
Aristeidis K. Georgoulias, Georgia Alexandri, Konstantinos A. Kourtidis, Jos Lelieveld, Prodromos Zanis, Ulrich Pöschl, Robert Levy, Vassilis Amiridis, Eleni Marinou, and Athanasios Tsikerdekis
Atmos. Chem. Phys., 16, 13853–13884, https://doi.org/10.5194/acp-16-13853-2016, https://doi.org/10.5194/acp-16-13853-2016, 2016
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In this work, single pixel observations from MODIS Terra and Aqua are analyzed together with data from other satellite sensors, reanalysis projects and a chemistry–aerosol-transport model to study the spatiotemporal variability of different aerosol types. The results are in accordance with previous works and are a good reference for future studies in the area focusing on aerosols, clouds, radiation and the effects of particle pollution on human health.
Gavin J. Phillips, Jim Thieser, Mingjin Tang, Nicolas Sobanski, Gerhard Schuster, Johannes Fachinger, Frank Drewnick, Stephan Borrmann, Heinz Bingemer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 16, 13231–13249, https://doi.org/10.5194/acp-16-13231-2016, https://doi.org/10.5194/acp-16-13231-2016, 2016
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We use trace gas measurements (N2O5, ClNO2, NO3) and particle properties (surface area, nitrate content etc.) to derive uptake coefficients (the probability of removal from the gas-phase on a per-collision basis) for the interaction of N2O5 with ambient aerosol and also the efficiency of formation of ClNO2. The uptake coefficients show high variability but are reasonably well captured by parameterisations based on laboratory measurements.
Kathleen A. Mar, Narendra Ojha, Andrea Pozzer, and Tim M. Butler
Geosci. Model Dev., 9, 3699–3728, https://doi.org/10.5194/gmd-9-3699-2016, https://doi.org/10.5194/gmd-9-3699-2016, 2016
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Ground-level ozone is an air pollutant with adverse effects on human and ecosystem health and is also a climate forcer with a significant warming effect. This paper presents the setup and evaluation of a model for ozone air quality over Europe. Within the model evaluation, we compare the use of two commonly used photochemical schemes, and we conclude that uncertainties in the representation of chemistry are important to consider when using air quality models for policy applications.
Nicolas Sobanski, Jan Schuladen, Gerhard Schuster, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 9, 5103–5118, https://doi.org/10.5194/amt-9-5103-2016, https://doi.org/10.5194/amt-9-5103-2016, 2016
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We report the characteristics and performances of a cavity ring-down spectrometer (CRDS) designed for field measurements that uses light absorption at 662 and 405 nm to detect different reactive nitrogen species or group of species in the gas phase, either directly or after thermal decomposition. We report improvements compared to currently existing instruments, and describe the corrections applied to the raw data to account for chemical and optical interferences.
Jos Lelieveld, Sergey Gromov, Andrea Pozzer, and Domenico Taraborrelli
Atmos. Chem. Phys., 16, 12477–12493, https://doi.org/10.5194/acp-16-12477-2016, https://doi.org/10.5194/acp-16-12477-2016, 2016
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The self-cleaning capacity of the atmosphere is controlled by hydroxyl (OH) radicals in the troposphere. There are primary and secondary OH sources, the former through the photodissociation of ozone, the latter through OH recycling. We used a global model, showing that secondary sources are larger than assumed previously, which buffers OH. Complementary OH formation mechanisms in pristine and polluted environments, connected through transport of ozone, can maintain stable global OH levels.
Narendra Singh, Raman Solanki, Narendra Ojha, Ruud H. H. Janssen, Andrea Pozzer, and Surendra K. Dhaka
Atmos. Chem. Phys., 16, 10559–10572, https://doi.org/10.5194/acp-16-10559-2016, https://doi.org/10.5194/acp-16-10559-2016, 2016
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Our study presents measurements and model simulations of boundary layer evolution over a mountain peak in the central Himalayas. The observations were made as a part of the Ganges Valley Aerosol Experiment. The implications of biases in model simulated boundary layer towards simulations of trace species is investigated.
Elham Baranizadeh, Benjamin N. Murphy, Jan Julin, Saeed Falahat, Carly L. Reddington, Antti Arola, Lars Ahlm, Santtu Mikkonen, Christos Fountoukis, David Patoulias, Andreas Minikin, Thomas Hamburger, Ari Laaksonen, Spyros N. Pandis, Hanna Vehkamäki, Kari E. J. Lehtinen, and Ilona Riipinen
Geosci. Model Dev., 9, 2741–2754, https://doi.org/10.5194/gmd-9-2741-2016, https://doi.org/10.5194/gmd-9-2741-2016, 2016
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The molecular mechanisms through which new ultrafine (< 100 nm) aerosol particles are formed in the atmosphere have puzzled the scientific community for decades. In the past few years, however, significant progress has been made in unraveling these processes through laboratory studies and computational efforts. In this work we have implemented these new developments to an air quality model and study the implications of anthropogenically driven particle formation for European air quality.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 16, 8939–8962, https://doi.org/10.5194/acp-16-8939-2016, https://doi.org/10.5194/acp-16-8939-2016, 2016
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In this work we use a global chemistry climate model together with a comprehensive global AMS data set in order to provide valuable insights into the temporal and geographical variability of the contribution of the emitted particles and the chemically processed organic material from combustion sources to total OA. This study reveals the high importance of SOA from anthropogenic sources on global OA concentrations and identifies plausible sources of discrepancy between models and measurements.
Steffen Beirle, Christoph Hörmann, Patrick Jöckel, Song Liu, Marloes Penning de Vries, Andrea Pozzer, Holger Sihler, Pieter Valks, and Thomas Wagner
Atmos. Meas. Tech., 9, 2753–2779, https://doi.org/10.5194/amt-9-2753-2016, https://doi.org/10.5194/amt-9-2753-2016, 2016
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237, https://doi.org/10.5194/acp-16-7213-2016, https://doi.org/10.5194/acp-16-7213-2016, 2016
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We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
David Cabrera-Perez, Domenico Taraborrelli, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 16, 6931–6947, https://doi.org/10.5194/acp-16-6931-2016, https://doi.org/10.5194/acp-16-6931-2016, 2016
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The global atmospheric budget and distribution of monocyclic aromatic compounds is estimated, using an atmospheric chemistry general circulation model. Simulation results are evaluated with observations with the goal of understanding emission, production and removal of these compounds. Anthropogenic and biomass burning are the main sources of aromatic compounds to the atmosphere. The main sink is photochemical decomposition and in lesser importance dry deposition.
Klaus Klingmüller, Andrea Pozzer, Swen Metzger, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 16, 5063–5073, https://doi.org/10.5194/acp-16-5063-2016, https://doi.org/10.5194/acp-16-5063-2016, 2016
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During the last decade, the Middle East experienced the strongest increase in atmospheric aerosol concentrations worldwide. Based on satellite observations, the present study corroborates this trend and reveals correlations with soil moisture and precipitation in and surrounding the Fertile Crescent. This suggests that the increasing drought conditions in this region have enhanced dust emissions, a tendency which is expected to be intensified by climate change.
N. Sobanski, M. J. Tang, J. Thieser, G. Schuster, D. Pöhler, H. Fischer, W. Song, C. Sauvage, J. Williams, J. Fachinger, F. Berkes, P. Hoor, U. Platt, J. Lelieveld, and J. N. Crowley
Atmos. Chem. Phys., 16, 4867–4883, https://doi.org/10.5194/acp-16-4867-2016, https://doi.org/10.5194/acp-16-4867-2016, 2016
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The nitrate radical (NO3) is an important nocturnal oxidant. By measuring NO3, its precursors (nitrogen dioxide and ozone) and several trace gases with which it reacts, we examined the chemical and meteorological factors influencing the lifetime of NO3 at a semi-rural mountain site. Unexpectedly long lifetimes, approaching 1 h, were observed on several nights and were associated with a low-lying residual layer. We discuss the role of other reactions that convert NO2 to NO3.
Patrick Jöckel, Holger Tost, Andrea Pozzer, Markus Kunze, Oliver Kirner, Carl A. M. Brenninkmeijer, Sabine Brinkop, Duy S. Cai, Christoph Dyroff, Johannes Eckstein, Franziska Frank, Hella Garny, Klaus-Dirk Gottschaldt, Phoebe Graf, Volker Grewe, Astrid Kerkweg, Bastian Kern, Sigrun Matthes, Mariano Mertens, Stefanie Meul, Marco Neumaier, Matthias Nützel, Sophie Oberländer-Hayn, Roland Ruhnke, Theresa Runde, Rolf Sander, Dieter Scharffe, and Andreas Zahn
Geosci. Model Dev., 9, 1153–1200, https://doi.org/10.5194/gmd-9-1153-2016, https://doi.org/10.5194/gmd-9-1153-2016, 2016
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With an advanced numerical global chemistry climate model (CCM) we performed several detailed
combined hind-cast and projection simulations of the period 1950 to 2100 to assess the
past, present, and potential future dynamical and chemical state of the Earth atmosphere.
The manuscript documents the model and the various applied model set-ups and provides
a first evaluation of the simulation results from a global perspective as a quality check of the data.
Christos Fountoukis, Athanasios G. Megaritis, Ksakousti Skyllakou, Panagiotis E. Charalampidis, Hugo A. C. Denier van der Gon, Monica Crippa, André S. H. Prévôt, Friederike Fachinger, Alfred Wiedensohler, Christodoulos Pilinis, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 3727–3741, https://doi.org/10.5194/acp-16-3727-2016, https://doi.org/10.5194/acp-16-3727-2016, 2016
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We use PMCAMx with high grid resolution over Paris to simulate carbonaceous aerosol during the summer and winter MEGAPOLI campaigns. PMCAMx reproduces BC observations well. Addition of cooking organic aerosol emissions of 80 mg per day per capita is needed to reproduce the corresponding observations. While the oxygenated organic aerosol predictions during the summer are encouraging a major wintertime source appears to be missing.
Armin Rauthe-Schöch, Angela K. Baker, Tanja J. Schuck, Carl A. M. Brenninkmeijer, Andreas Zahn, Markus Hermann, Greta Stratmann, Helmut Ziereis, Peter F. J. van Velthoven, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3609–3629, https://doi.org/10.5194/acp-16-3609-2016, https://doi.org/10.5194/acp-16-3609-2016, 2016
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The flying laboratory CARIBIC onboard a passenger aircraft measured trace gases and aerosol particles in the upper tropospheric Indian summer monsoon anticyclone in summer 2008. We used the measurements together with meteorological analyses to investigate the chemical signature of the northern and southern part of the monsoon, the source regions from where the air was entrained into the monsoon and which parts of the world received polluted air that had been chemically processed in the monsoon.
Narendra Ojha, Andrea Pozzer, Armin Rauthe-Schöch, Angela K. Baker, Jongmin Yoon, Carl A. M. Brenninkmeijer, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3013–3032, https://doi.org/10.5194/acp-16-3013-2016, https://doi.org/10.5194/acp-16-3013-2016, 2016
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We compare simulations of ozone and carbon monoxide using a regional chemistry transport model (WRF-Chem) with aircraft observations from CARIBIC program over India during monsoon period. Sensitivity simulations are conducted to assess the influences of regional emissions and long-range transport.
Andrea Paciga, Eleni Karnezi, Evangelia Kostenidou, Lea Hildebrandt, Magda Psichoudaki, Gabriella J. Engelhart, Byong-Hyoek Lee, Monica Crippa, André S. H. Prévôt, Urs Baltensperger, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 2013–2023, https://doi.org/10.5194/acp-16-2013-2016, https://doi.org/10.5194/acp-16-2013-2016, 2016
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We estimate the volatility distribution for the organic aerosol (OA) components during summer and winter field campaigns in Paris, France as part of the collaborative project MEGAPOLI. The OA factors (hydrocarbon like OA, cooking OA, marine OA, oxygenated OA) had a broad spectrum of volatilities with no direct link between the average volatility and average oxygen to carbon of the OA components.
J. Thieser, G. Schuster, J. Schuladen, G. J. Phillips, A. Reiffs, U. Parchatka, D. Pöhler, J. Lelieveld, and J. N. Crowley
Atmos. Meas. Tech., 9, 553–576, https://doi.org/10.5194/amt-9-553-2016, https://doi.org/10.5194/amt-9-553-2016, 2016
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We report on the use of thermal dissociation cavity ring-down spectroscopy to detect NO2, peroxy nitrates and alkyl nitrates. We present both laboratory studies that characterise the chemical formation and loss of NO2 in the heated inlets and also result from a first field deployment.
V. A. Karydis, A. P. Tsimpidi, A. Pozzer, M. Astitha, and J. Lelieveld
Atmos. Chem. Phys., 16, 1491–1509, https://doi.org/10.5194/acp-16-1491-2016, https://doi.org/10.5194/acp-16-1491-2016, 2016
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We provide an assessment of the chemical composition and global aerosol load of aerosol nitrate and determine the effect of mineral dust on its formation due to thermodynamical interactions. For this purpose we used an explicit geographical representation of the emitted soil particle size distribution and chemical composition. We conclude mineral dust aerosol chemistry is important for nitrate aerosol formation and significantly affects its global distribution, especially in the coarse mode.
G. I. Gkatzelis, D. K. Papanastasiou, K. Florou, C. Kaltsonoudis, E. Louvaris, and S. N. Pandis
Atmos. Meas. Tech., 9, 103–114, https://doi.org/10.5194/amt-9-103-2016, https://doi.org/10.5194/amt-9-103-2016, 2016
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A method for the measurement of the nonvolatile atmospheric particle size distribution is developed and tested. The tests include laboratory experiments with biogenic and anthropogenic secondary organic aerosol as well as nucleation experiments with ambient air. The method is then further tested during an ambient campaign.
S. Bacer, T. Christoudias, and A. Pozzer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-33049-2015, https://doi.org/10.5194/acpd-15-33049-2015, 2015
Preprint withdrawn
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We investigate the temporal variability of the North Atlantic Oscillation (NAO) pattern and its relation to the atmospheric dispersion of pollutants in the near past and in the future.
We use a global climate circulation model in order to analyze the NAO signal and its correlation with pollutant concentrations. We find that the NAO is influenced by natural climate variability and that the NAO Indices may be used as indicators of (future) pollutant transport over Europe.
E. Kostenidou, K. Florou, C. Kaltsonoudis, M. Tsiflikiotou, S. Vratolis, K. Eleftheriadis, and S. N. Pandis
Atmos. Chem. Phys., 15, 11355–11371, https://doi.org/10.5194/acp-15-11355-2015, https://doi.org/10.5194/acp-15-11355-2015, 2015
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The concentration and chemical composition of fine particulate matter were measured during the summer of 2012 in two Greek cities, Patras and Athens. The composition of PM1 was surprisingly similar in both areas, demonstrating the importance of regional sources. Analysis of the Aerosol Mass Spectrometer data suggested that the contribution of the primary sources to organic aerosol was important (22% in Patras and 35% in Athens) but not dominant.
M. Pikridas, J. Sciare, F. Freutel, S. Crumeyrolle, S.-L. von der Weiden-Reinmüller, A. Borbon, A. Schwarzenboeck, M. Merkel, M. Crippa, E. Kostenidou, M. Psichoudaki, L. Hildebrandt, G. J. Engelhart, T. Petäjä, A. S. H. Prévôt, F. Drewnick, U. Baltensperger, A. Wiedensohler, M. Kulmala, M. Beekmann, and S. N. Pandis
Atmos. Chem. Phys., 15, 10219–10237, https://doi.org/10.5194/acp-15-10219-2015, https://doi.org/10.5194/acp-15-10219-2015, 2015
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Aerosol size distribution measurements from three ground sites, two mobile laboratories, and one airplane are combined to investigate the spatial and temporal variability of ultrafine particles in and around Paris during the summer and winter MEGAPOLI campaigns. The role of nucleation as a particle source and the influence of Paris emissions on their surroundings are examined.
M. Beekmann, A. S. H. Prévôt, F. Drewnick, J. Sciare, S. N. Pandis, H. A. C. Denier van der Gon, M. Crippa, F. Freutel, L. Poulain, V. Ghersi, E. Rodriguez, S. Beirle, P. Zotter, S.-L. von der Weiden-Reinmüller, M. Bressi, C. Fountoukis, H. Petetin, S. Szidat, J. Schneider, A. Rosso, I. El Haddad, A. Megaritis, Q. J. Zhang, V. Michoud, J. G. Slowik, S. Moukhtar, P. Kolmonen, A. Stohl, S. Eckhardt, A. Borbon, V. Gros, N. Marchand, J. L. Jaffrezo, A. Schwarzenboeck, A. Colomb, A. Wiedensohler, S. Borrmann, M. Lawrence, A. Baklanov, and U. Baltensperger
Atmos. Chem. Phys., 15, 9577–9591, https://doi.org/10.5194/acp-15-9577-2015, https://doi.org/10.5194/acp-15-9577-2015, 2015
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A detailed characterization of air quality in the Paris (France) agglomeration, a megacity, during two summer and winter intensive campaigns and from additional 1-year observations, revealed that about 70% of the fine particulate matter (PM) at urban background is transported into the megacity from upwind regions. Unexpectedly, a major part of organic PM is of modern origin (woodburning and cooking activities, secondary formation from biogenic VOC).
M. Abdelkader, S. Metzger, R. E. Mamouri, M. Astitha, L. Barrie, Z. Levin, and J. Lelieveld
Atmos. Chem. Phys., 15, 9173–9189, https://doi.org/10.5194/acp-15-9173-2015, https://doi.org/10.5194/acp-15-9173-2015, 2015
H. G. Ouwersloot, A. Pozzer, B. Steil, H. Tost, and J. Lelieveld
Geosci. Model Dev., 8, 2435–2445, https://doi.org/10.5194/gmd-8-2435-2015, https://doi.org/10.5194/gmd-8-2435-2015, 2015
S. Fuzzi, U. Baltensperger, K. Carslaw, S. Decesari, H. Denier van der Gon, M. C. Facchini, D. Fowler, I. Koren, B. Langford, U. Lohmann, E. Nemitz, S. Pandis, I. Riipinen, Y. Rudich, M. Schaap, J. G. Slowik, D. V. Spracklen, E. Vignati, M. Wild, M. Williams, and S. Gilardoni
Atmos. Chem. Phys., 15, 8217–8299, https://doi.org/10.5194/acp-15-8217-2015, https://doi.org/10.5194/acp-15-8217-2015, 2015
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Particulate matter (PM) constitutes one of the most challenging problems both for air quality and climate change policies. This paper reviews the most recent scientific results on the issue and the policy needs that have driven much of the increase in monitoring and mechanistic research over the last 2 decades. The synthesis reveals many new processes and developments in the science underpinning climate-PM interactions and the effects of PM on human health and the environment.
L. Hildebrandt Ruiz, A. L. Paciga, K. M. Cerully, A. Nenes, N. M. Donahue, and S. N. Pandis
Atmos. Chem. Phys., 15, 8301–8313, https://doi.org/10.5194/acp-15-8301-2015, https://doi.org/10.5194/acp-15-8301-2015, 2015
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Secondary organic aerosol (SOA) is transformed after its initial formation. We explored the effects of this chemical aging on the composition, mass yield, volatility, and hygroscopicity of SOA formed from the photo-oxidation of small aromatic volatile organic compounds. Higher exposure to the hydroxyl radical resulted in different SOA composition, average carbon oxidation state, and mass yield. The vapor pressure of SOA formed under different conditions varied by as much as a factor of 30.
H. Fischer, A. Pozzer, T. Schmitt, P. Jöckel, T. Klippel, D. Taraborrelli, and J. Lelieveld
Atmos. Chem. Phys., 15, 6971–6980, https://doi.org/10.5194/acp-15-6971-2015, https://doi.org/10.5194/acp-15-6971-2015, 2015
D. Patoulias, C. Fountoukis, I. Riipinen, and S. N. Pandis
Atmos. Chem. Phys., 15, 6337–6350, https://doi.org/10.5194/acp-15-6337-2015, https://doi.org/10.5194/acp-15-6337-2015, 2015
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A new aerosol dynamics model (DMANx) describing the organic vapor condensation on nanoparticles based on the volatility basis set framework is used to simulate typical nucleation events in two contrasting environments in Hyytiälä (Finland) and Finokalia (Greece). The role of semivolatile, low, and extremely low volatility organics and the corresponding surface energies is investigated.
I. Riipinen, N. Rastak, and S. N. Pandis
Atmos. Chem. Phys., 15, 6305–6322, https://doi.org/10.5194/acp-15-6305-2015, https://doi.org/10.5194/acp-15-6305-2015, 2015
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Atmospheric organic aerosol is complex and thus a challenge to model. We introduce a theoretical framework (solubility distributions) to represent the solubility of multicomponent mixtures. Using the framework, we evaluate the commonly made assumptions about the cloud condensation nucleus (CCN) activity of organic mixtures. We find that material with water solubilities larger than 0.1-100 g/L can usually be treated as completely soluble, which simplifies the treatment of organic CCN.
A. Tasoglou and S. N. Pandis
Atmos. Chem. Phys., 15, 6035–6046, https://doi.org/10.5194/acp-15-6035-2015, https://doi.org/10.5194/acp-15-6035-2015, 2015
S. Zheng, A. Pozzer, C. X. Cao, and J. Lelieveld
Atmos. Chem. Phys., 15, 5715–5725, https://doi.org/10.5194/acp-15-5715-2015, https://doi.org/10.5194/acp-15-5715-2015, 2015
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The present study uses aerosol optical depth as proxy to estimate 12 years of PM2.5 data for the Beijing central area and calculate the yearly premature mortality by different diseases attributable to PM2.5. The estimated average total mortality due to PM2.5 is about 5100 individuals/year for the period 2001--2012 in the Beijing central area, and the per capita mortality for all ages due to PM2.5 is around 15 per 10,000 person-years for the period 2010--2012.
A. Pozzer, A. de Meij, J. Yoon, H. Tost, A. K. Georgoulias, and M. Astitha
Atmos. Chem. Phys., 15, 5521–5535, https://doi.org/10.5194/acp-15-5521-2015, https://doi.org/10.5194/acp-15-5521-2015, 2015
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Thanks to numerical simulations and satellite observations, it is shown that aerosol optical depth (AOD) trends (2000--2010 period) over the US and Europe are due to emission decrease, while over the Sahara Desert and the Middle East they are due to meteorological changes. Over Southeast Asia, both meteorology and emission changes are important for the AOD trends.
It is shown that soluble components strongly influence AOD, as their contribution is enhanced by the aerosol water content.
R. H. H. Janssen and A. Pozzer
Geosci. Model Dev., 8, 453–471, https://doi.org/10.5194/gmd-8-453-2015, https://doi.org/10.5194/gmd-8-453-2015, 2015
R. Sander, P. Jöckel, O. Kirner, A. T. Kunert, J. Landgraf, and A. Pozzer
Geosci. Model Dev., 7, 2653–2662, https://doi.org/10.5194/gmd-7-2653-2014, https://doi.org/10.5194/gmd-7-2653-2014, 2014
K. Klingmüller, B. Steil, C. Brühl, H. Tost, and J. Lelieveld
Geosci. Model Dev., 7, 2503–2516, https://doi.org/10.5194/gmd-7-2503-2014, https://doi.org/10.5194/gmd-7-2503-2014, 2014
A. Novelli, K. Hens, C. Tatum Ernest, D. Kubistin, E. Regelin, T. Elste, C. Plass-Dülmer, M. Martinez, J. Lelieveld, and H. Harder
Atmos. Meas. Tech., 7, 3413–3430, https://doi.org/10.5194/amt-7-3413-2014, https://doi.org/10.5194/amt-7-3413-2014, 2014
J. Yoon and A. Pozzer
Atmos. Chem. Phys., 14, 10465–10482, https://doi.org/10.5194/acp-14-10465-2014, https://doi.org/10.5194/acp-14-10465-2014, 2014
A. G. Megaritis, C. Fountoukis, P. E. Charalampidis, H. A. C. Denier van der Gon, C. Pilinis, and S. N. Pandis
Atmos. Chem. Phys., 14, 10283–10298, https://doi.org/10.5194/acp-14-10283-2014, https://doi.org/10.5194/acp-14-10283-2014, 2014
E. Karnezi, I. Riipinen, and S. N. Pandis
Atmos. Meas. Tech., 7, 2953–2965, https://doi.org/10.5194/amt-7-2953-2014, https://doi.org/10.5194/amt-7-2953-2014, 2014
C. Fountoukis, A. G. Megaritis, K. Skyllakou, P. E. Charalampidis, C. Pilinis, H. A. C. Denier van der Gon, M. Crippa, F. Canonaco, C. Mohr, A. S. H. Prévôt, J. D. Allan, L. Poulain, T. Petäjä, P. Tiitta, S. Carbone, A. Kiendler-Scharr, E. Nemitz, C. O'Dowd, E. Swietlicki, and S. N. Pandis
Atmos. Chem. Phys., 14, 9061–9076, https://doi.org/10.5194/acp-14-9061-2014, https://doi.org/10.5194/acp-14-9061-2014, 2014
H. Bozem, H. Fischer, C. Gurk, C. L. Schiller, U. Parchatka, R. Koenigstedt, A. Stickler, M. Martinez, H. Harder, D. Kubistin, J. Williams, G. Eerdekens, and J. Lelieveld
Atmos. Chem. Phys., 14, 8917–8931, https://doi.org/10.5194/acp-14-8917-2014, https://doi.org/10.5194/acp-14-8917-2014, 2014
D. Y. Chang, H. Tost, B. Steil, and J. Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-21975-2014, https://doi.org/10.5194/acpd-14-21975-2014, 2014
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K. Hens, A. Novelli, M. Martinez, J. Auld, R. Axinte, B. Bohn, H. Fischer, P. Keronen, D. Kubistin, A. C. Nölscher, R. Oswald, P. Paasonen, T. Petäjä, E. Regelin, R. Sander, V. Sinha, M. Sipilä, D. Taraborrelli, C. Tatum Ernest, J. Williams, J. Lelieveld, and H. Harder
Atmos. Chem. Phys., 14, 8723–8747, https://doi.org/10.5194/acp-14-8723-2014, https://doi.org/10.5194/acp-14-8723-2014, 2014
A. K. Mishra, K. Klingmueller, E. Fredj, J. Lelieveld, Y. Rudich, and I. Koren
Atmos. Chem. Phys., 14, 7213–7231, https://doi.org/10.5194/acp-14-7213-2014, https://doi.org/10.5194/acp-14-7213-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
B. N. Murphy, N. M. Donahue, A. L. Robinson, and S. N. Pandis
Atmos. Chem. Phys., 14, 5825–5839, https://doi.org/10.5194/acp-14-5825-2014, https://doi.org/10.5194/acp-14-5825-2014, 2014
A. Bougiatioti, I. Stavroulas, E. Kostenidou, P. Zarmpas, C. Theodosi, G. Kouvarakis, F. Canonaco, A. S. H. Prévôt, A. Nenes, S. N. Pandis, and N. Mihalopoulos
Atmos. Chem. Phys., 14, 4793–4807, https://doi.org/10.5194/acp-14-4793-2014, https://doi.org/10.5194/acp-14-4793-2014, 2014
T. Christoudias, Y. Proestos, and J. Lelieveld
Atmos. Chem. Phys., 14, 4607–4616, https://doi.org/10.5194/acp-14-4607-2014, https://doi.org/10.5194/acp-14-4607-2014, 2014
G. W. Mann, K. S. Carslaw, C. L. Reddington, K. J. Pringle, M. Schulz, A. Asmi, D. V. Spracklen, D. A. Ridley, M. T. Woodhouse, L. A. Lee, K. Zhang, S. J. Ghan, R. C. Easter, X. Liu, P. Stier, Y. H. Lee, P. J. Adams, H. Tost, J. Lelieveld, S. E. Bauer, K. Tsigaridis, T. P. C. van Noije, A. Strunk, E. Vignati, N. Bellouin, M. Dalvi, C. E. Johnson, T. Bergman, H. Kokkola, K. von Salzen, F. Yu, G. Luo, A. Petzold, J. Heintzenberg, A. Clarke, J. A. Ogren, J. Gras, U. Baltensperger, U. Kaminski, S. G. Jennings, C. D. O'Dowd, R. M. Harrison, D. C. S. Beddows, M. Kulmala, Y. Viisanen, V. Ulevicius, N. Mihalopoulos, V. Zdimal, M. Fiebig, H.-C. Hansson, E. Swietlicki, and J. S. Henzing
Atmos. Chem. Phys., 14, 4679–4713, https://doi.org/10.5194/acp-14-4679-2014, https://doi.org/10.5194/acp-14-4679-2014, 2014
K. Skyllakou, B. N. Murphy, A. G. Megaritis, C. Fountoukis, and S. N. Pandis
Atmos. Chem. Phys., 14, 2343–2352, https://doi.org/10.5194/acp-14-2343-2014, https://doi.org/10.5194/acp-14-2343-2014, 2014
J. A. Adame, M. Martínez, M. Sorribas, P. J. Hidalgo, H. Harder, J.-M. Diesch, F. Drewnick, W. Song, J. Williams, V. Sinha, M. A. Hernández-Ceballos, J. Vilà-Guerau de Arellano, R. Sander, Z. Hosaynali-Beygi, H. Fischer, J. Lelieveld, and B. De la Morena
Atmos. Chem. Phys., 14, 2325–2342, https://doi.org/10.5194/acp-14-2325-2014, https://doi.org/10.5194/acp-14-2325-2014, 2014
C. Liu, S. Beirle, T. Butler, P. Hoor, C. Frankenberg, P. Jöckel, M. Penning de Vries, U. Platt, A. Pozzer, M. G. Lawrence, J. Lelieveld, H. Tost, and T. Wagner
Atmos. Chem. Phys., 14, 1717–1732, https://doi.org/10.5194/acp-14-1717-2014, https://doi.org/10.5194/acp-14-1717-2014, 2014
Y. F. Elshorbany, P. J. Crutzen, B. Steil, A. Pozzer, H. Tost, and J. Lelieveld
Atmos. Chem. Phys., 14, 1167–1184, https://doi.org/10.5194/acp-14-1167-2014, https://doi.org/10.5194/acp-14-1167-2014, 2014
D. Giannadaki, A. Pozzer, and J. Lelieveld
Atmos. Chem. Phys., 14, 957–968, https://doi.org/10.5194/acp-14-957-2014, https://doi.org/10.5194/acp-14-957-2014, 2014
P. Zanis, P. Hadjinicolaou, A. Pozzer, E. Tyrlis, S. Dafka, N. Mihalopoulos, and J. Lelieveld
Atmos. Chem. Phys., 14, 115–132, https://doi.org/10.5194/acp-14-115-2014, https://doi.org/10.5194/acp-14-115-2014, 2014
J. Yoon, A. Pozzer, P. Hoor, D. Y. Chang, S. Beirle, T. Wagner, S. Schloegl, J. Lelieveld, and H. M. Worden
Atmos. Chem. Phys., 13, 11307–11316, https://doi.org/10.5194/acp-13-11307-2013, https://doi.org/10.5194/acp-13-11307-2013, 2013
E. Regelin, H. Harder, M. Martinez, D. Kubistin, C. Tatum Ernest, H. Bozem, T. Klippel, Z. Hosaynali-Beygi, H. Fischer, R. Sander, P. Jöckel, R. Königstedt, and J. Lelieveld
Atmos. Chem. Phys., 13, 10703–10720, https://doi.org/10.5194/acp-13-10703-2013, https://doi.org/10.5194/acp-13-10703-2013, 2013
L. Ahlm, J. Julin, C. Fountoukis, S. N. Pandis, and I. Riipinen
Atmos. Chem. Phys., 13, 10271–10283, https://doi.org/10.5194/acp-13-10271-2013, https://doi.org/10.5194/acp-13-10271-2013, 2013
E. Kostenidou, C. Kaltsonoudis, M. Tsiflikiotou, E. Louvaris, L. M. Russell, and S. N. Pandis
Atmos. Chem. Phys., 13, 8797–8811, https://doi.org/10.5194/acp-13-8797-2013, https://doi.org/10.5194/acp-13-8797-2013, 2013
J. Lelieveld, C. Barlas, D. Giannadaki, and A. Pozzer
Atmos. Chem. Phys., 13, 7023–7037, https://doi.org/10.5194/acp-13-7023-2013, https://doi.org/10.5194/acp-13-7023-2013, 2013
A.C. Nölscher, E. Bourtsoukidis, B. Bonn, J. Kesselmeier, J. Lelieveld, and J. Williams
Biogeosciences, 10, 4241–4257, https://doi.org/10.5194/bg-10-4241-2013, https://doi.org/10.5194/bg-10-4241-2013, 2013
Q. J. Zhang, M. Beekmann, F. Drewnick, F. Freutel, J. Schneider, M. Crippa, A. S. H. Prevot, U. Baltensperger, L. Poulain, A. Wiedensohler, J. Sciare, V. Gros, A. Borbon, A. Colomb, V. Michoud, J.-F. Doussin, H. A. C. Denier van der Gon, M. Haeffelin, J.-C. Dupont, G. Siour, H. Petetin, B. Bessagnet, S. N. Pandis, A. Hodzic, O. Sanchez, C. Honoré, and O. Perrussel
Atmos. Chem. Phys., 13, 5767–5790, https://doi.org/10.5194/acp-13-5767-2013, https://doi.org/10.5194/acp-13-5767-2013, 2013
C. Brühl, J. Lelieveld, M. Höpfner, and H. Tost
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-11395-2013, https://doi.org/10.5194/acpd-13-11395-2013, 2013
Revised manuscript not accepted
G. J. Phillips, N. Pouvesle, J. Thieser, G. Schuster, R. Axinte, H. Fischer, J. Williams, J. Lelieveld, and J. N. Crowley
Atmos. Chem. Phys., 13, 1129–1139, https://doi.org/10.5194/acp-13-1129-2013, https://doi.org/10.5194/acp-13-1129-2013, 2013
E. Athanasopoulou, H. Vogel, B. Vogel, A. P. Tsimpidi, S. N. Pandis, C. Knote, and C. Fountoukis
Atmos. Chem. Phys., 13, 625–645, https://doi.org/10.5194/acp-13-625-2013, https://doi.org/10.5194/acp-13-625-2013, 2013
J. Lelieveld, M. G. Lawrence, and D. Kunkel
Atmos. Chem. Phys., 13, 31–34, https://doi.org/10.5194/acp-13-31-2013, https://doi.org/10.5194/acp-13-31-2013, 2013
A. Jugold, F. Althoff, M. Hurkuck, M. Greule, K. Lenhart, J. Lelieveld, and F. Keppler
Biogeosciences, 9, 5291–5301, https://doi.org/10.5194/bg-9-5291-2012, https://doi.org/10.5194/bg-9-5291-2012, 2012
V.-M. Kerminen, M. Paramonov, T. Anttila, I. Riipinen, C. Fountoukis, H. Korhonen, E. Asmi, L. Laakso, H. Lihavainen, E. Swietlicki, B. Svenningsson, A. Asmi, S. N. Pandis, M. Kulmala, and T. Petäjä
Atmos. Chem. Phys., 12, 12037–12059, https://doi.org/10.5194/acp-12-12037-2012, https://doi.org/10.5194/acp-12-12037-2012, 2012
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Evaluation of the COSMO model (v5.1) in polarimetric radar space – impact of uncertainties in model microphysics, retrievals and forward operators
Development of aerosol optical properties for improving the MESSy photolysis module in the GEM-MACH v2.4 air quality model and application for calculating photolysis rates in a biomass burning plume
The sensitivity of simulated aerosol climatic impact to domain size using regional model (WRF-Chem v3.6)
WOMBAT v1.0: a fully Bayesian global flux-inversion framework
Analysis of the MODIS above-cloud aerosol retrieval algorithm using MCARS
How well can inverse analyses of high-resolution satellite data resolve heterogeneous methane fluxes? Observing system simulation experiments with the GEOS-Chem adjoint model (v35)
Reduced-complexity air quality intervention modeling over China: the development of InMAPv1.6.1-China and a comparison with CMAQv5.2
High-resolution modeling of the distribution of surface air pollutants and their intercontinental transport by a global tropospheric atmospheric chemistry source–receptor model (GNAQPMS-SM)
Bulk hydrometeor optical properties for microwave and sub-millimetre radiative transfer in RTTOV-SCATT v13.0
The effect of accounting for public holidays on the skills of the atmospheric composition model SILAM v.5.7
Concurrent calculation of radiative transfer in the atmospheric simulation in ECHAM-6.3.05p2
A comparative study of two-way and offline coupled WRF v3.4 and CMAQ v5.0.2 over the contiguous US: performance evaluation and impacts of chemistry–meteorology feedbacks on air quality
Black carbon modeling in urban areas: investigating the influence of resuspension and non-exhaust emissions in streets using the Street-in-Grid model for inert particles (SinG-inert)
Evaluation of global EMEP MSC-W (rv4.34) WRF (v3.9.1.1) model surface concentrations and wet deposition of reactive N and S with measurements
The CHIMERE v2020r1 online chemistry-transport model
Verification of boundary layer wind patterns in COSMO-REA2 using clear-air radar echoes
Object-based analysis of simulated thunderstorms in Switzerland: application and validation of automated thunderstorm tracking with simulation data
Mineral dust cycle in the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (MONARCH) Version 2.0
FORest Canopy Atmosphere Transfer (FORCAsT) 2.0: model updates and evaluation with observations at a mixed forest site
Impact of Infrared Atmospheric Sounding Interferometer (IASI) thermal infrared measurements on global ozone reanalyses
Modeling sensitivities of BVOCs to different versions of MEGAN emission schemes in WRF-Chem (v3.6) and its impacts over eastern China
Influence on the temperature estimation of the planetary boundary layer scheme with different minimum eddy diffusivity in WRF v3.9.1.1
EuLerian Identification of Ascending air Streams (ELIAS 2.0) in Numerical Weather Prediction and Climate Models. Part II: Model application to different data sets
GCAP 2.0: a global 3-D chemical-transport model framework for past, present, and future climate scenarios
EuLerian Identification of ascending Air Streams (ELIAS 2.0) in Numerical Weather Prediction and Climate Models. Part I: Development of deep learning model
Incorporation of volcanic SO2 emissions in the Hemispheric CMAQ (H-CMAQ) version 5.2 modeling system and assessing their impacts on sulfate aerosol over the Northern Hemisphere
Model development in practice: A comprehensive update to the boundary layer schemes in HARMONIE-AROME cycle 40
Efficient ensemble generation for uncertain correlated parameters in atmospheric chemical models: a case study for biogenic emissions from EURAD-IM version 5
Position correction in dust storm forecasting using LOTOS-EUROS v2.1: grid-distorted data assimilation v1.0
The CAMS volcanic forecasting system utilizing near-real time data assimilation of S5P/TROPOMI SO2 retrievals
Atmosphere–ocean–aerosol–chemistry–climate model SOCOLv4.0: description and evaluation
Harmonized Emissions Component (HEMCO) 3.0 as a versatile emissions component for atmospheric models: application in the GEOS-Chem, NASA GEOS, WRF-GC, CESM2, NOAA GEFS-Aerosol, and NOAA UFS models
Mesoscale nesting interface of the PALM model system 6.0
Multi-sensor analyses of the skin temperature for the assimilation of satellite radiances in the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System (IFS, cycle 47R1)
The Grell–Freitas (GF) convection parameterization: recent developments, extensions, and applications
Calibrating a global atmospheric chemistry transport model using Gaussian process emulation and ground-level concentrations of ozone and carbon monoxide
The Aerosol Module in the Community Radiative Transfer Model (v2.2 and v2.3): accounting for aerosol transmittance effects on the radiance observation operator
Integration-based Extraction and Visualization of Jet Stream Cores
The Community Inversion Framework v1.0: a unified system for atmospheric inversion studies
WRF v.3.9 sensitivity to land surface model and horizontal resolution changes over North America
Representation of the Autoconversion from Cloud to Rain Using a Weighted Ensemble Approach
Modeling of land–surface interactions in the PALM model system 6.0: land surface model description, first evaluation, and sensitivity to model parameters
Improvements to the representation of BVOC chemistry–climate interactions in UKCA (v11.5) with the CRI-Strat 2 mechanism: incorporation and evaluation
Extension of a gaseous dry deposition algorithm to oxidized volatile organic compounds and hydrogen cyanide for application in chemistry transport models
iNRACM: incorporating 15N into the Regional Atmospheric Chemistry Mechanism (RACM) for assessing the role photochemistry plays in controlling the isotopic composition of NOx, NOy, and atmospheric nitrate
Latent Linear Adjustment Autoencoder v1.0: a novel method for estimating and emulating dynamic precipitation at high resolution
Deep-Learning Spatial Principles from Deterministic Chemical Transport Model for Chemical Reanalysis: An Application in China for PM2.5
Validation of the PALM model system 6.0 in a real urban environment: a case study in Dejvice, Prague, the Czech Republic
Data reduction for inverse modeling: an adaptive approach v1.0
Comparison of source apportionment approaches and analysis of non-linearity in a real case model application
Prabhakar Shrestha, Jana Mendrok, Velibor Pejcic, Silke Trömel, Ulrich Blahak, and Jacob T. Carlin
Geosci. Model Dev., 15, 291–313, https://doi.org/10.5194/gmd-15-291-2022, https://doi.org/10.5194/gmd-15-291-2022, 2022
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The article focuses on the exploitation of radar polarimetry for model evaluation of stratiform precipitation. The model exhibited a low bias in simulated polarimetric moments at lower levels above the melting layer where snow was found to dominate. This necessitates further research into the missing microphysical processes in these lower levels (e.g. fragmentation due to ice–ice collisions) and use of more reliable snow-scattering models in the forward operator to draw valid conclusions.
Mahtab Majdzadeh, Craig A. Stroud, Christopher Sioris, Paul A. Makar, Ayodeji Akingunola, Chris McLinden, Xiaoyi Zhao, Michael D. Moran, Ihab Abboud, and Jack Chen
Geosci. Model Dev., 15, 219–249, https://doi.org/10.5194/gmd-15-219-2022, https://doi.org/10.5194/gmd-15-219-2022, 2022
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A new lookup table for aerosol optical properties based on a Mie scattering code was calculated and adopted within an improved version of the photolysis module in the GEM-MACH in-line chemical transport model. The modified version of the photolysis module makes use of online interactive aerosol feedback and applies core-shell parameterizations to the black carbon absorption efficiency based on Bond et al. (2006) to the size bins with black carbon mass fraction of less than 40 %.
Xiaodong Wang, Chun Zhao, Mingyue Xu, Qiuyan Du, Jianqiu Zheng, Yun Bi, Shengfu Lin, and Yali Luo
Geosci. Model Dev., 15, 199–218, https://doi.org/10.5194/gmd-15-199-2022, https://doi.org/10.5194/gmd-15-199-2022, 2022
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Regional models are widely used to investigate aerosol climatic impacts. However, there are few studies examining the sensitivities of modeling results to regional domain size. In this study, the regional model is used to study the aerosol impacts on the East Asian summer monsoon system and focus on the modeling sensitivities to domain size. This study highlights the important impacts of domain size on regional modeling results of aerosol climatic impacts, which may not be limited to East Asia.
Andrew Zammit-Mangion, Michael Bertolacci, Jenny Fisher, Ann Stavert, Matthew Rigby, Yi Cao, and Noel Cressie
Geosci. Model Dev., 15, 45–73, https://doi.org/10.5194/gmd-15-45-2022, https://doi.org/10.5194/gmd-15-45-2022, 2022
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We present a framework for estimating the sources and sinks (flux) of carbon dioxide from satellite data. The framework is statistical and yields measures of uncertainty alongside all estimates of flux and other parameters in the underlying model. It also allows us to generate other insights, such as the size of errors and biases in the data. The primary aim of this research was to develop a fully statistical flux inversion framework for use by atmospheric scientists.
Galina Wind, Arlindo M. da Silva, Kerry G. Meyer, Steven Platnick, and Peter M. Norris
Geosci. Model Dev., 15, 1–14, https://doi.org/10.5194/gmd-15-1-2022, https://doi.org/10.5194/gmd-15-1-2022, 2022
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This is the third paper in series about the Multi-sensor Cloud and Aerosol Retrieval Simulator (MCARS). In this paper we use MCARS to create a set of constraints that might be used to assimilate a new above-cloud aerosol retrieval product developed for the MODIS instrument into a general circulation model. We executed the above-cloud aerosol retrieval over a series of synthetic MODIS granules and found the product to be of excellent quality.
Xueying Yu, Dylan B. Millet, and Daven K. Henze
Geosci. Model Dev., 14, 7775–7793, https://doi.org/10.5194/gmd-14-7775-2021, https://doi.org/10.5194/gmd-14-7775-2021, 2021
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We conduct observing system simulation experiments to test how well inverse analyses of high-resolution satellite data from sensors such as TROPOMI can quantify methane emissions. Inversions can improve monthly flux estimates at 25 km even with a spatially biased prior or model transport errors, but results are strongly degraded when both are present. We further evaluate a set of alternate formalisms to overcome limitations of the widely used scale factor approach that arise for missing sources.
Ruili Wu, Christopher W. Tessum, Yang Zhang, Chaopeng Hong, Yixuan Zheng, Xinyin Qin, Shigan Liu, and Qiang Zhang
Geosci. Model Dev., 14, 7621–7638, https://doi.org/10.5194/gmd-14-7621-2021, https://doi.org/10.5194/gmd-14-7621-2021, 2021
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Reduced-complexity air quality models are less computationally intensive and easier to use. We developed a reduced-complexity air quality Intervention Model for Air Pollution over China (InMAP-China) to rapidly predict the air quality and estimate the health impacts of emission sources in China. We believe that this work will be of great interest to a broad audience, including environmentalists in China and scientists in relevant fields at both national and local institutes.
Qian Ye, Jie Li, Xueshun Chen, Huansheng Chen, Wenyi Yang, Huiyun Du, Xiaole Pan, Xiao Tang, Wei Wang, Lili Zhu, Jianjun Li, Zhe Wang, and Zifa Wang
Geosci. Model Dev., 14, 7573–7604, https://doi.org/10.5194/gmd-14-7573-2021, https://doi.org/10.5194/gmd-14-7573-2021, 2021
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We developed a global tropospheric atmospheric chemistry source–receptor model. This model can quantify the contributions of multiple air pollutants from various source regions in one simulation without introducing the nonlinear error of atmospheric chemistry. The S-R relationships of PM2.5 and O3 from a global high-resolution (0.5° × 0.5°) simulation were given and compared with previous studies. This model will be useful for creating a link between the scientific community and policymakers.
Alan J. Geer, Peter Bauer, Katrin Lonitz, Vasileios Barlakas, Patrick Eriksson, Jana Mendrok, Amy Doherty, James Hocking, and Philippe Chambon
Geosci. Model Dev., 14, 7497–7526, https://doi.org/10.5194/gmd-14-7497-2021, https://doi.org/10.5194/gmd-14-7497-2021, 2021
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Satellite observations of radiation from the earth can have strong sensitivity to cloud and precipitation in the atmosphere, with applications in weather forecasting and the development of models. Computing the radiation received at the satellite sensor using radiative transfer theory requires a simulation of the optical properties of a volume containing a large number of cloud and precipitation particles. This article describes the physics used to generate these
bulkoptical properties.
Yalda Fatahi, Rostislav Kouznetsov, and Mikhail Sofiev
Geosci. Model Dev., 14, 7459–7475, https://doi.org/10.5194/gmd-14-7459-2021, https://doi.org/10.5194/gmd-14-7459-2021, 2021
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Incorporating information on public holidays into anthropogenic sector emissions results in substantial short-term improvement of the chemistry transport model SILAM scores. The largest impact was found for NOx, which is controlled by the changes in the traffic intensity. Certain improvements were also found for other species, but the signal was weaker than that for NOx.
Mohammad Reza Heidari, Zhaoyang Song, Enrico Degregori, Jörg Behrens, and Hendryk Bockelmann
Geosci. Model Dev., 14, 7439–7457, https://doi.org/10.5194/gmd-14-7439-2021, https://doi.org/10.5194/gmd-14-7439-2021, 2021
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To improve our understanding of climate system dynamics and their variability, the numerical atmospheric model ECHAM6 is used to simulate a complete glacial cycle over the past 120 000 years. However, performing such simulations takes a long time even on state-of-the-art supercomputers. To accelerate the model simulation, we propose calculating radiative transfer processes in parallel with adiabatic processes in the atmosphere, which reduces the simulation time by nearly half.
Kai Wang, Yang Zhang, Shaocai Yu, David C. Wong, Jonathan Pleim, Rohit Mathur, James T. Kelly, and Michelle Bell
Geosci. Model Dev., 14, 7189–7221, https://doi.org/10.5194/gmd-14-7189-2021, https://doi.org/10.5194/gmd-14-7189-2021, 2021
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The two-way coupled WRF-CMAQ model accounting for complex chemistry–meteorology feedbacks has been applied to the long-term predictions of regional meteorology and air quality over the US. The model results show superior performance and importance of chemistry–meteorology feedbacks when compared to the offline coupled WRF and CMAQ simulations, which suggests that feedbacks should be considered along with other factors in developing future model applications to inform policy making.
Lya Lugon, Jérémy Vigneron, Christophe Debert, Olivier Chrétien, and Karine Sartelet
Geosci. Model Dev., 14, 7001–7019, https://doi.org/10.5194/gmd-14-7001-2021, https://doi.org/10.5194/gmd-14-7001-2021, 2021
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The multiscale Street-in-Grid model is used to simulate black carbon (BC) concentrations in streets. To respect street-surface mass balance, particle resuspension is estimated with a new approach based on deposited mass. The contribution of resuspension is low, but non-exhaust emissions from tyre wear may largely contribute to BC concentrations. The impact of the two-way dynamic coupling between scales on BC concentrations varies depending on the street geometry and traffic emission intensity.
Yao Ge, Mathew R. Heal, David S. Stevenson, Peter Wind, and Massimo Vieno
Geosci. Model Dev., 14, 7021–7046, https://doi.org/10.5194/gmd-14-7021-2021, https://doi.org/10.5194/gmd-14-7021-2021, 2021
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This study reports the first evaluation of the global EMEP MSC-W ACTM driven by WRF meteorology, with a focus on surface concentrations and wet deposition of reactive N and S species. The model–measurement comparison is conducted both spatially and temporally, covering 10 monitoring networks worldwide. The statistics from the comprehensive evaluations presented in this study support the application of this model framework for global analysis of the budgets and fluxes of reactive N and SIA.
Laurent Menut, Bertrand Bessagnet, Régis Briant, Arineh Cholakian, Florian Couvidat, Sylvain Mailler, Romain Pennel, Guillaume Siour, Paolo Tuccella, Solène Turquety, and Myrto Valari
Geosci. Model Dev., 14, 6781–6811, https://doi.org/10.5194/gmd-14-6781-2021, https://doi.org/10.5194/gmd-14-6781-2021, 2021
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The CHIMERE chemistry-transport model is presented in its new version, V2020r1. Many changes are proposed compared to the previous version. These include online modeling, new parameterizations for aerosols, new emissions schemes, a new parameter file format, the subgrid-scale variability of urban concentrations and new transport schemes.
Sebastian Buschow and Petra Friederichs
Geosci. Model Dev., 14, 6765–6780, https://doi.org/10.5194/gmd-14-6765-2021, https://doi.org/10.5194/gmd-14-6765-2021, 2021
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When insects fill the lower kilometers of the atmosphere, they get caught in the convergent parts of the wind field. Their concentration visualizes the otherwise invisible circulation on radar images. This study shows how clear-air radar data can be compared to simulated wind fields in terms of scale, anisotropy, and direction. Despite known difficulties with simulating these near-surface wind systems, we find decent agreement between a long-term simulation and the German radar mosaic.
Timothy H. Raupach, Andrey Martynov, Luca Nisi, Alessandro Hering, Yannick Barton, and Olivia Martius
Geosci. Model Dev., 14, 6495–6514, https://doi.org/10.5194/gmd-14-6495-2021, https://doi.org/10.5194/gmd-14-6495-2021, 2021
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When simulated thunderstorms are compared to observations or other simulations, a match between overall storm properties is often more important than exact matches to individual storms. We tested a comparison method that uses a thunderstorm tracking algorithm to characterise simulated storms. For May 2018 in Switzerland, the method produced reasonable matches to independent observations for most storm properties, showing its feasibility for summarising simulated storms over mountainous terrain.
Martina Klose, Oriol Jorba, María Gonçalves Ageitos, Jeronimo Escribano, Matthew L. Dawson, Vincenzo Obiso, Enza Di Tomaso, Sara Basart, Gilbert Montané Pinto, Francesca Macchia, Paul Ginoux, Juan Guerschman, Catherine Prigent, Yue Huang, Jasper F. Kok, Ron L. Miller, and Carlos Pérez García-Pando
Geosci. Model Dev., 14, 6403–6444, https://doi.org/10.5194/gmd-14-6403-2021, https://doi.org/10.5194/gmd-14-6403-2021, 2021
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Mineral soil dust is a major atmospheric airborne particle type. We present and evaluate MONARCH, a model used for regional and global dust-weather prediction. An important feature of the model is that it allows different approximations to represent dust, ranging from more simplified to more complex treatments. Using these different treatments, MONARCH can help us better understand impacts of dust in the Earth system, such as its interactions with radiation.
Dandan Wei, Hariprasad D. Alwe, Dylan B. Millet, Brandon Bottorff, Michelle Lew, Philip S. Stevens, Joshua D. Shutter, Joshua L. Cox, Frank N. Keutsch, Qianwen Shi, Sarah C. Kavassalis, Jennifer G. Murphy, Krystal T. Vasquez, Hannah M. Allen, Eric Praske, John D. Crounse, Paul O. Wennberg, Paul B. Shepson, Alexander A. T. Bui, Henry W. Wallace, Robert J. Griffin, Nathaniel W. May, Megan Connor, Jonathan H. Slade, Kerri A. Pratt, Ezra C. Wood, Mathew Rollings, Benjamin L. Deming, Daniel C. Anderson, and Allison L. Steiner
Geosci. Model Dev., 14, 6309–6329, https://doi.org/10.5194/gmd-14-6309-2021, https://doi.org/10.5194/gmd-14-6309-2021, 2021
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Over the past decade, understanding of isoprene oxidation has improved, and proper representation of isoprene oxidation and isoprene-derived SOA (iSOA) formation in canopy–chemistry models is now recognized to be important for an accurate understanding of forest–atmosphere exchange. The updated FORCAsT version 2.0 improves the estimation of some isoprene oxidation products and is one of the few canopy models currently capable of simulating SOA formation from monoterpenes and isoprene.
Emanuele Emili and Mohammad El Aabaribaoune
Geosci. Model Dev., 14, 6291–6308, https://doi.org/10.5194/gmd-14-6291-2021, https://doi.org/10.5194/gmd-14-6291-2021, 2021
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This study presents the latest version of the global ozone reanalysis product developed at Cerfacs. The reanalysis is based on the assimilation of satellite data from the Infrared Atmospheric Sounding Interferometer (IASI) in the Météo-France chemical transport model. The results show that the quality of the ozone fields is comparable to current state-of-the-art systems and suggest that IASI provides useful information for ozone reanalyses, especially in the upper troposphere.
Mingshuai Zhang, Chun Zhao, Yuhan Yang, Qiuyan Du, Yonglin Shen, Shengfu Lin, Dasa Gu, Wenjing Su, and Cheng Liu
Geosci. Model Dev., 14, 6155–6175, https://doi.org/10.5194/gmd-14-6155-2021, https://doi.org/10.5194/gmd-14-6155-2021, 2021
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Biogenic volatile organic compounds (BVOCs) can influence atmospheric chemistry and secondary pollutant formation. This study examines the performance of different versions of the Model of Emissions of Gases and Aerosols from Nature (MEGAN) in modeling BVOCs and ozone and their sensitivities to vegetation distributions over eastern China. The results suggest more accurate vegetation distribution and measurements of BVOC emission fluxes are needed to reduce the uncertainties.
Hongyi Ding, Le Cao, Haimei Jiang, Wenxing Jia, Yong Chen, and Junling An
Geosci. Model Dev., 14, 6135–6153, https://doi.org/10.5194/gmd-14-6135-2021, https://doi.org/10.5194/gmd-14-6135-2021, 2021
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We performed a WRF model study to figure out the mechanism of how the change in minimum eddy diffusivity (Kzmin) in the planetary boundary layer (PBL) closure scheme (ACM2) affects the simulated near-surface temperature in Beijing, China. Moreover, the influence of changing Kzmin on the temperature prediction in areas with different land-use categories was studied. The model performance using a functional-type Kzmin for capturing the temperature change in this area was also clarified.
Julian Francesco Quinting, Christian Michael Grams, Annika Oertel, and Moritz Pickl
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-278, https://doi.org/10.5194/gmd-2021-278, 2021
Revised manuscript accepted for GMD
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This study applies novel artificial intelligence-based models which allow the identification of one specific weather system which affects the midlatitude circulation. We show that the models yield similar results as their trajectory-based counterpart which requires data at higher spatio-temporal resolution and is computationally more expensive. Overall, we aim to show how deep learning methods can be used efficiently to support process-understanding of biases in weather prediction models.
Lee T. Murray, Eric M. Leibensperger, Clara Orbe, Loretta J. Mickley, and Melissa Sulprizio
Geosci. Model Dev., 14, 5789–5823, https://doi.org/10.5194/gmd-14-5789-2021, https://doi.org/10.5194/gmd-14-5789-2021, 2021
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Chemical-transport models are tools used to study air pollution and inform public policy. However, they are limited by the availability of archived meteorology. Here, we describe how the GEOS-Chem chemical-transport model may now be driven by meteorology archived from a state-of-the-art general circulation model for past and future climates, allowing it to be used to explore the impact of climate change on air pollution and atmospheric composition.
Julian Francesco Quinting and Christian M. Grams
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-276, https://doi.org/10.5194/gmd-2021-276, 2021
Revised manuscript accepted for GMD
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Physical processes in weather systems importantly affect the midlatitude large-scale circulation. This study introduces an artificial intelligence-based framework which allows the identification of an important weather system – the so-called warm conveyor belt – at comparably low computational costs and from data at low spatial and temporal resolution. The framework thus newly enables the systematic investigation of WCBs in large data sets such as climate model projections.
Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, Sergey L. Napelenok, and Yang Zhang
Geosci. Model Dev., 14, 5751–5768, https://doi.org/10.5194/gmd-14-5751-2021, https://doi.org/10.5194/gmd-14-5751-2021, 2021
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The Community Multiscale Air Quality (CMAQ) modeling system extended for hemispheric-scale applications (H-CMAQ) incorporated the satellite-constrained degassing SO2 emissions from 50 volcanos across the Northern Hemisphere. The impact on tropospheric sulfate aerosol (SO42−) is assessed for 2010. Although the considered volcanic emissions occurred at or below the middle of free troposphere (500 hPa), SO42− enhancements of more than 10 % were detected up to the top of free troposphere (250 hPa).
Wim C. de Rooy, Pier Siebesma, Peter Baas, Geert Lenderink, Stephan de Roode, Hylke de Vries, Erik van Meijgaard, Jan Fokke Meirink, Sander Tijm, and Bram van 't Veen
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-184, https://doi.org/10.5194/gmd-2021-184, 2021
Revised manuscript accepted for GMD
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This paper describes a comprehensive model update to the boundary-layer schemes. Because the involved parameterisations are all built on widely applied frameworks, the here described modifications are applicable to many NWP and climate models. The model update contains substantial modifications to the cloud, turbulence and convection schemes and leads to a substantial improvement on several aspects of the model, especially low cloud forecasts.
Annika Vogel and Hendrik Elbern
Geosci. Model Dev., 14, 5583–5605, https://doi.org/10.5194/gmd-14-5583-2021, https://doi.org/10.5194/gmd-14-5583-2021, 2021
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While atmospheric chemical forecasts rely on uncertain model parameters, their huge dimensions hamper an efficient uncertainty estimation. This study presents a novel approach to efficiently sample these uncertainties by extracting dominant dependencies and correlations. Applying the algorithm to biogenic emissions, their uncertainties can be estimated from a low number of dominant components. This states the capability of an efficient treatment of parameter uncertainties in atmospheric models.
Jianbing Jin, Arjo Segers, Hai Xiang Lin, Bas Henzing, Xiaohui Wang, Arnold Heemink, and Hong Liao
Geosci. Model Dev., 14, 5607–5622, https://doi.org/10.5194/gmd-14-5607-2021, https://doi.org/10.5194/gmd-14-5607-2021, 2021
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When discussing the accuracy of a dust forecast, the shape and position of the plume as well as the intensity are key elements. The position forecast determines which locations will be affected, while the intensity only describes the actual dust level. A dust forecast with position misfit directly results in incorrect timing profiles of dust loads. In this paper, an image-morphing-based data assimilation is designed for realigning a simulated dust plume to correct for the position error.
Antje Inness, Melanie Ades, Dimitris Balis, Dmitry Efremenko, Johannes Flemming, Pascal Hedelt, Maria-Elissavet Koukouli, Diego Loyola, and Roberto Ribas
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-219, https://doi.org/10.5194/gmd-2021-219, 2021
Revised manuscript accepted for GMD
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This paper describes the way the Copernicus Atmosphere Monitoring Service (CAMS) produces forecasts of volcanic SO2. These forecast are provided routinely every day. They are cerated by blending SO2 data from satellite instruments (TROPOMI and GOME-2) with the CAMS model. We show that the quality of the CAMS SO2 forecasts can be improved if additional information about the height of volcanic plumes is provided in the satellite data.
Timofei Sukhodolov, Tatiana Egorova, Andrea Stenke, William T. Ball, Christina Brodowsky, Gabriel Chiodo, Aryeh Feinberg, Marina Friedel, Arseniy Karagodin-Doyennel, Thomas Peter, Jan Sedlacek, Sandro Vattioni, and Eugene Rozanov
Geosci. Model Dev., 14, 5525–5560, https://doi.org/10.5194/gmd-14-5525-2021, https://doi.org/10.5194/gmd-14-5525-2021, 2021
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This paper features the new atmosphere–ocean–aerosol–chemistry–climate model SOCOLv4.0 and its validation. The model performance is evaluated against reanalysis products and observations of atmospheric circulation and trace gas distribution, with a focus on stratospheric processes. Although we identified some problems to be addressed in further model upgrades, we demonstrated that SOCOLv4.0 is already well suited for studies related to chemistry–climate–aerosol interactions.
Haipeng Lin, Daniel J. Jacob, Elizabeth W. Lundgren, Melissa P. Sulprizio, Christoph A. Keller, Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Patrick C. Campbell, Barry Baker, Rick D. Saylor, and Raffaele Montuoro
Geosci. Model Dev., 14, 5487–5506, https://doi.org/10.5194/gmd-14-5487-2021, https://doi.org/10.5194/gmd-14-5487-2021, 2021
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Emissions are a central component of atmospheric chemistry models. The Harmonized Emissions Component (HEMCO) is a software component for computing emissions from a user-selected ensemble of emission inventories and algorithms. It allows users to select, add, and scale emissions from different sources through a configuration file with no change to the model source code. We demonstrate the implementation of HEMCO in several models, all sharing the same HEMCO core code and database library.
Eckhard Kadasch, Matthias Sühring, Tobias Gronemeier, and Siegfried Raasch
Geosci. Model Dev., 14, 5435–5465, https://doi.org/10.5194/gmd-14-5435-2021, https://doi.org/10.5194/gmd-14-5435-2021, 2021
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In this paper, we provide a technical description of a newly developed interface for coupling the PALM model system 6.0 to the weather prediction model COSMO. The interface allows users of PALM to simulate the detailed atmospheric flow for relatively small regions of tens of kilometres under specific weather conditions, for instance, periods around observation campaigns or extreme weather situations. We demonstrate the interface using a benchmark simulation.
Sebastien Massart, Niels Bormann, Massimo Bonavita, and Cristina Lupu
Geosci. Model Dev., 14, 5467–5485, https://doi.org/10.5194/gmd-14-5467-2021, https://doi.org/10.5194/gmd-14-5467-2021, 2021
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Numerical weather predictions combine data from satellites with atmospheric forecasts. Some satellites measure the radiance emitted by the Earth's surface. To use this data, one must have knowledge of the surface properties, like the temperature of the thin layer above the surface. Error in this temperature leads to a misuse of the satellite data and affects the quality of the weather forecast. We updated our approach to better estimate this temperature, which should help improve the forecast.
Saulo R. Freitas, Georg A. Grell, and Haiqin Li
Geosci. Model Dev., 14, 5393–5411, https://doi.org/10.5194/gmd-14-5393-2021, https://doi.org/10.5194/gmd-14-5393-2021, 2021
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Convection parameterization (CP) is a component of atmospheric models aiming to represent the statistical effects of subgrid-scale convective clouds. Because the atmosphere contains circulations with a broad spectrum of scales, the truncation needed to run models in computers requires the introduction of parameterizations to account for processes that are not explicitly resolved. We detail recent developments in the Grell–Freitas CP, which has been applied in several regional and global models.
Edmund Ryan and Oliver Wild
Geosci. Model Dev., 14, 5373–5391, https://doi.org/10.5194/gmd-14-5373-2021, https://doi.org/10.5194/gmd-14-5373-2021, 2021
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Atmospheric chemistry transport models are important tools to investigate the local, regional and global controls on atmospheric composition and air quality. In this study, we estimate some of the model parameters using machine learning and statistics. Our findings identify the level of error and spatial coverage in the O2 and CO data that are needed to achieve good parameter estimates. We also highlight the benefits of using multiple constraints to calibrate atmospheric chemistry models.
Cheng-Hsuan Lu, Quanhua Liu, Shih-Wei Wei, Benjamin T. Johnson, Cheng Dang, Patrick G. Stegmann, Dustin Grogan, Guoqing Ge, and Ming Hu
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-145, https://doi.org/10.5194/gmd-2021-145, 2021
Revised manuscript accepted for GMD
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This article is a technical note on the aerosol absorption and scattering calculations of the Community Radiative Transfer Model (CRTM) v2.2 and v2.3. It also provides guidance for prospective users of the CRTM aerosol option and Gridpoint Statistical Interpolation (GSI) aerosol-aware radiance assimilation. Scientific aspects of aerosol-affected BT in atmospheric data assimilation are also briefly discussed.
Lukas Bösiger, Michael Sprenger, Maxi Böttcher, Hanna Joos, and Tobias Günther
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-240, https://doi.org/10.5194/gmd-2021-240, 2021
Revised manuscript accepted for GMD
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Jet streams are coherent air flows that interact with atmospheric structures such as warm conveyor belts (WCBs) and the tropopause. Individually, these structures have a significant impact on the weather evolution. A first step towards a deeper understanding of the meteorological processes is to extract jet stream corelines, for which we develop a novel feature extraction algorithm. Based on the line geometry, we automatically detect and visualize potential interactions between WCBs and jets.
Antoine Berchet, Espen Sollum, Rona L. Thompson, Isabelle Pison, Joël Thanwerdas, Grégoire Broquet, Frédéric Chevallier, Tuula Aalto, Adrien Berchet, Peter Bergamaschi, Dominik Brunner, Richard Engelen, Audrey Fortems-Cheiney, Christoph Gerbig, Christine D. Groot Zwaaftink, Jean-Matthieu Haussaire, Stephan Henne, Sander Houweling, Ute Karstens, Werner L. Kutsch, Ingrid T. Luijkx, Guillaume Monteil, Paul I. Palmer, Jacob C. A. van Peet, Wouter Peters, Philippe Peylin, Elise Potier, Christian Rödenbeck, Marielle Saunois, Marko Scholze, Aki Tsuruta, and Yuanhong Zhao
Geosci. Model Dev., 14, 5331–5354, https://doi.org/10.5194/gmd-14-5331-2021, https://doi.org/10.5194/gmd-14-5331-2021, 2021
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We present here the Community Inversion Framework (CIF) to help rationalize development efforts and leverage the strengths of individual inversion systems into a comprehensive framework. The CIF is a programming protocol to allow various inversion bricks to be exchanged among researchers.
The ensemble of bricks makes a flexible, transparent and open-source Python-based tool. We describe the main structure and functionalities and demonstrate it in a simple academic case.
Almudena García-García, Francisco José Cuesta-Valero, Hugo Beltrami, Fidel González-Rouco, and Elena García-Bustamante
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-243, https://doi.org/10.5194/gmd-2021-243, 2021
Revised manuscript accepted for GMD
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We study the sensitivity of a regional climate model to resolution and soil scheme changes. Our results show that the use of finer resolutions mainly affects precipitation outputs, particularly in summer due to changes in convective processes. Finer resolutions are associated with larger biases in comparison with observations. Changing the LSM scheme greatly affects the simulation of near-surface temperatures, yielding the lowest biases in mean temperature with the most complex soil scheme.
Jinfang Yin, Xudong Liang, Hong Wang, and Haile Xue
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-230, https://doi.org/10.5194/gmd-2021-230, 2021
Revised manuscript accepted for GMD
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An ensemble (EN) approach was designed to improving autoconversion (ATC) from cloud water to rainwater in cloud microphysics schemes. One unique feature of the EN approach is that the ATC rate is a mean value based on the calculations from several widely used ATC schemes. The ensemble approach proposed herein appears to be helpful for improving the representation of cloud and precipitation processes in weather and climate models.
Katrin Frieda Gehrke, Matthias Sühring, and Björn Maronga
Geosci. Model Dev., 14, 5307–5329, https://doi.org/10.5194/gmd-14-5307-2021, https://doi.org/10.5194/gmd-14-5307-2021, 2021
James Weber, Scott Archer-Nicholls, Nathan Luke Abraham, Youngsub M. Shin, Thomas J. Bannan, Carl J. Percival, Asan Bacak, Paulo Artaxo, Michael Jenkin, M. Anwar H. Khan, Dudley E. Shallcross, Rebecca H. Schwantes, Jonathan Williams, and Alex T. Archibald
Geosci. Model Dev., 14, 5239–5268, https://doi.org/10.5194/gmd-14-5239-2021, https://doi.org/10.5194/gmd-14-5239-2021, 2021
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The new mechanism CRI-Strat 2 features state-of-the-art isoprene chemistry not previously available in UKCA and improves UKCA's ability to reproduce observed concentrations of isoprene, monoterpenes, and OH in tropical regions. The enhanced ability to model isoprene, the most widely emitted non-methane volatile organic compound (VOC), will allow understanding of how isoprene and other biogenic VOCs affect atmospheric composition and, through biosphere–atmosphere feedbacks, climate change.
Zhiyong Wu, Leiming Zhang, John T. Walker, Paul A. Makar, Judith A. Perlinger, and Xuemei Wang
Geosci. Model Dev., 14, 5093–5105, https://doi.org/10.5194/gmd-14-5093-2021, https://doi.org/10.5194/gmd-14-5093-2021, 2021
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A community dry deposition algorithm for modeling the gaseous dry deposition process in chemistry transport models was extended to include an additional 12 oxidized volatile organic compounds and hydrogen cyanide based on their physicochemical properties and was then evaluated using field flux measurements over a mixed forest. This study provides a useful tool that is needed in chemistry transport models with increasing complexity for simulating an important atmospheric process.
Huan Fang, Wendell W. Walters, David Mase, and Greg Michalski
Geosci. Model Dev., 14, 5001–5022, https://doi.org/10.5194/gmd-14-5001-2021, https://doi.org/10.5194/gmd-14-5001-2021, 2021
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A new photochemical reaction scheme that incorporates nitrogen isotopes has been developed to simulate isotope tracers in air pollution. The model contains 16 N compounds, and 96 reactions involving N used in the Regional Atmospheric Chemistry Mechanism (RACM) were replicated using 15N in a new mechanism called iNRACM. The model is able to predict d15N variations in NOx, HONO, and HNO3 that are similar to those observed in aerosol and gases in the troposphere.
Christina Heinze-Deml, Sebastian Sippel, Angeline G. Pendergrass, Flavio Lehner, and Nicolai Meinshausen
Geosci. Model Dev., 14, 4977–4999, https://doi.org/10.5194/gmd-14-4977-2021, https://doi.org/10.5194/gmd-14-4977-2021, 2021
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Quantifying dynamical and thermodynamical components of regional precipitation change is a key challenge in climate science. We introduce a novel statistical model (Latent Linear Adjustment Autoencoder) that combines the flexibility of deep neural networks with the robustness advantages of linear regression. The method enables estimation of the contribution of a coarse-scale atmospheric circulation proxy to daily precipitation at high resolution and in a spatially coherent manner.
Baolei Lyu, Ran Huang, Xinlu Wang, Weiguo Wang, and Yongtao Hu
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-253, https://doi.org/10.5194/gmd-2021-253, 2021
Revised manuscript accepted for GMD
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Data fusion is to estimate spatially completed and smooth reanalysis fields from multiple data sources of observations and model simulations. We developed a well-designed deep learning model framework to embed spatial correlation principles. The model has very high accuracy to predict reanalysis data fields from isolated observation data points. Besides, it is also feasible for operational applications due to computational efficiency.
Jaroslav Resler, Kryštof Eben, Jan Geletič, Pavel Krč, Martin Rosecký, Matthias Sühring, Michal Belda, Vladimír Fuka, Tomáš Halenka, Peter Huszár, Jan Karlický, Nina Benešová, Jana Ďoubalová, Kateřina Honzáková, Josef Keder, Šárka Nápravníková, and Ondřej Vlček
Geosci. Model Dev., 14, 4797–4842, https://doi.org/10.5194/gmd-14-4797-2021, https://doi.org/10.5194/gmd-14-4797-2021, 2021
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We describe validation of the PALM model v6.0 against measurements collected during two observational campaigns in Dejvice, Prague. The study focuses on the evaluation of the newly developed or improved radiative and energy balance modules in PALM related to urban modelling. In addition to the energy-related quantities, it also evaluates air flow and air quality under street canyon conditions.
Xiaoling Liu, August L. Weinbren, He Chang, Jovan M. Tadić, Marikate E. Mountain, Michael E. Trudeau, Arlyn E. Andrews, Zichong Chen, and Scot M. Miller
Geosci. Model Dev., 14, 4683–4696, https://doi.org/10.5194/gmd-14-4683-2021, https://doi.org/10.5194/gmd-14-4683-2021, 2021
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Observations of greenhouse gases have become far more numerous in recent years due to new satellite observations. The sheer size of these datasets makes it challenging to incorporate these data into statistical models and use these data to estimate greenhouse gas sources and sinks. In this paper, we develop an approach to reduce the size of these datasets while preserving the most information possible. We subsequently test this approach using satellite observations of carbon dioxide.
Claudio A. Belis, Guido Pirovano, Maria Gabriella Villani, Giuseppe Calori, Nicola Pepe, and Jean Philippe Putaud
Geosci. Model Dev., 14, 4731–4750, https://doi.org/10.5194/gmd-14-4731-2021, https://doi.org/10.5194/gmd-14-4731-2021, 2021
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The study presents an in-depth analysis of the implications that using different CTM source apportionment approaches (tagged species and brute force) have for the source allocation of secondary inorganic aerosol, an important component of PM10 and PM2.5. A set of runs combining different emission levels and models was carried out, aiming to describe the situations in which strong non-linearity may lead the two approaches to deliver different results and when they are expected to be comparable.
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