Articles | Volume 11, issue 10
https://doi.org/10.5194/gmd-11-4021-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/gmd-11-4021-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Development and technical paper
| 
05 Oct 2018
Development and technical paper |
| 05 Oct 2018
Implementation of a comprehensive ice crystal formation parameterization for cirrus and mixed-phase clouds in the EMAC model (based on MESSy 2.53)
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
Sylvia C. Sullivan
School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, USA
Vlassis A. Karydis
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
now at: Institute for Energy and Climate Research – 8, Forschungszentrum Jülich, Jülich, Germany
Donifan Barahona
NASA Goddard Space Flight Center, Greenbelt, Maryland, USA
Martina Krämer
Institute for Energy and Climate Research – 7, Forschungszentrum Jülich, Jülich, Germany
Athanasios Nenes
School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, USA
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, USA
ICE-HT, Foundation for Research and Technology, Hellas, Greece
IERSD, National Observatory of Athens, Athens, Greece
Laboratory of Atmospheric Processes and Their Impacts, École Polytechnique Fédérale de Lausanne, Lausanne, Switzerland
Holger Tost
Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, Germany
Alexandra P. Tsimpidi
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
Jos Lelieveld
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
Energy, Environment and Water Research Center, The Cyprus Institute, Nicosia, Cyprus
Andrea Pozzer
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
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Imran A. Girach, Narendra Ojha, Prabha R. Nair, Kandula V. Subrahmanyam, Neelakantan Koushik, Mohammed M. Nazeer, Nadimpally Kiran Kumar, Surendran Nair Suresh Babu, Jos Lelieveld, and Andrea Pozzer
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Seyed Omid Nabavi, Theodoros Christoudias, Yiannis Proestos, Christos Fountoukis, Huda Al-Sulaiti, and Jos Lelieveld
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Sylvia Sullivan, Behrooz Keshtgar, Nicole Albern, Elzina Bala, Christoph Braun, Anubhav Choudhary, Johannes Hörner, Hilke Lentink, Georgios Papavasileiou, and Aiko Voigt
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Clouds absorb and re-emit infrared radiation from Earth's surface and absorb and reflect incoming solar radiation. As a result, they change atmospheric temperature gradients that drive large-scale circulation. To better simulate this circulation, we study how the radiative heating and cooling from clouds depends on model settings like grid spacing; whether we describe convection approximately or exactly; and the level of detail used to describe small-scale processes, or microphysics, in clouds.
Sara Bacer, Julien Beaumet, Martin Ménégoz, Hubert Gallée, Enzo Le Bouëdec, and Chantal Staquet
EGUsphere, https://doi.org/10.5194/egusphere-2023-1199, https://doi.org/10.5194/egusphere-2023-1199, 2023
Short summary
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The impact of climate change on cold-air pools (CAPs) is studied until 2100 for the Grenoble valleys. The CAP atmospheric stability is analysed statistically using data from a regional climate model for two scenarios. Only for SSP5-8.5 does the stability in the CAP slightly vary, decaying by 0.6 K/km over 100 years. The CAP structure is addressed for two similar episodes in 1988 and 2043: the air temperature is about 4 K higher in 2043 with similar valley heat deficit but stronger stability.
Blaž Gasparini, Sylvia C. Sullivan, Adam B. Sokol, Bernd Kärcher, Eric Jensen, and Dennis L. Hartmann
EGUsphere, https://doi.org/10.5194/egusphere-2023-1214, https://doi.org/10.5194/egusphere-2023-1214, 2023
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Tropical cirrus clouds are essential for the climate, but our understanding of these clouds is limited due to their dependence on a wide range of small- and large-scale climate processes. In this Opinion, we review recent advances in the study of tropical cirrus clouds, highlight remaining open questions, and discuss what we can do to resolve them.
Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Nicole Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg McFarquhar, Jens Redemann, Arther J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema
EGUsphere, https://doi.org/10.5194/egusphere-2023-886, https://doi.org/10.5194/egusphere-2023-886, 2023
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To better understand smoke properties and its interactions with clouds, we compare WRF-CAM5 with observations from ORACLES, CLARIFY, and LASIC field campaigns in the Southeastern Atlantic in August 2017. The model transports and mixes smoke well but is not fully capturing some important processes. These include smoke chemical and physical aging over 4–12 days, smoke removal by rain, new particle formation, aerosol activation into cloud droplets, and boundary layer turbulence.
Zaneta Hamryszczak, Antonia Hartmann, Dirk Dienhart, Sascha Hafermann, Bettina Brendel, Rainer Königstedt, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-114, https://doi.org/10.5194/amt-2023-114, 2023
Revised manuscript accepted for AMT
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Edward Groot and Holger Tost
Atmos. Chem. Phys., 23, 6065–6081, https://doi.org/10.5194/acp-23-6065-2023, https://doi.org/10.5194/acp-23-6065-2023, 2023
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It is shown that the outflow from cumulonimbus clouds or thunderstorms in the upper troposphere and lower stratosphere in idealized high-resolution simulations (LESs) depends linearly on the net amount of latent heat released by the cloud for fixed geometry of the clouds. However, it is shown that, in more realistic situations, convective organization and aggregation (collecting mechanisms of cumulonimbus clouds) affect the amount of outflow non-linearly through non-idealized geometry.
Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev., 16, 3013–3028, https://doi.org/10.5194/gmd-16-3013-2023, https://doi.org/10.5194/gmd-16-3013-2023, 2023
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Zaneta Hamryszczak, Dirk Dienhart, Bettina Brendel, Roland Rohloff, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Birger Bohn, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 5929–5943, https://doi.org/10.5194/acp-23-5929-2023, https://doi.org/10.5194/acp-23-5929-2023, 2023
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Hydrogen peroxide is a key contributor to the oxidative chemistry of the atmosphere through its link to the most prominent oxidants controlling its self-cleansing capacity, HOx. During the CAFE-Africa campaign, H2O2 was measured over the Atlantic Ocean and western Africa in August/September 2018. The study gives an overview of the distribution of H2O2 in the upper tropical troposphere and investigates the impact of convective processes in the Intertropical Convergence Zone on the budget of H2O2.
Irene Bartolomé García, Odran Sourdeval, Reinhold Spang, and Martina Krämer
EGUsphere, https://doi.org/10.5194/egusphere-2023-754, https://doi.org/10.5194/egusphere-2023-754, 2023
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Ghislain Motos, Gabriel Freitas, Paraskevi Georgakaki, Jörg Wieder, Guangyu Li, Wenche Aas, Chris Lunder, Radovan Krejci, Julie Therese Pasquier, Jan Henneberger, Robert Oscar David, Christoph Ritter, Claudia Mohr, Paul Zieger, and Athanasios Nenes
EGUsphere, https://doi.org/10.5194/egusphere-2023-530, https://doi.org/10.5194/egusphere-2023-530, 2023
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Low-altitude clouds play a key role in regulating the climate of the Arctic, a region that suffers from climate change more than any other on the planet. We gathered meteorological and aerosol physical and chemical data over a year and utilized them for a parameterization that help us unravel the factors driving and limiting the efficiency of cloud droplet formation. We then linked these information to the sources of aerosol found during each season and to processes of cloud glaciation.
Clara M. Nussbaumer, Horst Fischer, Jos Lelieveld, and Andrea Pozzer
EGUsphere, https://doi.org/10.5194/egusphere-2023-816, https://doi.org/10.5194/egusphere-2023-816, 2023
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Ozone is a greenhouse gas and contributes to the earth’s radiative energy budget and therefore to global warming. This effect is largest in the upper troposphere. In this study, we investigate the processes controlling ozone formation and the sensitivity to its precursors in the upper tropical troposphere based on model simulations by the ECHAM5/MESSy2 Atmospheric Chemistry (EMAC) model. We find that NOx emissions from lightning most importantly affect ozone chemistry at these altitudes.
Ryan Vella, Andrea Pozzer, Matthew Forrest, Jos Lelieveld, Thomas Hickler, and Holger Tost
EGUsphere, https://doi.org/10.5194/egusphere-2023-777, https://doi.org/10.5194/egusphere-2023-777, 2023
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We investigated the effect of the El Niño-Southern Oscillation (ENSO) on biogenic volatile organic compound (BVOC) emissions from plants. ENSO events can cause a significant increase in these emissions, which have a long-term impact on the Earth's atmosphere. Persistent ENSO conditions can cause long-term changes in vegetation, resulting in even higher BVOC emissions. We link ENSO-induced emission anomalies with driving atmospheric and vegetational variables.
Meghna Soni, Rolf Sander, Lokesh K. Sahu, Domenico Taraborrelli, Pengfei Liu, Ankit Patel, Imran A. Girach, Andrea Pozzer, Sachin S. Gunthe, and Narendra Ojha
EGUsphere, https://doi.org/10.5194/egusphere-2023-652, https://doi.org/10.5194/egusphere-2023-652, 2023
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The study presents the implementation of comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA. Simulations for contrasting urban environments of Asia and Europe highlight the significant impacts of chlorine on atmospheric oxidation capacity and composition. Chemical processes governing the production and loss of chlorine-containing species have been discussed. The updated chemical mechanism will be useful to interpret field measurements and for future air quality studies.
Emily D. Lenhardt, Lan Gao, Jens Redemann, Feng Xu, Sharon P. Burton, Brian Cairns, Ian Chang, Richard A. Ferrare, Chris A. Hostetler, Pablo E. Saide, Calvin Howes, Yohei Shinozuka, Snorre Stamnes, Mary Kacarab, Amie Dobracki, Jenny Wong, Steffen Freitag, and Athanasios Nenes
Atmos. Meas. Tech., 16, 2037–2054, https://doi.org/10.5194/amt-16-2037-2023, https://doi.org/10.5194/amt-16-2037-2023, 2023
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Small atmospheric particles, such as smoke from wildfires or pollutants from human activities, impact cloud properties, and clouds have a strong influence on climate. To better understand the distributions of these particles, we develop relationships to derive their concentrations from remote sensing measurements from an instrument called a lidar. Our method is reliable for smoke particles, and similar steps can be taken to develop relationships for other particle types.
Paul Konopka, Christian Rolf, Marc von Hobe, Sergey M. Khaykin, Benjamin Clouser, Elizabeth Moyer, Fabrizio Ravegnani, Francesco D'Amato, Silvia Viciani, Nicole Spelten, Armin Afchine, Martina Krämer, Fred Stroh, and Felix Ploeger
EGUsphere, https://doi.org/10.5194/egusphere-2023-498, https://doi.org/10.5194/egusphere-2023-498, 2023
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We studied water vapor in a critical region of the atmosphere, the Asian summer monsoon anticyclone, using rare in-situ observations. Our study shows that extremely high water vapor values observed above the Asian monsoon anticyclone still undergo significant freeze-drying, and that water vapor concentrations set by the Lagrangian dry point are a better proxy for the stratospheric water vapor budget than rare observations of enhanced water mixing ratios.
Edward Groot, Patrick Kuntze, Annette Katharina Miltenberger, and Holger Tost
EGUsphere, https://doi.org/10.5194/egusphere-2023-664, https://doi.org/10.5194/egusphere-2023-664, 2023
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Deep convective clouds systems are often associated with severe weather conditions. They can organise into coherent convective cloud systems. Accurate representation in numerical weather prediction is challenging due to the dynamics of the systems and its dependency on resolution. Here, the effect of convective organisation and geometry on outflow winds (altitudes of 7–14 km) is investigated. The divergent outflow originating from these systems is represented in more detail at higher resolution.
Elena De La Torre Castro, Tina Jurkat-Witschas, Armin Afchine, Volker Grewe, Valerian Hahn, Simon Kirschler, Martina Krämer, Johannes Lucke, Nicole Spelten, Heini Wernli, Martin Zöger, and Christiane Voigt
EGUsphere, https://doi.org/10.5194/egusphere-2023-374, https://doi.org/10.5194/egusphere-2023-374, 2023
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In this study we show the differences in the microphysical properties between high latitudes (HL) cirrus and mid-latitude (ML) cirrus over the Arctic, North Atlantic, and Central Europe during summer. The in situ measurements are combined with backward trajectories to investigate the influence of the region of cloud formation. We show that HL cirrus are characterized by lower concentration of larger ice crystals compared to ML cirrus.
Georgios Dekoutsidis, Silke Groß, Martin Wirth, Martina Krämer, and Christian Rolf
Atmos. Chem. Phys., 23, 3103–3117, https://doi.org/10.5194/acp-23-3103-2023, https://doi.org/10.5194/acp-23-3103-2023, 2023
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Cirrus clouds affect Earth's atmosphere, deeming our study important. Here we use water vapor measurements by lidar and study the relative humidity (RHi) within and around midlatitude cirrus clouds. We find high supersaturations in the cloud-free air and within the clouds, especially near the cloud top. We study two cloud types with different formation processes. Finally, we conclude that the shape of the distribution of RHi can be used as an indicator of different cloud evolutionary stages.
Lenard L. Röder, Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 1167–1178, https://doi.org/10.5194/amt-16-1167-2023, https://doi.org/10.5194/amt-16-1167-2023, 2023
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Field experiments in atmospheric chemistry provide insights into chemical interactions of our atmosphere. However, high data coverage and accuracy are needed to enable further analysis. In this study, we explore a statistical method that combines knowledge about the chemical reactions with information from measurements to increase the quality of field experiment datasets. We test the algorithm for several applications and discuss limitations that depend on the specific variable and the dynamics.
Francesco Cairo, Martina Krämer, Armin Afchine, Luca Di Liberto, Sergey Khaykin, Lorenza Lucaferri, Valentin Mitev, Max Port, Christian Rolf, Marcel Snels, Nicole Spelten, Ralf Weigel, and Stephan Borrmann
EGUsphere, https://doi.org/10.5194/egusphere-2023-112, https://doi.org/10.5194/egusphere-2023-112, 2023
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Cirrus clouds have been observed over the Hymalaian region between 10 km and the tropopause at 17–18 km. Data from backscattersonde, hygrometers and particle cloud spectrometers have been compared to assess their consistency. Empirical relationships between optical parameters accessible with remote sensing lidars, and cloud microphysical parameters, as Ice Water Content, Particle Number and Surface Area Density, and particle aspherical fraction, have been established.
Matthias Kohl, Jos Lelieveld, Sourangsu Chowdhury, Sebastian Ehrhart, Disha Sharma, Yafang Cheng, Sachchida Nand Tripathi, Mathew Sebastian, Govindan Pandithurai, Hongli Wang, and Andrea Pozzer
EGUsphere, https://doi.org/10.5194/egusphere-2023-317, https://doi.org/10.5194/egusphere-2023-317, 2023
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Knowledge on atmospheric ultrafine particles (UFP) with a diameter smaller than 100 nm is crucial for public health and the hydrological cycle. We present a new global dataset of UFP concentrations at the Earth's surface derived with a comprehensive chemistry climate model, and evaluated with ground-based observations. The evaluation results are combined with high-resolution primary emissions to downscale UFP concentrations to an unprecedented horizontal resolution of 0.1° x 0.1°.
Fayçal Lamraoui, Martina Krämer, Armin Afchine, Adam B. Sokol, Sergey Khaykin, Apoorva Pandey, and Zhiming Kuang
Atmos. Chem. Phys., 23, 2393–2419, https://doi.org/10.5194/acp-23-2393-2023, https://doi.org/10.5194/acp-23-2393-2023, 2023
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Cirrus in the tropical tropopause layer (TTL) can play a key role in vertical transport. We investigate the role of different cloud regimes and the associated ice habits in regulating the properties of the TTL. We use high-resolution numerical experiments at the scales of large-eddy simulations (LESs) and aircraft measurements. We found that LES-scale parameterizations that predict ice shape are crucial for an accurate representation of TTL cirrus and thus the associated (de)hydration process.
Susanna Strada, Andrea Pozzer, Filippo Giorgi, Graziano Giuliani, Erika Coppola, Fabien Solmon, Xiaoyan Jiang, and Alex Guenther
EGUsphere, https://doi.org/10.5194/egusphere-2022-1522, https://doi.org/10.5194/egusphere-2022-1522, 2023
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Water deficit modifies emissions of isoprene, an aromatic compound released by plants that influence the production of a pollutant such as surface ozone. Numerical modeling shows that, during the warmest and driest summers, isoprene decreases between −20 to −60 % over the Euro-Mediterranean region, while surface ozone only diminishes by few percents. Decreases in isoprene emissions not only happen simultaneously of dry conditions, but could also occur after prolonged or repeated water deficit.
Yun Li, Christoph Mahnke, Susanne Rohs, Ulrich Bundke, Nicole Spelten, Georgios Dekoutsidis, Silke Groß, Christiane Voigt, Ulrich Schumann, Andreas Petzold, and Martina Krämer
Atmos. Chem. Phys., 23, 2251–2271, https://doi.org/10.5194/acp-23-2251-2023, https://doi.org/10.5194/acp-23-2251-2023, 2023
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The radiative effect of aviation-induced cirrus is closely related to ambient conditions and its microphysical properties. Our study investigated the occurrence of contrail and natural cirrus measured above central Europe in spring 2014. It finds that contrail cirrus appears frequently in the pressure range 200 to 245 hPa and occurs more often in slightly ice-subsaturated environments than expected. Avoiding slightly ice-subsaturated regions by aviation might help mitigate contrail cirrus.
Leon Kuhn, Steffen Beirle, Vinod Kumar, Sergey Osipov, Andrea Pozzer, Tim Bösch, Rajesh Kumar, and Thomas Wagner
EGUsphere, https://doi.org/10.5194/egusphere-2022-1473, https://doi.org/10.5194/egusphere-2022-1473, 2023
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NO₂ is an important air pollutant. It was observed that state of the art models for chemistry and transport show significant deviations in NO₂ abundance when compared to measurements. We use the model WRF-Chem for a 1-month simulation over central Europe and show that these deviations can be mostly resolved by precise temporal tuning of the emission data driving the model. In order to validate our results, they are compared to in-situ, satellite and MAX-DOAS measurements.
Ryan Vella, Matthew Forrest, Jos Lelieveld, and Holger Tost
Geosci. Model Dev., 16, 885–906, https://doi.org/10.5194/gmd-16-885-2023, https://doi.org/10.5194/gmd-16-885-2023, 2023
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Biogenic volatile organic compounds (BVOCs) are released by vegetation and have a major impact on atmospheric chemistry and aerosol formation. Non-interacting vegetation constrains the majority of numerical models used to estimate global BVOC emissions, and thus, the effects of changing vegetation on emissions are not addressed. In this work, we replace the offline vegetation with dynamic vegetation states by linking a chemistry–climate model with a global dynamic vegetation model.
Marios Chatziparaschos, Nikos Daskalakis, Stelios Myriokefalitakis, Nikos Kalivitis, Athanasios Nenes, María Gonçalves Ageitos, Montserrat Costa-Surós, Carlos Pérez García-Pando, Medea Zanoli, Mihalis Vrekoussis, and Maria Kanakidou
Atmos. Chem. Phys., 23, 1785–1801, https://doi.org/10.5194/acp-23-1785-2023, https://doi.org/10.5194/acp-23-1785-2023, 2023
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Ice formation is enabled by ice-nucleating particles (INP) at higher temperatures than homogeneous formation and can profoundly affect the properties of clouds. Our global model results show that K-feldspar is the most important contributor to INP concentrations globally, affecting mid-level mixed-phase clouds. However, quartz can significantly contribute and dominates the lowest and the highest altitudes of dust-derived INP, affecting mainly low-level and high-level mixed-phase clouds.
Jennifer Schallock, Christoph Brühl, Christine Bingen, Michael Höpfner, Landon Rieger, and Jos Lelieveld
Atmos. Chem. Phys., 23, 1169–1207, https://doi.org/10.5194/acp-23-1169-2023, https://doi.org/10.5194/acp-23-1169-2023, 2023
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We characterized the influence of volcanic aerosols for the period 1990–2019 and established a volcanic SO2 emission inventory that includes more than 500 eruptions. From limb-based satellite observations of SO2 and extinction, we derive 3D plumes of SO2 perturbations and injected mass by a novel method. We calculate instantaneous radiative forcing with a comprehensive chemisty climate model. Our results show that smaller eruptions can also contribute to the stratospheric aerosol forcing.
Andreas Marsing, Ralf Meerkötter, Romy Heller, Stefan Kaufmann, Tina Jurkat-Witschas, Martina Krämer, Christian Rolf, and Christiane Voigt
Atmos. Chem. Phys., 23, 587–609, https://doi.org/10.5194/acp-23-587-2023, https://doi.org/10.5194/acp-23-587-2023, 2023
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We employ highly resolved aircraft measurements of profiles of the ice water content (IWC) in Arctic cirrus clouds in winter and spring, when solar irradiation is low. Using radiation transfer calculations, we assess the cloud radiative effect over different surfaces like snow or ocean. The variability in the IWC of the clouds affects their overall radiative effect and drives internal processes. This helps understand the role of cirrus in a rapidly changing Arctic environment.
Stylianos Kakavas, Spyros Pandis, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-815, https://doi.org/10.5194/acp-2022-815, 2023
Revised manuscript accepted for ACP
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Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds, but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out year-long aerosol simulations over the continental US. We show that such organic water impacts can have an important impact on dry PM1 levels when RH levels and PM1 concentrations are high.
Edward Groot and Holger Tost
Atmos. Chem. Phys., 23, 565–585, https://doi.org/10.5194/acp-23-565-2023, https://doi.org/10.5194/acp-23-565-2023, 2023
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Thunderstorm systems play an important role in the dynamics of the Earth’s atmosphere, and some of them form a well-organised line: squall lines. Simulations of such squall lines with very small initial perturbations are compared to a reference simulation. The evolution of perturbations and processes amplifying them are analysed. It is shown that the formation of new secondary thunderstorm cells (after the initial primary cells) directly ahead of the line affects the spread strongly.
Mohamed Abdelkader, Georgiy Stenchikov, Andrea Pozzer, Holger Tost, and Jos Lelieveld
Atmos. Chem. Phys., 23, 471–500, https://doi.org/10.5194/acp-23-471-2023, https://doi.org/10.5194/acp-23-471-2023, 2023
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We study the effect of injected volcanic ash, water vapor, and SO2 on the development of the volcanic cloud and the stratospheric aerosol optical depth (AOD). Both are sensitive to the initial injection height and to the aging of the volcanic ash shaped by heterogeneous chemistry coupled with the ozone cycle. The paper explains the large differences in AOD for different injection scenarios, which could improve the estimate of the radiative forcing of volcanic eruptions.
Dirk Dienhart, Bettina Brendel, John N. Crowley, Philipp G. Eger, Hartwig Harder, Monica Martinez, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Sebastian Tauer, David Walter, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 119–142, https://doi.org/10.5194/acp-23-119-2023, https://doi.org/10.5194/acp-23-119-2023, 2023
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Formaldehyde and hydroperoxide measurements were performed in the marine boundary layer around the Arabian Peninsula and highlight the Suez Canal and Arabian (Persian) Gulf as a hotspot of photochemical air pollution. A comparison with the EMAC model shows that the formaldehyde results match within a factor of 2, while hydrogen peroxide was overestimated by more than a factor of 5, which revealed enhanced HOx (OH+HO2) radicals in the simulation and an underestimation of dry deposition velocites.
Laura Tomsche, Andreas Marsing, Tina Jurkat-Witschas, Johannes Lucke, Stefan Kaufmann, Katharina Kaiser, Johannes Schneider, Monika Scheibe, Hans Schlager, Lenard Röder, Horst Fischer, Florian Obersteiner, Andreas Zahn, Martin Zöger, Jos Lelieveld, and Christiane Voigt
Atmos. Chem. Phys., 22, 15135–15151, https://doi.org/10.5194/acp-22-15135-2022, https://doi.org/10.5194/acp-22-15135-2022, 2022
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The detection of sulfur compounds in the upper troposphere (UT) and lower stratosphere (LS) is a challenge. In-flight measurements of SO2 and sulfate aerosol were performed during the BLUESKY mission in spring 2020 under exceptional atmospheric conditions. Reduced sinks in the dry UTLS and lower but still significant air traffic influenced the enhanced SO2 in the UT, and aged volcanic plumes enhanced the LS sulfate aerosol impacting the atmospheric radiation budget and global climate.
Charlotte M. Beall, Thomas C. J. Hill, Paul J. DeMott, Tobias Köneman, Michael Pikridas, Frank Drewnick, Hartwig Harder, Christopher Pöhlker, Jos Lelieveld, Bettina Weber, Minas Iakovides, Roman Prokeš, Jean Sciare, Meinrat O. Andreae, M. Dale Stokes, and Kimberly A. Prather
Atmos. Chem. Phys., 22, 12607–12627, https://doi.org/10.5194/acp-22-12607-2022, https://doi.org/10.5194/acp-22-12607-2022, 2022
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Ice-nucleating particles (INPs) are rare aerosols that can trigger ice formation in clouds and affect climate-relevant cloud properties such as phase, reflectivity and lifetime. Dust is the dominant INP source, yet few measurements have been reported near major dust sources. We report INP observations within hundreds of kilometers of the biggest dust source regions globally: the Sahara and the Arabian Peninsula. Results show that at temperatures > −15 °C, INPs are dominated by organics.
Mengze Li, Andrea Pozzer, Jos Lelieveld, and Jonathan Williams
Earth Syst. Sci. Data, 14, 4351–4364, https://doi.org/10.5194/essd-14-4351-2022, https://doi.org/10.5194/essd-14-4351-2022, 2022
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We present a northern hemispheric airborne measurement dataset of atmospheric ethane, propane and methane and temporal trends for the time period 2006–2016 in the upper troposphere and lower stratosphere. The growth rates of ethane, methane, and propane in the upper troposphere are -2.24, 0.33, and -0.78 % yr-1, respectively, and in the lower stratosphere they are -3.27, 0.26, and -4.91 % yr-1, respectively, in 2006–2016.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, 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 A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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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 emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Clare E. Singer, Benjamin W. Clouser, Sergey M. Khaykin, Martina Krämer, Francesco Cairo, Thomas Peter, Alexey Lykov, Christian Rolf, Nicole Spelten, Armin Afchine, Simone Brunamonti, and Elisabeth J. Moyer
Atmos. Meas. Tech., 15, 4767–4783, https://doi.org/10.5194/amt-15-4767-2022, https://doi.org/10.5194/amt-15-4767-2022, 2022
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In situ measurements of water vapor in the upper troposphere are necessary to study cloud formation and hydration of the stratosphere but challenging due to cold–dry conditions. We compare measurements from three water vapor instruments from the StratoClim campaign in 2017. In clear sky (clouds), point-by-point differences were <1.5±8 % (<1±8 %). This excellent agreement allows detection of fine-scale structures required to understand the impact of convection on stratospheric water vapor.
Zaneta T. Hamryszczak, Andrea Pozzer, Florian Obersteiner, Birger Bohn, Benedikt Steil, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 9483–9497, https://doi.org/10.5194/acp-22-9483-2022, https://doi.org/10.5194/acp-22-9483-2022, 2022
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Hydrogen peroxide plays a pivotal role in the chemistry of the atmosphere. Together with organic hydroperoxides, it forms a reservoir for peroxy radicals, which are known to be the key contributors to the self-cleaning processes of the atmosphere. Hydroperoxides were measured over Europe during the BLUESKY campaign in May–June 2020. The paper gives an overview of the distribution of the species in the troposphere and investigates the impact of wet scavenging and deposition on the budget of H2O2.
Caroline Dang, Michal Segal-Rozenhaimer, Haochi Che, Lu Zhang, Paola Formenti, Jonathan Taylor, Amie Dobracki, Sara Purdue, Pui-Shan Wong, Athanasios Nenes, Arthur Sedlacek III, Hugh Coe, Jens Redemann, Paquita Zuidema, Steven Howell, and James Haywood
Atmos. Chem. Phys., 22, 9389–9412, https://doi.org/10.5194/acp-22-9389-2022, https://doi.org/10.5194/acp-22-9389-2022, 2022
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Transmission electron microscopy was used to analyze aged African smoke particles and how the smoke interacts with the marine atmosphere. We found that the volatility of organic aerosol increases with biomass burning plume age, that black carbon is often mixed with potassium salts and that the marine atmosphere can incorporate Na and Cl into smoke particles. Marine salts are more processed when mixed with smoke plumes, and there are interesting Cl-rich yet Na-absent marine particles.
Lu Zhang, Michal Segal-Rozenhaimer, Haochi Che, Caroline Dang, Arthur J. Sedlacek III, Ernie R. Lewis, Amie Dobracki, Jenny P. S. Wong, Paola Formenti, Steven G. Howell, and Athanasios Nenes
Atmos. Chem. Phys., 22, 9199–9213, https://doi.org/10.5194/acp-22-9199-2022, https://doi.org/10.5194/acp-22-9199-2022, 2022
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Widespread biomass burning (BB) events occur annually in Africa and contribute ~ 1 / 3 of global BB emissions, which contain a large family of light-absorbing organics, known as brown carbon (BrC), whose absorption of incident radiation is difficult to estimate, leading to large uncertainties in the global radiative forcing estimation. This study quantifies the BrC absorption of aged BB particles and highlights the potential presence of absorbing iron oxides in this climatically important region.
Marco Wietzoreck, Marios Kyprianou, Benjamin A. Musa Bandowe, Siddika Celik, John N. Crowley, Frank Drewnick, Philipp Eger, Nils Friedrich, Minas Iakovides, Petr Kukučka, Jan Kuta, Barbora Nežiková, Petra Pokorná, Petra Přibylová, Roman Prokeš, Roland Rohloff, Ivan Tadic, Sebastian Tauer, Jake Wilson, Hartwig Harder, Jos Lelieveld, Ulrich Pöschl, Euripides G. Stephanou, and Gerhard Lammel
Atmos. Chem. Phys., 22, 8739–8766, https://doi.org/10.5194/acp-22-8739-2022, https://doi.org/10.5194/acp-22-8739-2022, 2022
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A unique dataset of concentrations and sources of polycyclic aromatic hydrocarbons (PAHs) and their alkylated, oxygenated and nitrated derivatives, in total 74 individual species, in the marine atmosphere is presented. Exposure to these substances poses a major health risk. We found very low concentrations over the Arabian Sea, while both local and long-range-transported pollution caused elevated levels over the Mediterranean Sea and the Arabian Gulf.
Ovid O. Krüger, Bruna A. Holanda, Sourangsu Chowdhury, Andrea Pozzer, David Walter, Christopher Pöhlker, Maria Dolores Andrés Hernández, John P. Burrows, Christiane Voigt, Jos Lelieveld, Johannes Quaas, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 22, 8683–8699, https://doi.org/10.5194/acp-22-8683-2022, https://doi.org/10.5194/acp-22-8683-2022, 2022
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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 on board 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 41 %.
Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, Akima Ringsdorf, Achim Edtbauer, Horst Fischer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 7051–7069, https://doi.org/10.5194/acp-22-7051-2022, https://doi.org/10.5194/acp-22-7051-2022, 2022
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We measured the gas-phase reactivity of the NO3 radical on the summit (825 m a.s.l.) of a semi-rural mountain in southwestern Germany in July 2021. The impact of VOC-induced NO3 losses (mostly monoterpenes) competing with a loss by reaction with NO and photolysis throughout the diel cycle was estimated. Besides chemistry, boundary layer dynamics and plant-physiological processes presumably have a great impact on our observations, which were compared to previous NO3 measurements at the same site.
George K. Georgiou, Theodoros Christoudias, Yiannis Proestos, Jonilda Kushta, Michael Pikridas, Jean Sciare, Chrysanthos Savvides, and Jos Lelieveld
Geosci. Model Dev., 15, 4129–4146, https://doi.org/10.5194/gmd-15-4129-2022, https://doi.org/10.5194/gmd-15-4129-2022, 2022
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We evaluate the skill of the WRF-Chem model to perform high-resolution air quality forecasts (including ozone, nitrogen dioxide, and fine particulate matter) over the Eastern Mediterranean, during winter and summer. We compare the forecast output to observational data from background and urban locations and the forecast output from CAMS. WRF-Chem was found to forecast the concentrations and diurnal profiles of gas-phase pollutants in urban areas with higher accuracy.
Dimitris Akritidis, Andrea Pozzer, Johannes Flemming, Antje Inness, Philippe Nédélec, and Prodromos Zanis
Atmos. Chem. Phys., 22, 6275–6289, https://doi.org/10.5194/acp-22-6275-2022, https://doi.org/10.5194/acp-22-6275-2022, 2022
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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, but 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., 22, 6151–6165, https://doi.org/10.5194/acp-22-6151-2022, https://doi.org/10.5194/acp-22-6151-2022, 2022
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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.
Mireia Papke Chica, Valerian Hahn, Tiziana Braeuer, Elena de la Torre Castro, Florian Ewald, Mathias Gergely, Simon Kirschler, Luca Bugliaro Goggia, Stefanie Knobloch, Martina Kraemer, Johannes Lucke, Johanna Mayer, Raphael Maerkl, Manuel Moser, Laura Tomsche, Tina Jurkat-Witschas, Martin Zoeger, Christian von Savigny, and Christiane Voigt
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-255, https://doi.org/10.5194/acp-2022-255, 2022
Preprint withdrawn
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The mixed-phase temperature regime in convective clouds challenges our understanding of microphysical and radiative cloud properties. We provide a rare and unique dataset of aircraft in situ measurements in a strong mid-latitude convective system. We find that mechanisms initiating ice nucleation and growth strongly depend on temperature, relative humidity, and vertical velocity and variate within the measured system, resulting in altitude dependent changes of the cloud liquid and ice fraction.
Wenyu Sun, Matias Berasategui, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 4969–4984, https://doi.org/10.5194/acp-22-4969-2022, https://doi.org/10.5194/acp-22-4969-2022, 2022
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The reaction between OH and SO2 is a termolecular process that in the atmosphere results in the formation of H2SO4 and thus aerosols. We present the first temperature- and pressure-dependent measurements of the rate coefficients in N2. This is also the first study to examine the effects of water vapour on the kinetics of this reaction. Our results indicate the rate coefficient is larger than that recommended by evaluation panels, with deviations of up to 30 % in some parts of the atmosphere.
Stelios Myriokefalitakis, Elisa Bergas-Massó, María Gonçalves-Ageitos, Carlos Pérez García-Pando, Twan van Noije, Philippe Le Sager, Akinori Ito, Eleni Athanasopoulou, Athanasios Nenes, Maria Kanakidou, Maarten C. Krol, and Evangelos Gerasopoulos
Geosci. Model Dev., 15, 3079–3120, https://doi.org/10.5194/gmd-15-3079-2022, https://doi.org/10.5194/gmd-15-3079-2022, 2022
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We here describe the implementation of atmospheric multiphase processes in the EC-Earth Earth system model. We provide global budgets of oxalate, sulfate, and iron-containing aerosols, along with an analysis of the links among atmospheric composition, aqueous-phase processes, and aerosol dissolution, supported by comparison to observations. This work is a first step towards an interactive calculation of the deposition of bioavailable atmospheric iron coupled to the model’s ocean component.
Sara Bacer, Fatima Jomaa, Julien Beaumet, Hubert Gallée, Enzo Le Bouëdec, Martin Ménégoz, and Chantal Staquet
Weather Clim. Dynam., 3, 377–389, https://doi.org/10.5194/wcd-3-377-2022, https://doi.org/10.5194/wcd-3-377-2022, 2022
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We study the impact of climate change on wintertime atmospheric blocking over Europe. We focus on the frequency, duration, and size of blocking events. The blocking events are identified via the weather type decomposition methodology. We find that blocking frequency, duration, and size are mostly stationary over the 21st century. Additionally, we compare the blocking size results with the size of the blocking events identified via a different approach using a blocking index.
Andrea Pozzer, Simon F. Reifenberg, Vinod Kumar, Bruno Franco, Matthias Kohl, Domenico Taraborrelli, Sergey 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., 15, 2673–2710, https://doi.org/10.5194/gmd-15-2673-2022, https://doi.org/10.5194/gmd-15-2673-2022, 2022
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A newly developed setup of the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) is evaluated here. A comprehensive organic degradation mechanism is used and coupled with a volatility base model.
The results show that the model reproduces most of the tracers and aerosols satisfactorily but shows discrepancies for oxygenated organic gases. It is also shown that this model configuration can be used for further research in atmospheric chemistry.
Ehud Strobach, Andrea Molod, Donifan Barahona, Atanas Trayanov, Dimitris Menemenlis, and Gael Forget
Geosci. Model Dev., 15, 2309–2324, https://doi.org/10.5194/gmd-15-2309-2022, https://doi.org/10.5194/gmd-15-2309-2022, 2022
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The Green's functions methodology offers a systematic, easy-to-implement, computationally cheap, scalable, and extendable method to tune uncertain parameters in models accounting for the dependent response of the model to a change in various parameters. Herein, we successfully show for the first time that long-term errors in earth system models can be considerably reduced using Green's functions methodology. The method can be easily applied to any model containing uncertain parameters.
Sergey M. Khaykin, Elizabeth Moyer, Martina Krämer, Benjamin Clouser, Silvia Bucci, Bernard Legras, Alexey Lykov, Armin Afchine, Francesco Cairo, Ivan Formanyuk, Valentin Mitev, Renaud Matthey, Christian Rolf, Clare E. Singer, Nicole Spelten, Vasiliy Volkov, Vladimir Yushkov, and Fred Stroh
Atmos. Chem. Phys., 22, 3169–3189, https://doi.org/10.5194/acp-22-3169-2022, https://doi.org/10.5194/acp-22-3169-2022, 2022
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The Asian monsoon anticyclone is the key contributor to the global annual maximum in lower stratospheric water vapour. We investigate the impact of deep convection on the lower stratospheric water using a unique set of observations aboard the high-altitude M55-Geophysica aircraft deployed in Nepal in summer 2017 within the EU StratoClim project. We find that convective plumes of wet air can persist within the Asian anticyclone for weeks, thereby enhancing the occurrence of high-level clouds.
Paraskevi Georgakaki, Georgia Sotiropoulou, Étienne Vignon, Anne-Claire Billault-Roux, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 22, 1965–1988, https://doi.org/10.5194/acp-22-1965-2022, https://doi.org/10.5194/acp-22-1965-2022, 2022
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The modelling study focuses on the importance of ice multiplication processes in orographic mixed-phase clouds, which is one of the least understood cloud types in the climate system. We show that the consideration of ice seeding and secondary ice production through ice–ice collisional breakup is essential for correct predictions of precipitation in mountainous terrain, with important implications for radiation processes.
Dina Khordakova, Christian Rolf, Jens-Uwe Grooß, Rolf Müller, Paul Konopka, Andreas Wieser, Martina Krämer, and Martin Riese
Atmos. Chem. Phys., 22, 1059–1079, https://doi.org/10.5194/acp-22-1059-2022, https://doi.org/10.5194/acp-22-1059-2022, 2022
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Extreme storms transport humidity from the troposphere to the stratosphere. Here it has a strong impact on the climate. With ongoing global warming, we expect more storms and, hence, an enhancement of this effect. A case study was performed in order to measure the impact of the direct injection of water vapor into the lower stratosphere. The measurements displayed a significant transport of water vapor into the lower stratosphere, and this was supported by satellite and reanalysis data.
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.
Manuel Baumgartner, Christian Rolf, Jens-Uwe Grooß, Julia Schneider, Tobias Schorr, Ottmar Möhler, Peter Spichtinger, and Martina Krämer
Atmos. Chem. Phys., 22, 65–91, https://doi.org/10.5194/acp-22-65-2022, https://doi.org/10.5194/acp-22-65-2022, 2022
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An important mechanism for the appearance of ice particles in the upper troposphere at low temperatures is homogeneous nucleation. This process is commonly described by the
Koop line, predicting the humidity at freezing. However, laboratory measurements suggest that the freezing humidities are above the Koop line, motivating the present study to investigate the influence of different physical parameterizations on the homogeneous freezing with the help of a detailed numerical model.
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.
Irini Tsiodra, Georgios Grivas, Kalliopi Tavernaraki, Aikaterini Bougiatioti, Maria Apostolaki, Despina Paraskevopoulou, Alexandra Gogou, Constantine Parinos, Konstantina Oikonomou, Maria Tsagkaraki, Pavlos Zarmpas, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 21, 17865–17883, https://doi.org/10.5194/acp-21-17865-2021, https://doi.org/10.5194/acp-21-17865-2021, 2021
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We analyze observations from year-long measurements at Athens, Greece. Nighttime wintertime PAH levels are 4 times higher than daytime, and wintertime values are 15 times higher than summertime. Biomass burning aerosol during wintertime pollution events is responsible for these significant wintertime enhancements and accounts for 43 % of the population exposure to PAH carcinogenic risk. Biomass burning poses additional health risks beyond those associated with the high PM levels that develop.
Mária Lbadaoui-Darvas, Satoshi Takahama, and Athanasios Nenes
Atmos. Chem. Phys., 21, 17687–17714, https://doi.org/10.5194/acp-21-17687-2021, https://doi.org/10.5194/acp-21-17687-2021, 2021
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Aerosol–cloud interactions constitute the most uncertain contribution to climate change. The uptake kinetics of water by aerosol is a central process of cloud droplet formation, yet its molecular-scale mechanism is unknown. We use molecular simulations to study this process for phase-separated organic particles. Our results explain the increased cloud condensation activity of such particles and can be generalized over various compositions, thus possibly serving as a basis for future models.
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.
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.
Christoph Mahnke, Ralf Weigel, Francesco Cairo, Jean-Paul Vernier, Armin Afchine, Martina Krämer, Valentin Mitev, Renaud Matthey, Silvia Viciani, Francesco D'Amato, Felix Ploeger, Terry Deshler, and Stephan Borrmann
Atmos. Chem. Phys., 21, 15259–15282, https://doi.org/10.5194/acp-21-15259-2021, https://doi.org/10.5194/acp-21-15259-2021, 2021
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In 2017, in situ aerosol measurements were conducted aboard the M55 Geophysica in the Asian monsoon region. The vertical particle mixing ratio profiles show a distinct layer (15–18.5 km), the Asian tropopause aerosol layer (ATAL). The backscatter ratio (BR) was calculated based on the aerosol size distributions and compared with the BRs detected by a backscatter probe and a lidar aboard M55, and by the CALIOP lidar. All four methods show enhanced BRs in the ATAL altitude range (max. at 17.5 km).
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.
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.
Julia Schneider, Kristina Höhler, Robert Wagner, Harald Saathoff, Martin Schnaiter, Tobias Schorr, Isabelle Steinke, Stefan Benz, Manuel Baumgartner, Christian Rolf, Martina Krämer, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 21, 14403–14425, https://doi.org/10.5194/acp-21-14403-2021, https://doi.org/10.5194/acp-21-14403-2021, 2021
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Homogeneous freezing is a relevant mechanism for the formation of cirrus clouds in the upper troposphere. Based on an extensive set of homogeneous freezing experiments at the AIDA chamber with aqueous sulfuric acid aerosol, we provide a new fit line for homogeneous freezing onset conditions of sulfuric acid aerosol focusing on cirrus temperatures. In the atmosphere, homogeneous freezing thresholds have important implications on the cirrus cloud occurrence and related cloud radiative effects.
Huisheng Bian, Eunjee Lee, Randal D. Koster, Donifan Barahona, Mian Chin, Peter R. Colarco, Anton Darmenov, Sarith Mahanama, Michael Manyin, Peter Norris, John Shilling, Hongbin Yu, and Fanwei Zeng
Atmos. Chem. Phys., 21, 14177–14197, https://doi.org/10.5194/acp-21-14177-2021, https://doi.org/10.5194/acp-21-14177-2021, 2021
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The study using the NASA Earth system model shows ~2.6 % increase in burning season gross primary production and ~1.5 % increase in annual net primary production across the Amazon Basin during 2010–2016 due to the change in surface downward direct and diffuse photosynthetically active radiation by biomass burning aerosols. Such an aerosol effect is strongly dependent on the presence of clouds. The cloud fraction at which aerosols switch from stimulating to inhibiting plant growth occurs at ~0.8.
Ralf Weigel, Christoph Mahnke, Manuel Baumgartner, Martina Krämer, Peter Spichtinger, Nicole Spelten, Armin Afchine, Christian Rolf, Silvia Viciani, Francesco D'Amato, Holger Tost, and Stephan Borrmann
Atmos. Chem. Phys., 21, 13455–13481, https://doi.org/10.5194/acp-21-13455-2021, https://doi.org/10.5194/acp-21-13455-2021, 2021
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In July and August 2017, the StratoClim mission took place in Nepal with eight flights of the M-55 Geophysica at up to 20 km in the Asian monsoon anticyclone. New particle formation (NPF) next to cloud ice was detected in situ by abundant nucleation-mode aerosols (> 6 nm) along with ice particles (> 3 µm). NPF was observed mainly below the tropopause, down to 15 % being non-volatile residues. Observed intra-cloud NPF indicates its importance for the composition in the tropical tropopause layer.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
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.
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.
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.
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.
Paraskevi Georgakaki, Aikaterini Bougiatioti, Jörg Wieder, Claudia Mignani, Fabiola Ramelli, Zamin A. Kanji, Jan Henneberger, Maxime Hervo, Alexis Berne, Ulrike Lohmann, and Athanasios Nenes
Atmos. Chem. Phys., 21, 10993–11012, https://doi.org/10.5194/acp-21-10993-2021, https://doi.org/10.5194/acp-21-10993-2021, 2021
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Aerosol and cloud observations coupled with a droplet activation parameterization was used to investigate the aerosol–cloud droplet link in alpine mixed-phase clouds. Predicted droplet number, Nd, agrees with observations and never exceeds a characteristic “limiting droplet number”, Ndlim, which depends solely on σw. Nd becomes velocity limited when it is within 50 % of Ndlim. Identifying when dynamical changes control Nd variability is central for understanding aerosol–cloud interactions.
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.
Georgia Sotiropoulou, Luisa Ickes, Athanasios Nenes, and Annica M. L. Ekman
Atmos. Chem. Phys., 21, 9741–9760, https://doi.org/10.5194/acp-21-9741-2021, https://doi.org/10.5194/acp-21-9741-2021, 2021
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Mixed-phase clouds are a large source of uncertainty in projections of the Arctic climate. This is partly due to the poor representation of the cloud ice formation processes. Implementing a parameterization for ice multiplication due to mechanical breakup upon collision of two ice particles in a high-resolution model improves cloud ice phase representation; however, cloud liquid remains overestimated.
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.
Katherine H. Breen, Donifan Barahona, Tianle Yuan, Huisheng Bian, and Scott C. James
Atmos. Chem. Phys., 21, 7749–7771, https://doi.org/10.5194/acp-21-7749-2021, https://doi.org/10.5194/acp-21-7749-2021, 2021
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Increases in atmospheric aerosols affect the scattering and absorption of solar radiation by altering the macrophysical and microphysical processes of clouds. We analyzed aerosol–cloud interactions in response to degassing events from the Kilauea volcano in 2008 and 2018 by comparing satellite and simulated cloud properties. Results showed a threshold response to overcome meteorological effects that is largely controlled by aerosol concentration, composition, plume height, and ENSO state.
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.
Irene Bartolome Garcia, Reinhold Spang, Jörn Ungermann, Sabine Griessbach, Martina Krämer, Michael Höpfner, and Martin Riese
Atmos. Meas. Tech., 14, 3153–3168, https://doi.org/10.5194/amt-14-3153-2021, https://doi.org/10.5194/amt-14-3153-2021, 2021
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Cirrus clouds contribute to the general radiation budget of the Earth. Measuring optically thin clouds is challenging but the IR limb sounder GLORIA possesses the necessary technical characteristics to make it possible. This study analyses data from the WISE campaign obtained with GLORIA. We developed a cloud detection method and derived characteristics of the observed cirrus-like cloud top, cloud bottom or position with respect to the tropopause.
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.
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.
Yilin Chen, Huizhong Shen, Jennifer Kaiser, Yongtao Hu, Shannon L. Capps, Shunliu Zhao, Amir Hakami, Jhih-Shyang Shih, Gertrude K. Pavur, Matthew D. Turner, Daven K. Henze, Jaroslav Resler, Athanasios Nenes, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Tianfeng Chai, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, and Armistead G. Russell
Atmos. Chem. Phys., 21, 2067–2082, https://doi.org/10.5194/acp-21-2067-2021, https://doi.org/10.5194/acp-21-2067-2021, 2021
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Ammonia (NH3) emissions can exert adverse impacts on air quality and ecosystem well-being. NH3 emission inventories are viewed as highly uncertain. Here we optimize the NH3 emission estimates in the US using an air quality model and NH3 measurements from the IASI satellite instruments. The optimized NH3 emissions are much higher than the National Emissions Inventory estimates in April. The optimized NH3 emissions improved model performance when evaluated against independent observation.
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.
Jens Redemann, Robert Wood, Paquita Zuidema, Sarah J. Doherty, Bernadette Luna, Samuel E. LeBlanc, Michael S. Diamond, Yohei Shinozuka, Ian Y. Chang, Rei Ueyama, Leonhard Pfister, Ju-Mee Ryoo, Amie N. Dobracki, Arlindo M. da Silva, Karla M. Longo, Meloë S. Kacenelenbogen, Connor J. Flynn, Kristina Pistone, Nichola M. Knox, Stuart J. Piketh, James M. Haywood, Paola Formenti, Marc Mallet, Philip Stier, Andrew S. Ackerman, Susanne E. Bauer, Ann M. Fridlind, Gregory R. Carmichael, Pablo E. Saide, Gonzalo A. Ferrada, Steven G. Howell, Steffen Freitag, Brian Cairns, Brent N. Holben, Kirk D. Knobelspiesse, Simone Tanelli, Tristan S. L'Ecuyer, Andrew M. Dzambo, Ousmane O. Sy, Greg M. McFarquhar, Michael R. Poellot, Siddhant Gupta, Joseph R. O'Brien, Athanasios Nenes, Mary Kacarab, Jenny P. S. Wong, Jennifer D. Small-Griswold, Kenneth L. Thornhill, David Noone, James R. Podolske, K. Sebastian Schmidt, Peter Pilewskie, Hong Chen, Sabrina P. Cochrane, Arthur J. Sedlacek, Timothy J. Lang, Eric Stith, Michal Segal-Rozenhaimer, Richard A. Ferrare, Sharon P. Burton, Chris A. Hostetler, David J. Diner, Felix C. Seidel, Steven E. Platnick, Jeffrey S. Myers, Kerry G. Meyer, Douglas A. Spangenberg, Hal Maring, and Lan Gao
Atmos. Chem. Phys., 21, 1507–1563, https://doi.org/10.5194/acp-21-1507-2021, https://doi.org/10.5194/acp-21-1507-2021, 2021
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Southern Africa produces significant biomass burning emissions whose impacts on regional and global climate are poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA investigation designed to study the key processes that determine these climate impacts. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project, the dataset it produced, and the most important initial findings.
Johannes Schneider, Ralf Weigel, Thomas Klimach, Antonis Dragoneas, Oliver Appel, Andreas Hünig, Sergej Molleker, Franziska Köllner, Hans-Christian Clemen, Oliver Eppers, Peter Hoppe, Peter Hoor, Christoph Mahnke, Martina Krämer, Christian Rolf, Jens-Uwe Grooß, Andreas Zahn, Florian Obersteiner, Fabrizio Ravegnani, Alexey Ulanovsky, Hans Schlager, Monika Scheibe, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Martin Zöger, and Stephan Borrmann
Atmos. Chem. Phys., 21, 989–1013, https://doi.org/10.5194/acp-21-989-2021, https://doi.org/10.5194/acp-21-989-2021, 2021
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During five aircraft missions, we detected aerosol particles containing meteoric material in the lower stratosphere. The stratospheric measurements span a latitude range from 15 to 68° N, and we find that at potential temperature levels of more than 40 K above the tropopause; particles containing meteoric material occur at similar abundance fractions across latitudes and seasons. We conclude that meteoric material is efficiently distributed between high and low latitudes by isentropic mixing.
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.
Georgia Sotiropoulou, Étienne Vignon, Gillian Young, Hugh Morrison, Sebastian J. O'Shea, Thomas Lachlan-Cope, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 21, 755–771, https://doi.org/10.5194/acp-21-755-2021, https://doi.org/10.5194/acp-21-755-2021, 2021
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Summer clouds have a significant impact on the radiation budget of the Antarctic surface and thus on ice-shelf melting. However, these are poorly represented in climate models due to errors in their microphysical structure, including the number of ice crystals that they contain. We show that breakup from ice particle collisions can substantially magnify the ice crystal number concentration with significant implications for surface radiation. This process is currently missing in climate models.
Jörn Ungermann, Irene Bartolome, Sabine Griessbach, Reinhold Spang, Christian Rolf, Martina Krämer, Michael Höpfner, and Martin Riese
Atmos. Meas. Tech., 13, 7025–7045, https://doi.org/10.5194/amt-13-7025-2020, https://doi.org/10.5194/amt-13-7025-2020, 2020
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This study examines the potential of new IR limb imager instruments and tomographic methods for cloud detection purposes. Simple color-ratio-based methods are examined and compared against more involved nonlinear convex optimization. In a second part, 3-D measurements of the airborne limb sounder GLORIA taken during the Wave-driven ISentropic Exchange campaign are used to exemplarily derive the location and extent of small-scale cirrus clouds with high spatial accuracy.
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.
Johannes Quaas, Antti Arola, Brian Cairns, Matthew Christensen, Hartwig Deneke, Annica M. L. Ekman, Graham Feingold, Ann Fridlind, Edward Gryspeerdt, Otto Hasekamp, Zhanqing Li, Antti Lipponen, Po-Lun Ma, Johannes Mülmenstädt, Athanasios Nenes, Joyce E. Penner, Daniel Rosenfeld, Roland Schrödner, Kenneth Sinclair, Odran Sourdeval, Philip Stier, Matthias Tesche, Bastiaan van Diedenhoven, and Manfred Wendisch
Atmos. Chem. Phys., 20, 15079–15099, https://doi.org/10.5194/acp-20-15079-2020, https://doi.org/10.5194/acp-20-15079-2020, 2020
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Anthropogenic pollution particles – aerosols – serve as cloud condensation nuclei and thus increase cloud droplet concentration and the clouds' reflection of sunlight (a cooling effect on climate). This Twomey effect is poorly constrained by models and requires satellite data for better quantification. The review summarizes the challenges in properly doing so and outlines avenues for progress towards a better use of aerosol retrievals and better retrievals of droplet concentrations.
Edward Groot and Holger Tost
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1142, https://doi.org/10.5194/acp-2020-1142, 2020
Publication in ACP not foreseen
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Sensitivities and variability of upper tropospheric flow (~10 km height) resulting immediately and as a direct consequence of (thunder)storm activity have been modeled in detail down to resolutions of 100–200 m and explored for different (organisation/) storm types. It is shown that the amount of water condensation explains much of emerging variability in upper atmospheric flow. Part of the effects on the nearby upper atmospheric flow is suggested to be explained by (organisation/) storm type.
Ari Laaksonen, Jussi Malila, and Athanasios Nenes
Atmos. Chem. Phys., 20, 13579–13589, https://doi.org/10.5194/acp-20-13579-2020, https://doi.org/10.5194/acp-20-13579-2020, 2020
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Aerosol particles containing black carbon are ubiquitous in the atmosphere and originate from combustion processes. We examine their capability to act as condensation centers for water vapor. We make use of published experimental data sets for different types of black carbon particles, ranging from very pure particles to particles that contain both black carbon and water soluble organic matter, and we show that a recently developed theory reproduces most of the experimental results.
Lanxiadi Chen, Chao Peng, Wenjun Gu, Hanjing Fu, Xing Jian, Huanhuan Zhang, Guohua Zhang, Jianxi Zhu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13611–13626, https://doi.org/10.5194/acp-20-13611-2020, https://doi.org/10.5194/acp-20-13611-2020, 2020
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We investigated hygroscopic properties of a number of mineral dust particles in a quantitative manner, via measuring the sample mass at different relative humidities. The robust and comprehensive data obtained would significantly improve our knowledge of hygroscopicity of mineral dust and its impacts on atmospheric chemistry and climate.
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.
Jie Gong, Xiping Zeng, Dong L. Wu, S. Joseph Munchak, Xiaowen Li, Stefan Kneifel, Davide Ori, Liang Liao, and Donifan Barahona
Atmos. Chem. Phys., 20, 12633–12653, https://doi.org/10.5194/acp-20-12633-2020, https://doi.org/10.5194/acp-20-12633-2020, 2020
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This work provides a novel way of using polarized passive microwave measurements to study the interlinked cloud–convection–precipitation processes. The magnitude of differences between polarized radiances is found linked to ice microphysics (shape, size, orientation and density), mesoscale dynamic and thermodynamic structures, and surface precipitation. We conclude that passive sensors with multiple polarized channel pairs may serve as cheaper and useful substitutes for spaceborne radar sensors.
Martina Krämer, Christian Rolf, Nicole Spelten, Armin Afchine, David Fahey, Eric Jensen, Sergey Khaykin, Thomas Kuhn, Paul Lawson, Alexey Lykov, Laura L. Pan, Martin Riese, Andrew Rollins, Fred Stroh, Troy Thornberry, Veronika Wolf, Sarah Woods, Peter Spichtinger, Johannes Quaas, and Odran Sourdeval
Atmos. Chem. Phys., 20, 12569–12608, https://doi.org/10.5194/acp-20-12569-2020, https://doi.org/10.5194/acp-20-12569-2020, 2020
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To improve the representations of cirrus clouds in climate predictions, extended knowledge of their properties and geographical distribution is required. This study presents extensive airborne in situ and satellite remote sensing climatologies of cirrus and humidity, which serve as a guide to cirrus clouds. Further, exemplary radiative characteristics of cirrus types and also in situ observations of tropical tropopause layer cirrus and humidity in the Asian monsoon anticyclone are shown.
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.
Aikaterini Bougiatioti, Athanasios Nenes, Jack J. Lin, Charles A. Brock, Joost A. de Gouw, Jin Liao, Ann M. Middlebrook, and André Welti
Atmos. Chem. Phys., 20, 12163–12176, https://doi.org/10.5194/acp-20-12163-2020, https://doi.org/10.5194/acp-20-12163-2020, 2020
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The number concentration of droplets in clouds in the summertime in the southeastern United States is influenced by aerosol variations but limited by the strong competition for supersaturated water vapor. Concurrent variations in vertical velocity magnify the response of cloud droplet number to aerosol increases by up to a factor of 5. Omitting the covariance of vertical velocity with aerosol number may therefore bias estimates of the cloud albedo effect from aerosols.
David L. Mitchell, John Mejia, Anne Garnier, Yuta Tomii, Martina Krämer, and Farnaz Hosseinpour
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-846, https://doi.org/10.5194/acp-2020-846, 2020
Publication in ACP not foreseen
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This may be the first estimate of the radiative contribution of homogeneous ice nucleation in cirrus clouds on a global, regional and seasonal scale. This is achieved by constraining an atmospheric global climate model with measured cirrus cloud properties via satellite remote sensing. The results show that the overall radiative warming contributed by homogeneous ice nucleation at the top of the atmosphere is 2.4 W m-2 outside the ± 30° latitude zone during non-summer months (JJA).
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.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Publication in ACP not foreseen
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Andreas Petzold, Patrick Neis, Mihal Rütimann, Susanne Rohs, Florian Berkes, Herman G. J. Smit, Martina Krämer, Nicole Spelten, Peter Spichtinger, Philippe Nédélec, and Andreas Wahner
Atmos. Chem. Phys., 20, 8157–8179, https://doi.org/10.5194/acp-20-8157-2020, https://doi.org/10.5194/acp-20-8157-2020, 2020
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The first analysis of 15 years of global-scale water vapour and relative humidity observations by passenger aircraft in the MOZAIC and IAGOS programmes resolves detailed features of water vapour and ice-supersaturated air in the mid-latitude tropopause. Key results provide in-depth insight into seasonal and regional variability and chemical signatures of ice-supersaturated air masses, including trend analyses, and show a close link to cirrus clouds and their highly important effects on climate.
Shunliu Zhao, Matthew G. Russell, Amir Hakami, Shannon L. Capps, Matthew D. Turner, Daven K. Henze, Peter B. Percell, Jaroslav Resler, Huizhong Shen, Armistead G. Russell, Athanasios Nenes, Amanda J. Pappin, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Charles O. Stanier, and Tianfeng Chai
Geosci. Model Dev., 13, 2925–2944, https://doi.org/10.5194/gmd-13-2925-2020, https://doi.org/10.5194/gmd-13-2925-2020, 2020
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.
Harald Rybka and Holger Tost
Geosci. Model Dev., 13, 2671–2694, https://doi.org/10.5194/gmd-13-2671-2020, https://doi.org/10.5194/gmd-13-2671-2020, 2020
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Simulating cloud processes and their interactions with their environment is one of the biggest challenges in atmospheric science. This study couples a cloud-resolving model with a global climate model to improve the representation of small-scale processes for climate simulations. Unlike conventional approaches, tropical precipitation is better simulated with the new model setup. However, the diurnal cycle of precipitation and cloud amounts can be significantly influenced by the chosen setup.
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.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Mattia Righi, Johannes Hendricks, Ulrike Lohmann, Christof Gerhard Beer, Valerian Hahn, Bernd Heinold, Romy Heller, Martina Krämer, Michael Ponater, Christian Rolf, Ina Tegen, and Christiane Voigt
Geosci. Model Dev., 13, 1635–1661, https://doi.org/10.5194/gmd-13-1635-2020, https://doi.org/10.5194/gmd-13-1635-2020, 2020
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A new cloud microphysical scheme is implemented in the global EMAC-MADE3 aerosol model and evaluated. The new scheme features a detailed parameterization for aerosol-driven ice formation in cirrus clouds, accounting for the competition between homogeneous and heterogeneous ice formation processes. The comparison against satellite data and in situ measurements shows that the model performance is in line with similar global coupled models featuring ice cloud parameterizations.
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.
Mary Kacarab, K. Lee Thornhill, Amie Dobracki, Steven G. Howell, Joseph R. O'Brien, Steffen Freitag, Michael R. Poellot, Robert Wood, Paquita Zuidema, Jens Redemann, and Athanasios Nenes
Atmos. Chem. Phys., 20, 3029–3040, https://doi.org/10.5194/acp-20-3029-2020, https://doi.org/10.5194/acp-20-3029-2020, 2020
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We find that extensive biomass burning aerosol plumes from southern Africa can profoundly influence clouds in the southeastern Atlantic. Concurrent variations in vertical velocity, however, are found to magnify the relationship between boundary layer aerosol and the cloud droplet number. Neglecting these covariances may strongly bias the sign and magnitude of aerosol impacts on the cloud droplet number.
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.
Arnaldo Negron, Natasha DeLeon-Rodriguez, Samantha M. Waters, Luke D. Ziemba, Bruce Anderson, Michael Bergin, Konstantinos T. Konstantinidis, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1817–1838, https://doi.org/10.5194/acp-20-1817-2020, https://doi.org/10.5194/acp-20-1817-2020, 2020
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Airborne biological particles impact human health, cloud formation, and ecosystems, but few techniques are available to characterize their atmospheric abundance. Combining a newly developed high-volume sampling/flow cytometry technique together with an laser-induced fluorescence instrument, we detect a highly dynamic bioaerosol community over urban Atlanta, composed of pollen, fungi, and bacteria with low and high nucleic acid content.
Fan Mei, Jian Wang, Jennifer M. Comstock, Ralf Weigel, Martina Krämer, Christoph Mahnke, John E. Shilling, Johannes Schneider, Christiane Schulz, Charles N. Long, Manfred Wendisch, Luiz A. T. Machado, Beat Schmid, Trismono Krisna, Mikhail Pekour, John Hubbe, Andreas Giez, Bernadett Weinzierl, Martin Zoeger, Mira L. Pöhlker, Hans Schlager, Micael A. Cecchini, Meinrat O. Andreae, Scot T. Martin, Suzane S. de Sá, Jiwen Fan, Jason Tomlinson, Stephen Springston, Ulrich Pöschl, Paulo Artaxo, Christopher Pöhlker, Thomas Klimach, Andreas Minikin, Armin Afchine, and Stephan Borrmann
Atmos. Meas. Tech., 13, 661–684, https://doi.org/10.5194/amt-13-661-2020, https://doi.org/10.5194/amt-13-661-2020, 2020
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In 2014, the US DOE G1 aircraft and the German HALO aircraft overflew the Amazon basin to study how aerosols influence cloud cycles under a clean condition and around a tropical megacity. This paper describes how to meaningfully compare similar measurements from two research aircraft and identify the potential measurement issue. We also discuss the uncertainty range for each measurement for further usage in model evaluation and satellite data validation.
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.
Georgia Sotiropoulou, Sylvia Sullivan, Julien Savre, Gary Lloyd, Thomas Lachlan-Cope, Annica M. L. Ekman, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1301–1316, https://doi.org/10.5194/acp-20-1301-2020, https://doi.org/10.5194/acp-20-1301-2020, 2020
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Arctic clouds constitute a large source of uncertainty in predictions of future climate. Observations indicate that the number concentration of cloud ice crystals exceeds the concentration of aerosols that can act as ice-nucleating particles (INPs). We show that ice multiplication due to mechanical break-up upon collisions between the few primary ice crystals (formed from INPs) can explain the discrepancy. Including a description of the process in climate models can improve cloud representation.
Lei Gu, Jie Chen, Jiabo Yin, Sylvia C. Sullivan, Hui-Min Wang, Shenglian Guo, Liping Zhang, and Jong-Suk Kim
Hydrol. Earth Syst. Sci., 24, 451–472, https://doi.org/10.5194/hess-24-451-2020, https://doi.org/10.5194/hess-24-451-2020, 2020
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Focusing on the multifaceted nature of droughts, this study quantifies the change in global drought risks for 1.5 and 2.0 °C warming trajectories by a multi-model ensemble under three representative concentration pathways (RCP2.6, 4.5 and 8.5). Socioeconomic exposures are investigated by incorporating the dynamic shared socioeconomic pathways (SSPs) into the drought impact assessment. The results show that even the ambitious 1.5 °C warming level can cause substantial increases on the global scale.
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.
Michael A. Battaglia Jr., Rodney J. Weber, Athanasios Nenes, and Christopher J. Hennigan
Atmos. Chem. Phys., 19, 14607–14620, https://doi.org/10.5194/acp-19-14607-2019, https://doi.org/10.5194/acp-19-14607-2019, 2019
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The effects of water-soluble organic carbon (WSOC) on aerosol pH were characterized for aqueous-phase particles containing a mixture of inorganics and organics. The ISORROPIA-II and E-AIM models were used in conjunction with AIOMFAC to quantify the effect of organics on aerosol pH through (1) changes to the aerosol liquid water content and (2) changes to the hydrogen ion activity coefficient. The study included both organic acids and nonacids, at RH levels ranging from 70 to 90 %.
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.
Keun-Ok Lee, Thibaut Dauhut, Jean-Pierre Chaboureau, Sergey Khaykin, Martina Krämer, and Christian Rolf
Atmos. Chem. Phys., 19, 11803–11820, https://doi.org/10.5194/acp-19-11803-2019, https://doi.org/10.5194/acp-19-11803-2019, 2019
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This study focuses on the hydration patch that was measured during the StratoClim field campaign and the corresponding convective overshoots over the Sichuan Basin. Through analysis using airborne and spaceborne measurements and the numerical simulation using a non-hydrostatic model, we show the key hydration process and pathway of the hydration patch in tropical tropopause layer.
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.
Eleni Marinou, Matthias Tesche, Athanasios Nenes, Albert Ansmann, Jann Schrod, Dimitra Mamali, Alexandra Tsekeri, Michael Pikridas, Holger Baars, Ronny Engelmann, Kalliopi-Artemis Voudouri, Stavros Solomos, Jean Sciare, Silke Groß, Florian Ewald, and Vassilis Amiridis
Atmos. Chem. Phys., 19, 11315–11342, https://doi.org/10.5194/acp-19-11315-2019, https://doi.org/10.5194/acp-19-11315-2019, 2019
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We assess the feasibility of ground-based and spaceborne lidars to retrieve profiles of cloud-relevant aerosol concentrations and ice-nucleating particles. The retrieved profiles are in good agreement with airborne in situ measurements. Our methodology will be applied to satellite observations in the future so as to provide a global 3D product of cloud-relevant properties.
Mega Octaviani, Holger Tost, and Gerhard Lammel
Geosci. Model Dev., 12, 3585–3607, https://doi.org/10.5194/gmd-12-3585-2019, https://doi.org/10.5194/gmd-12-3585-2019, 2019
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This work presents a submodel description for the atmospheric cycling and air–surface exchange processes of semivolatile organic compounds. The submodel is meant to be applied within a global atmospheric chemistry–climate model. The simulation results for polycyclic aromatic hydrocarbons confirm progress in modelling semivolatile species, verified by comparison with surface monitoring data. The significance of new modelling features for tracer distributions was quantified in a sensitivity study.
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.
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).
Jenny P. S. Wong, Maria Tsagkaraki, Irini Tsiodra, Nikolaos Mihalopoulos, Kalliopi Violaki, Maria Kanakidou, Jean Sciare, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 19, 7319–7334, https://doi.org/10.5194/acp-19-7319-2019, https://doi.org/10.5194/acp-19-7319-2019, 2019
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Biomass burning is a major source of light-absorbing organic species in atmospheric aerosols, and it can play an important role in climate and atmospheric chemistry. Through a combination of laboratory experiments and field observations, this work demonstrated that the light absorption properties of aged biomass burning organic aerosols are dominated by high-molecular-weight compounds. In addition, we found that total hydrated sugars may be a robust tracer for aged biomass burning aerosols.
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.
Panayiotis Kalkavouras, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Maria Tombrou, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 6185–6203, https://doi.org/10.5194/acp-19-6185-2019, https://doi.org/10.5194/acp-19-6185-2019, 2019
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We study how new particle formation (NPF) events affect clouds throughout the year at a ground site in the E Mediterranean. Using a new tools and evaluation metrics, NPF is found to affect only evening and nocturnal clouds by modestly increasing droplet number by 7 to 12 %. A conventional analysis based on CCN concentration at prescribed supersaturation levels or aerosol size can considerably bias the perceived influence of NPF events on regional clouds, the hydrological cycle, and climate.
Sabine Robrecht, Bärbel Vogel, Jens-Uwe Grooß, Karen Rosenlof, Troy Thornberry, Andrew Rollins, Martina Krämer, Lance Christensen, and Rolf Müller
Atmos. Chem. Phys., 19, 5805–5833, https://doi.org/10.5194/acp-19-5805-2019, https://doi.org/10.5194/acp-19-5805-2019, 2019
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The potential destruction of stratospheric ozone in the mid-latitudes has been discussed recently. We analysed this ozone loss mechanism and its sensitivities. In a certain temperature range, we found a threshold in water vapour, which has to be exceeded for ozone loss to occur. We show the dependence of this water vapour threshold on temperature, sulfate content and air composition. This study provides a basis to estimate the impact of potential sulphate geoengineering on stratospheric ozone.
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.
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.
Nønne L. Prisle, Jack J. Lin, Sara Purdue, Haisheng Lin, J. Carson Meredith, and Athanasios Nenes
Atmos. Chem. Phys., 19, 4741–4761, https://doi.org/10.5194/acp-19-4741-2019, https://doi.org/10.5194/acp-19-4741-2019, 2019
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We measure surface activity and cloud-forming potential of pollenkitt, an organic mixture coating pollen grains. Cloud droplet formation is affected through both surface tension and bulk depletion, with a consistent particle size-dependent signature. We observe nonideal solution effects in pollenkitt mixtures with ammonium sulfate salt. Our results suggest sensitivity of general water interactions, including cloud formation by pollen and their fragments, to both atmospheric humidity and aging.
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.
J. Christopher Kaiser, Johannes Hendricks, Mattia Righi, Patrick Jöckel, Holger Tost, Konrad Kandler, Bernadett Weinzierl, Daniel Sauer, Katharina Heimerl, Joshua P. Schwarz, Anne E. Perring, and Thomas Popp
Geosci. Model Dev., 12, 541–579, https://doi.org/10.5194/gmd-12-541-2019, https://doi.org/10.5194/gmd-12-541-2019, 2019
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The implementation of the aerosol microphysics submodel MADE3 into the global atmospheric chemistry model EMAC is described and evaluated against an extensive pool of observational data, focusing on aerosol mass and number concentrations, size distributions, composition, and optical properties. EMAC (MADE3) is able to reproduce main aerosol properties reasonably well, in line with the performance of other global aerosol models.
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.
Michael Weger, Bernd Heinold, Christa Engler, Ulrich Schumann, Axel Seifert, Romy Fößig, Christiane Voigt, Holger Baars, Ulrich Blahak, Stephan Borrmann, Corinna Hoose, Stefan Kaufmann, Martina Krämer, Patric Seifert, Fabian Senf, Johannes Schneider, and Ina Tegen
Atmos. Chem. Phys., 18, 17545–17572, https://doi.org/10.5194/acp-18-17545-2018, https://doi.org/10.5194/acp-18-17545-2018, 2018
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The impact of desert dust on cloud formation is investigated for a major Saharan dust event over Europe by interactive regional dust modeling. Dust particles are very efficient ice-nucleating particles promoting the formation of ice crystals in clouds. The simulations show that the observed extensive cirrus development was likely related to the above-average dust load. The interactive dust–cloud feedback in the model significantly improves the agreement with aircraft and satellite observations.
Veronika Wolf, Thomas Kuhn, Mathias Milz, Peter Voelger, Martina Krämer, and Christian Rolf
Atmos. Chem. Phys., 18, 17371–17386, https://doi.org/10.5194/acp-18-17371-2018, https://doi.org/10.5194/acp-18-17371-2018, 2018
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Balloon-borne measurements of microphysical properties of Arctic ice clouds have been performed with an in situ particle imager and been analyzed for the first time with respect to how the ice particles have formed. Ice particle size, shape and number show large variations from cloud to cloud, which cannot be explained with local conditions only, and rather depend on conditions at cloud formation. Taking this into account when parametrizing ice cloud properties may improve retrievals and models.
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
Hongyu Guo, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 17307–17323, https://doi.org/10.5194/acp-18-17307-2018, https://doi.org/10.5194/acp-18-17307-2018, 2018
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Overprediction of fine-particle ammonium-sulfate molar ratios (R) by thermodynamic models is suggested as evidence for organic aerosol limiting the condensation of ammonia onto particles, with significant impacts on aerosol chemistry. We find that the effects of small amounts of salt and dust, combined with measurement artifacts, explain the discrepancy in R. These results are highly insensitive to mixing state. This means that aerosol predictions are much more robust than thought before.
Donifan Barahona
Atmos. Chem. Phys., 18, 17119–17141, https://doi.org/10.5194/acp-18-17119-2018, https://doi.org/10.5194/acp-18-17119-2018, 2018
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This work develops a model for ice formation mediated by particles immersed within droplets. Ice nucleation is not only enhanced by the modification of the thermodynamic properties of the vicinal water but is also inhibited by decreased water mobility near the particle. The ice nucleation rate is thus determined by competing kinetic and thermodynamic factors during ice formation. A new regime where ice nucleation is mediated mainly by kinetics instead of thermodynamics is discovered.
Stefan Kaufmann, Christiane Voigt, Romy Heller, Tina Jurkat-Witschas, Martina Krämer, Christian Rolf, Martin Zöger, Andreas Giez, Bernhard Buchholz, Volker Ebert, Troy Thornberry, and Ulrich Schumann
Atmos. Chem. Phys., 18, 16729–16745, https://doi.org/10.5194/acp-18-16729-2018, https://doi.org/10.5194/acp-18-16729-2018, 2018
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We present an intercomparison of the airborne water vapor measurements during the ML-CIRRUS mission. Although the agreement of the hygrometers significantly improved compared to studies from recent decades, systematic differences remain under specific meteorological conditions. We compare the measurements to model data, where we observe a model wet bias in the lower stratosphere close to the tropopause, likely caused by a blurred humidity gradient in the model tropopause.
Sylvia C. Sullivan, Christian Barthlott, Jonathan Crosier, Ilya Zhukov, Athanasios Nenes, and Corinna Hoose
Atmos. Chem. Phys., 18, 16461–16480, https://doi.org/10.5194/acp-18-16461-2018, https://doi.org/10.5194/acp-18-16461-2018, 2018
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Ice crystal formation in clouds can occur via thermodynamic nucleation, but also via mechanical collisions between pre-existing crystals or co-existing droplets. When descriptions of this mechanical ice generation are implemented into the COSMO weather model, we find that the contributions to crystal number from thermodynamic and mechanical processes are of the same order. Mechanical ice generation also intensifies differences in precipitation intensity between dynamic and quiescent regions.
Stelios Myriokefalitakis, Akinori Ito, Maria Kanakidou, Athanasios Nenes, Maarten C. Krol, Natalie M. Mahowald, Rachel A. Scanza, Douglas S. Hamilton, Matthew S. Johnson, Nicholas Meskhidze, Jasper F. Kok, Cecile Guieu, Alex R. Baker, Timothy D. Jickells, Manmohan M. Sarin, Srinivas Bikkina, Rachel Shelley, Andrew Bowie, Morgane M. G. Perron, and Robert A. Duce
Biogeosciences, 15, 6659–6684, https://doi.org/10.5194/bg-15-6659-2018, https://doi.org/10.5194/bg-15-6659-2018, 2018
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The first atmospheric iron (Fe) deposition model intercomparison is presented in this study, as a result of the deliberations of the United Nations Joint Group of Experts on the Scientific Aspects of Marine Environmental Protection (GESAMP; http://www.gesamp.org/) Working Group 38. We conclude that model diversity over remote oceans reflects uncertainty in the Fe content parameterizations of dust aerosols, combustion aerosol emissions and the size distribution of transported aerosol Fe.
Christiane Schulz, Johannes Schneider, Bruna Amorim Holanda, Oliver Appel, Anja Costa, Suzane S. de Sá, Volker Dreiling, Daniel Fütterer, Tina Jurkat-Witschas, Thomas Klimach, Christoph Knote, Martina Krämer, Scot T. Martin, Stephan Mertes, Mira L. Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Bernadett Weinzierl, Helmut Ziereis, Martin Zöger, Meinrat O. Andreae, Paulo Artaxo, Luiz A. T. Machado, Ulrich Pöschl, Manfred Wendisch, and Stephan Borrmann
Atmos. Chem. Phys., 18, 14979–15001, https://doi.org/10.5194/acp-18-14979-2018, https://doi.org/10.5194/acp-18-14979-2018, 2018
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Aerosol chemical composition measurements in the tropical upper troposphere over the Amazon region show that 78 % of the aerosol in the upper troposphere consists of organic matter. Up to 20 % of the organic aerosol can be attributed to isoprene epoxydiol secondary organic aerosol (IEPOX-SOA). Furthermore, organic nitrates were identified, suggesting a connection to the IEPOX-SOA formation.
Odran Sourdeval, Edward Gryspeerdt, Martina Krämer, Tom Goren, Julien Delanoë, Armin Afchine, Friederike Hemmer, and Johannes Quaas
Atmos. Chem. Phys., 18, 14327–14350, https://doi.org/10.5194/acp-18-14327-2018, https://doi.org/10.5194/acp-18-14327-2018, 2018
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The number concentration of ice crystals (Ni) is a key cloud property that remains very uncertain due to difficulties in determining it using satellites. This lack of global observational constraints limits our ability to constrain this property in models responsible for predicting future climate. This pair of papers fills this gap by showing and analyzing the first rigorously evaluated global climatology of Ni, leading to new information shedding light on the processes that control high clouds.
Edward Gryspeerdt, Odran Sourdeval, Johannes Quaas, Julien Delanoë, Martina Krämer, and Philipp Kühne
Atmos. Chem. Phys., 18, 14351–14370, https://doi.org/10.5194/acp-18-14351-2018, https://doi.org/10.5194/acp-18-14351-2018, 2018
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The concentration of ice crystals in a cloud affects both the properties and the life cycle of the cloud. This work uses a new satellite retrieval to investigate controls on the ice crystal concentration at a global scale. Both temperature and vertical wind speed in a cloud have a strong impact on the concentration of ice crystals. The ice crystal number is also related to the aerosol environment; defining this relation opens up new ways to investigate human impacts on clouds and the climate.
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.
Annette Filges, Christoph Gerbig, Chris W. Rella, John Hoffnagle, Herman Smit, Martina Krämer, Nicole Spelten, Christian Rolf, Zoltán Bozóki, Bernhard Buchholz, and Volker Ebert
Atmos. Meas. Tech., 11, 5279–5297, https://doi.org/10.5194/amt-11-5279-2018, https://doi.org/10.5194/amt-11-5279-2018, 2018
Petros Vasilakos, Armistead Russell, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys., 18, 12765–12775, https://doi.org/10.5194/acp-18-12765-2018, https://doi.org/10.5194/acp-18-12765-2018, 2018
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In this work, we investigated the role of emission reductions on aerosol acidity and particulate nitrate. We found that models exhibit positive biases in pH predictions, attributed to very high levels of crustal elements (Mg, Ca, K) in model simulations, which in turn led to an increasing aerosol pH trend over the past decade and allowed nitrate to become an important component of aerosol, which is inconsistent with the measurements, highlighting the importance of accurate pH prediction.
Hongyu Guo, Rene Otjes, Patrick Schlag, Astrid Kiendler-Scharr, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 12241–12256, https://doi.org/10.5194/acp-18-12241-2018, https://doi.org/10.5194/acp-18-12241-2018, 2018
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Reduction in ammonia has been proposed as a way to lower fine particle mass and improve air quality, but gas-phase ammonia is linked to agricultural productivity. We assess the feasibility of ammonia control at a variety of locations through an aerosol thermodynamic analysis. We show that aerosol response to ammonia control is highly nonlinear and only becomes effective when ambient particle pH drops below approximately 3. Particle pH is a relevant aerosol air quality parameter.
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.
Theodora Nah, Hongyu Guo, Amy P. Sullivan, Yunle Chen, David J. Tanner, Athanasios Nenes, Armistead Russell, Nga Lee Ng, L. Gregory Huey, and Rodney J. Weber
Atmos. Chem. Phys., 18, 11471–11491, https://doi.org/10.5194/acp-18-11471-2018, https://doi.org/10.5194/acp-18-11471-2018, 2018
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We present measurements from a field study conducted in an agriculturally intensive region in the southeastern US during the fall of 2016 to investigate how NH3 affects particle acidity and SOA formation via gas–particle partitioning of semi-volatile organic acids. For this study, higher NH3 concentrations relative to what has been measured in the region in previous studies had minor effects on PM1 organic acids and their influence on the overall organic aerosol and PM1 mass concentrations.
Sören Johansson, Wolfgang Woiwode, Michael Höpfner, Felix Friedl-Vallon, Anne Kleinert, Erik Kretschmer, Thomas Latzko, Johannes Orphal, Peter Preusse, Jörn Ungermann, Michelle L. Santee, Tina Jurkat-Witschas, Andreas Marsing, Christiane Voigt, Andreas Giez, Martina Krämer, Christian Rolf, Andreas Zahn, Andreas Engel, Björn-Martin Sinnhuber, and Hermann Oelhaf
Atmos. Meas. Tech., 11, 4737–4756, https://doi.org/10.5194/amt-11-4737-2018, https://doi.org/10.5194/amt-11-4737-2018, 2018
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We present two-dimensional cross sections of temperature, HNO3, O3, ClONO2, H2O and CFC-12 from measurements of the GLORIA infrared limb imager during the POLSTRACC/GW-LCYCLE/SALSA aircraft campaigns in the Arctic winter 2015/2016. GLORIA sounded the atmosphere between 5 and 14 km with vertical resolutions of 0.4–1 km. Estimated errors are in the range of 1–2 K (temperature) and 10 %–20 % (trace gases). Comparisons to in situ instruments onboard the aircraft and to Aura/MLS are shown.
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.
Armin Afchine, Christian Rolf, Anja Costa, Nicole Spelten, Martin Riese, Bernhard Buchholz, Volker Ebert, Romy Heller, Stefan Kaufmann, Andreas Minikin, Christiane Voigt, Martin Zöger, Jessica Smith, Paul Lawson, Alexey Lykov, Sergey Khaykin, and Martina Krämer
Atmos. Meas. Tech., 11, 4015–4031, https://doi.org/10.5194/amt-11-4015-2018, https://doi.org/10.5194/amt-11-4015-2018, 2018
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The ice water content (IWC) of cirrus clouds is an essential parameter that determines their radiative properties and is thus important for climate simulations. Experimental investigations of IWCs measured on board research aircraft reveal that their accuracy is influenced by the sampling position. IWCs detected at the aircraft roof deviate significantly from wing, side or bottom IWCs. The reasons are deflections of the gas streamlines and ice particle trajectories behind the aircraft cockpit.
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.
Christian Rolf, Bärbel Vogel, Peter Hoor, Armin Afchine, Gebhard Günther, Martina Krämer, Rolf Müller, Stefan Müller, Nicole Spelten, and Martin Riese
Atmos. Chem. Phys., 18, 2973–2983, https://doi.org/10.5194/acp-18-2973-2018, https://doi.org/10.5194/acp-18-2973-2018, 2018
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The Asian monsoon is a pronounced circulation system linked to rapid vertical transport of surface air from India and east Asia in the summer months. We found, based on aircraft measurements, higher concentration of water vapor in the lowermost stratosphere caused by the Asian monsoon. Enrichment of water vapor concentrations in the lowermost stratosphere impacts the radiation budget and thus climate. Understanding those variations in water vapor is important for climate projections.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
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.
Sylvia C. Sullivan, Corinna Hoose, Alexei Kiselev, Thomas Leisner, and Athanasios Nenes
Atmos. Chem. Phys., 18, 1593–1610, https://doi.org/10.5194/acp-18-1593-2018, https://doi.org/10.5194/acp-18-1593-2018, 2018
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Ice multiplication (IM) processes can have a profound impact on cloud and precipitation development but are poorly understood. Here we study whether a lower limit of ice nuclei exists to initiate IM. The lower limit is found to be extremely low (0.01 per liter or less). A counterintuitive but profound conclusion thus emerges: IM requires cloud formation around a thermodynamic
sweet spotand is sensitive to fluctuations in cloud condensation nuclei concentration alone.
George K. Georgiou, Theodoros Christoudias, Yiannis Proestos, Jonilda Kushta, Panos Hadjinicolaou, and Jos Lelieveld
Atmos. Chem. Phys., 18, 1555–1571, https://doi.org/10.5194/acp-18-1555-2018, https://doi.org/10.5194/acp-18-1555-2018, 2018
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We investigate the impact of the choice of gas-phase and aerosol mechanisms, on the simulated summertime concentrations of several pollutants over the eastern Mediterranean, using the WRF-Chem model. The selection of mechanisms significantly affects ozone and fine particulate matter concentrations, and to a lesser extent other gaseous pollutants (NOx, CO). Meteorological components are also affected by the choice of mechanisms due to the interaction of aerosols with radiation.
Meinrat O. Andreae, Armin Afchine, Rachel Albrecht, Bruna Amorim Holanda, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Micael A. Cecchini, Anja Costa, Maximilian Dollner, Daniel Fütterer, Emma Järvinen, Tina Jurkat, Thomas Klimach, Tobias Konemann, Christoph Knote, Martina Krämer, Trismono Krisna, Luiz A. T. Machado, Stephan Mertes, Andreas Minikin, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Daniel Sauer, Hans Schlager, Martin Schnaiter, Johannes Schneider, Christiane Schulz, Antonio Spanu, Vinicius B. Sperling, Christiane Voigt, Adrian Walser, Jian Wang, Bernadett Weinzierl, Manfred Wendisch, and Helmut Ziereis
Atmos. Chem. Phys., 18, 921–961, https://doi.org/10.5194/acp-18-921-2018, https://doi.org/10.5194/acp-18-921-2018, 2018
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We made airborne measurements of aerosol particle concentrations and properties over the Amazon Basin. We found extremely high concentrations of very small particles in the region between 8 and 14 km altitude all across the basin, which had been recently formed by gas-to-particle conversion at these altitudes. This makes the upper troposphere a very important source region of atmospheric particles with significant implications for the Earth's climate system.
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
Micael A. Cecchini, Luiz A. T. Machado, Manfred Wendisch, Anja Costa, Martina Krämer, Meinrat O. Andreae, Armin Afchine, Rachel I. Albrecht, Paulo Artaxo, Stephan Borrmann, Daniel Fütterer, Thomas Klimach, Christoph Mahnke, Scot T. Martin, Andreas Minikin, Sergej Molleker, Lianet H. Pardo, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, and Bernadett Weinzierl
Atmos. Chem. Phys., 17, 14727–14746, https://doi.org/10.5194/acp-17-14727-2017, https://doi.org/10.5194/acp-17-14727-2017, 2017
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This study introduces and explores the concept of gamma phase space. This space is able to represent all possible variations in the cloud droplet size distributions (DSDs). The methodology was applied to recent in situ aircraft measurements over the Amazon. It is shown that the phase space is able to represent several processes occurring in the clouds in a simple manner. The consequences for cloud studies, modeling, and the representation of the transition from warm to mixed phase are discussed.
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.
Anja Costa, Jessica Meyer, Armin Afchine, Anna Luebke, Gebhard Günther, James R. Dorsey, Martin W. Gallagher, Andre Ehrlich, Manfred Wendisch, Darrel Baumgardner, Heike Wex, and Martina Krämer
Atmos. Chem. Phys., 17, 12219–12238, https://doi.org/10.5194/acp-17-12219-2017, https://doi.org/10.5194/acp-17-12219-2017, 2017
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The paper presents 38 h of in situ cloud spectrometer observations of microphysical cloud properties in the Arctic, midlatitudes and tropics. The clouds are classified via particle concentrations, size distributions, and – as a novelty – small particle aspherical fractions. Cloud-type profiles are given for different temperatures and locations. The results confine regions where different cloud transformation processes occurred and emphasise the importance of small particle shape detection.
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.
Evelyn Jäkel, Manfred Wendisch, Trismono C. Krisna, Florian Ewald, Tobias Kölling, Tina Jurkat, Christiane Voigt, Micael A. Cecchini, Luiz A. T. Machado, Armin Afchine, Anja Costa, Martina Krämer, Meinrat O. Andreae, Ulrich Pöschl, Daniel Rosenfeld, and Tianle Yuan
Atmos. Chem. Phys., 17, 9049–9066, https://doi.org/10.5194/acp-17-9049-2017, https://doi.org/10.5194/acp-17-9049-2017, 2017
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Vertical profiles of the cloud particle phase state in tropical deep convective clouds (DCCs) were investigated using airborne imaging spectrometer measurements during the ACRIDICON-CHUVA campaign, which was conducted over the Brazilian rainforest in September 2014. A phase discrimination retrieval was applied to observations of clouds formed in different aerosol conditions. The profiles were compared to in situ and satellite measurements.
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.