Articles | Volume 19, issue 4
https://doi.org/10.5194/gmd-19-1581-2026
© Author(s) 2026. 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-19-1581-2026
© Author(s) 2026. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Prognostic simulations of mixed-phase clouds with model AC-1D v1.0: the impact of aerosol types and freezing parameterizations on ice crystal budgets
Yijia Sun
Stony Brook University, Stony Brook, NY 11794, USA
Ann M. Fridlind
NASA Goddard Institute for Space Studies, New York, NY 10025, USA
Israel Silber
Pacific Northwest National Laboratory, Richland, WA 99352, USA
Nicole Riemer
University of Illinois Urbana-Champaign, Urbana, IL 61801, USA
Daniel A. Knopf
CORRESPONDING AUTHOR
Stony Brook University, Stony Brook, NY 11794, USA
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Israel Silber, Donna M. Flynn, Jennifer M. Comstock, Erol L. Cromwell, and Brian D. Ermold
EGUsphere, https://doi.org/10.5194/egusphere-2025-6134, https://doi.org/10.5194/egusphere-2025-6134, 2026
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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We describe ASISKYCOVER, a new machine learning algorithm for pixel segmentation of all-sky imager (ASI-16) data used by the Atmospheric Radiation Measurement (ARM) User Facility. ASISKYCOVER provides cloud cover and thickness estimates, detects artifacts, and reports uncertainties. Using one year of data from the ARM Southern Great Plains site and comparisons with other ARM datasets, we demonstrate its use and robustness, which will improve cloud cover analyses and data evaluation efforts.
Oscar H. Díaz-Ibarra, Samuel G. Frederick, Jeffrey H. Curtis, Zachary D'Aquino, Peter A. Bosler, Lekha Patel, Cosmin Safta, Matthew West, and Nicole Riemer
Geosci. Model Dev., 19, 1281–1299, https://doi.org/10.5194/gmd-19-1281-2026, https://doi.org/10.5194/gmd-19-1281-2026, 2026
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We developed TChem-atm, a new open-source tool for simulating atmospheric chemistry and aerosols. As models become more detailed, traditional methods are too slow. TChem-atm runs on both standard processors and graphics processors, making these simulations faster and more efficient. The tool provides a foundation for next-generation models that improve predictions of air quality and climate.
Israel Silber, Jennifer M. Comstock, Adam K. Theisen, Michael R. Kieburtz, Zeen Zhu, and Jenni Kyrouac
Atmos. Meas. Tech., 19, 485–506, https://doi.org/10.5194/amt-19-485-2026, https://doi.org/10.5194/amt-19-485-2026, 2026
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We present PrecipBE, a multi-instrument precipitation event best-estimate data product developed at the Atmospheric Radiation Measurement (ARM) User Facility, providing time series and tabular statistics of events, which could help advance model evaluation and cloud-process studies. We demonstrate PrecipBE's utilization with a brief 30-year trend analysis of ARM Southern Great Plains (SGP) site data, suggesting shorter, less intense events, but rising annual rainfall, driven by rare extremes.
Timothy W. Juliano, Florian Tornow, Ann M. Fridlind, Andrew S. Ackerman, Gregory S. Elsaesser, Bart Geerts, Christian P. Lackner, David Painemal, Israel Silber, Mikhail Ovchinnikov, Gunilla Svensson, Michael Tjernström, Peng Wu, Alejandro Baró Pérez, Peter Bogenschutz, Dmitry Chechin, Kamal Kant Chandrakar, Jan Chylik, Andrey Debolskiy, Rostislav Fadeev, Anu Gupta, Luisa Ickes, Michail Karalis, Martin Köhler, Branko Kosović, Peter Kuma, Weiwei Li, Evgeny Mortikov, Hugh Morrison, Roel A. J. Neggers, Anna Possner, Tomi Raatikainen, Sami Romakkaniemi, Niklas Schnierstein, Shin-ichiro Shima, Nikita Silin, Mikhail Tolstykh, Lulin Xue, Meng Zhang, and Xue Zheng
EGUsphere, https://doi.org/10.5194/egusphere-2025-6217, https://doi.org/10.5194/egusphere-2025-6217, 2026
Preprint archived
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Models struggle to capture cloud and precipitation processes and their radiative effects in marine cold-air outbreaks. We use a quasi-Lagrangian framework to compare large-eddy simulation (LES) and single-column model (SCM) output with field and satellite observations. With fixed droplet and ice numbers, LES and SCM agree in liquid-only tests. In mixed-phase conditions, LES plausibly capture cloud thinning and breakup, while SCMs largely remain overcast and thereby miss cloud radiative effects.
Cristofer Jimenez, Albert Ansmann, Kevin Ohneiser, Hannes Griesche, Ronny Engelmann, Martin Radenz, Julian Hofer, Dietrich Althausen, Daniel A. Knopf, Sandro Dahlke, Johannes Bühl, Holger Baars, Patric Seifert, and Ulla Wandinger
Atmos. Chem. Phys., 25, 12955–12981, https://doi.org/10.5194/acp-25-12955-2025, https://doi.org/10.5194/acp-25-12955-2025, 2025
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We studied the water and ice phases of Arctic mixed-phase clouds (MPCs) using dual FOV polarization lidar and Doppler radar on board Polarstern during the MOSAiC expedition. Two long-lasting Arctic MPCs and year-round statistics show persistent droplet activation and dominant immersion freezing, indicating well-filled cloud condensation nuclei and ice-nucleating particle reservoirs. These findings help explain MPC longevity and may improve cloud life cycle representation in weather and climate models.
Samuel G. Frederick, Matin Mohebalhojeh, Jeffrey H. Curtis, Matthew West, and Nicole Riemer
EGUsphere, https://doi.org/10.5194/egusphere-2025-4351, https://doi.org/10.5194/egusphere-2025-4351, 2025
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We show with detailed computer simulations that spatial patterns of emissions strongly affect aerosols and their ability to seed clouds. Highly variable emissions can raise cloud-forming particle concentrations in the boundary layer by up to 25 %. Because clouds regulate climate and precipitation, these findings underscore the need to represent realistic emission patterns to improve climate predictions.
McKenna W. Stanford, Ann M. Fridlind, Andrew S. Ackerman, Bastiaan van Diedenhoven, Qian Xiao, Jian Wang, Toshihisa Matsui, Daniel Hernandez-Deckers, and Paul Lawson
Atmos. Chem. Phys., 25, 11199–11231, https://doi.org/10.5194/acp-25-11199-2025, https://doi.org/10.5194/acp-25-11199-2025, 2025
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The evolution of cloud droplets, from the point they are activated by atmospheric aerosol to the formation of precipitation, is an important process relevant to understanding cloud–climate feedbacks. This study demonstrates a benchmark framework for using novel airborne measurements and retrievals to constrain high-resolution simulations of moderately deep cumulus clouds and pathways for scaling results to large-scale models and space-based observational platforms.
Wenhan Tang, Sylwester Arabas, Jeffrey H. Curtis, Daniel A. Knopf, Matthew West, and Nicole Riemer
EGUsphere, https://doi.org/10.5194/egusphere-2025-4326, https://doi.org/10.5194/egusphere-2025-4326, 2025
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We studied how aerosol particles help form ice in clouds. Using new theory and detailed computer simulations, we found that the way different materials are mixed within these particles has a strong impact on how much ice forms. When ice-forming material is spread across all particles, more droplets freeze than when it is only in a few. This result means that to better predict clouds and climate, models need to account for how particle materials are mixed.
Florian Tornow, Ann Fridlind, George Tselioudis, Brian Cairns, Andrew Ackerman, Seethala Chellappan, David Painemal, Paquita Zuidema, Christiane Voigt, Simon Kirschler, and Armin Sorooshian
Atmos. Chem. Phys., 25, 5053–5074, https://doi.org/10.5194/acp-25-5053-2025, https://doi.org/10.5194/acp-25-5053-2025, 2025
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The recent NASA campaign ACTIVATE (Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment) performed 71 tandem flights in mid-latitude marine cold-air outbreaks off the US eastern seaboard. We provide meteorological and cloud transition stage context, allowing us to identify days that are most suitable for Lagrangian modeling and analysis. Surveyed cloud properties show signatures of cloud microphysical processes, such as cloud-top entrainment and secondary ice formation.
Albert Ansmann, Cristofer Jimenez, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Daniel A. Knopf, Sandro Dahlke, Tom Gaudek, Patric Seifert, and Ulla Wandinger
Atmos. Chem. Phys., 25, 4847–4866, https://doi.org/10.5194/acp-25-4847-2025, https://doi.org/10.5194/acp-25-4847-2025, 2025
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In this study, we focus on the potential impact of wildfire smoke on cirrus formation. For the first time, state-of-the-art aerosol and cirrus observations with lidar and radar, presented in this paper (Part 1 of a series of two articles), are closely linked to the comprehensive modeling of gravity-wave-induced ice nucleation in cirrus evolution processes, presented in a companion paper (Part 2). We found a clear impact of wildfire smoke on cirrus evolution.
Albert Ansmann, Cristofer Jimenez, Daniel A. Knopf, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, and Ronny Engelmann
Atmos. Chem. Phys., 25, 4867–4884, https://doi.org/10.5194/acp-25-4867-2025, https://doi.org/10.5194/acp-25-4867-2025, 2025
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In this study, we focus on the potential impact of wildfire smoke on cirrus formation. Aerosol and cirrus observations with lidar and radar during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition, presented in the companion paper (Ansmann et al., 2025), are closely linked to comprehensive modeling of ice nucleation in cirrus evolution processes, presented in this article. A clear impact of wildfire smoke on cirrus formation was found.
Fan Mei, Qi Zhang, Damao Zhang, Jerome D. Fast, Gourihar Kulkarni, Mikhail S. Pekour, Christopher R. Niedek, Susanne Glienke, Israel Silber, Beat Schmid, Jason M. Tomlinson, Hardeep S. Mehta, Xena Mansoura, Zezhen Cheng, Gregory W. Vandergrift, Nurun Nahar Lata, Swarup China, and Zihua Zhu
Atmos. Chem. Phys., 25, 3425–3444, https://doi.org/10.5194/acp-25-3425-2025, https://doi.org/10.5194/acp-25-3425-2025, 2025
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This study highlights the unique capability of the ArcticShark, an uncrewed aerial system, in measuring vertically resolved atmospheric properties. Data from 32 research flights in 2023 reveal seasonal patterns and correlations with conventional measurements. The consistency and complementarity of in situ and remote sensing methods are highlighted. The study demonstrates the ArcticShark’s versatility in bridging data gaps and improving the understanding of vertical atmospheric structures.
Zhouyang Zhang, Jiandong Wang, Jiaping Wang, Nicole Riemer, Chao Liu, Yuzhi Jin, Zeyuan Tian, Jing Cai, Yueyue Cheng, Ganzhen Chen, Bin Wang, Shuxiao Wang, and Aijun Ding
Atmos. Chem. Phys., 25, 1869–1881, https://doi.org/10.5194/acp-25-1869-2025, https://doi.org/10.5194/acp-25-1869-2025, 2025
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Black carbon (BC) exerts notable warming effects. We use a particle-resolved model to investigate the long-term behavior of the BC mixing state, revealing its compositions, coating thickness distribution, and optical properties all stabilize with a characteristic time of less than 1 d. This study can effectively simplify the description of the BC mixing state, which facilitates the precise assessment of the optical properties of BC aerosols in global and chemical transport models.
Israel Silber, Jennifer M. Comstock, Michael R. Kieburtz, and Lynn M. Russell
Earth Syst. Sci. Data, 17, 29–42, https://doi.org/10.5194/essd-17-29-2025, https://doi.org/10.5194/essd-17-29-2025, 2025
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We present ARMTRAJ, a set of multipurpose trajectory datasets, which augments cloud, aerosol, and boundary layer studies utilizing the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility data. ARMTRAJ data include ensemble run statistics that enhance consistency and serve as uncertainty metrics for air mass coordinates and state variables. ARMTRAJ will soon become a near real-time product that will accompany past, ongoing, and future ARM deployments.
Johannes Mülmenstädt, Andrew S. Ackerman, Ann M. Fridlind, Meng Huang, Po-Lun Ma, Naser Mahfouz, Susanne E. Bauer, Susannah M. Burrows, Matthew W. Christensen, Sudhakar Dipu, Andrew Gettelman, L. Ruby Leung, Florian Tornow, Johannes Quaas, Adam C. Varble, Hailong Wang, Kai Zhang, and Youtong Zheng
Atmos. Chem. Phys., 24, 13633–13652, https://doi.org/10.5194/acp-24-13633-2024, https://doi.org/10.5194/acp-24-13633-2024, 2024
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Stratocumulus clouds play a large role in Earth's climate by reflecting incoming solar energy back to space. Turbulence at stratocumulus cloud top mixes in dry, warm air, which can lead to cloud dissipation. This process is challenging for coarse-resolution global models to represent. We show that global models nevertheless agree well with our process understanding. Global models also think the process is less important for the climate than other lines of evidence have led us to conclude.
Jeffrey H. Curtis, Nicole Riemer, and Matthew West
Geosci. Model Dev., 17, 8399–8420, https://doi.org/10.5194/gmd-17-8399-2024, https://doi.org/10.5194/gmd-17-8399-2024, 2024
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This paper introduces a numerical method for simulating particle-based aerosol transport in atmospheric models. We detail the various numerical properties of the advection order method and demonstrate its implementation in a 3D weather prediction model (WRF) for the first time. Particle-based techniques improve the accuracy of aerosol size and composition predictions, which are key for aerosol–cloud and aerosol–radiation interactions.
Alexei Korolev, Zhipeng Qu, Jason Milbrandt, Ivan Heckman, Mélissa Cholette, Mengistu Wolde, Cuong Nguyen, Greg M. McFarquhar, Paul Lawson, and Ann M. Fridlind
Atmos. Chem. Phys., 24, 11849–11881, https://doi.org/10.5194/acp-24-11849-2024, https://doi.org/10.5194/acp-24-11849-2024, 2024
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The phenomenon of high ice water content (HIWC) occurs in mesoscale convective systems (MCSs) when a large number of small ice particles with typical sizes of a few hundred micrometers is found at high altitudes. It was found that secondary ice production in the vicinity of the melting layer plays a key role in the formation and maintenance of HIWC. This study presents a conceptual model of the formation of HIWC in tropical MCSs based on in situ observations and numerical simulation.
Abigail S. Williams, Jeramy L. Dedrick, Lynn M. Russell, Florian Tornow, Israel Silber, Ann M. Fridlind, Benjamin Swanson, Paul J. DeMott, Paul Zieger, and Radovan Krejci
Atmos. Chem. Phys., 24, 11791–11805, https://doi.org/10.5194/acp-24-11791-2024, https://doi.org/10.5194/acp-24-11791-2024, 2024
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The measured aerosol size distribution modes reveal distinct properties characteristic of cold-air outbreaks in the Norwegian Arctic. We find higher sea spray number concentrations, smaller Hoppel minima, lower effective supersaturations, and accumulation-mode particle scavenging during cold-air outbreaks. These results advance our understanding of cold-air outbreak aerosol–cloud interactions in order to improve their accurate representation in models.
Toshi Matsui, Daniel Hernandez-Deckers, Scott E. Giangrande, Thiago S. Biscaro, Ann Fridlind, and Scott Braun
Atmos. Chem. Phys., 24, 10793–10814, https://doi.org/10.5194/acp-24-10793-2024, https://doi.org/10.5194/acp-24-10793-2024, 2024
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Using computer simulations and real measurements, we discovered that storms over the Amazon were narrower but more intense during the dry periods, producing heavier rain and more ice particles in the clouds. Our research showed that cumulus bubbles played a key role in creating these intense storms. This study can improve the representation of the effect of continental and ocean environments on tropical regions' rainfall patterns in simulations.
Grégory V. Cesana, Olivia Pierpaoli, Matteo Ottaviani, Linh Vu, Zhonghai Jin, and Israel Silber
Atmos. Chem. Phys., 24, 7899–7909, https://doi.org/10.5194/acp-24-7899-2024, https://doi.org/10.5194/acp-24-7899-2024, 2024
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Better characterizing the relationship between sea ice and clouds is key to understanding Arctic climate because clouds and sea ice affect surface radiation and modulate Arctic surface warming. Our results indicate that Arctic liquid clouds robustly increase in response to sea ice decrease. This increase has a cooling effect on the surface because more solar radiation is reflected back to space, and it should contribute to dampening future Arctic surface warming.
Johannes Mülmenstädt, Edward Gryspeerdt, Sudhakar Dipu, Johannes Quaas, Andrew S. Ackerman, Ann M. Fridlind, Florian Tornow, Susanne E. Bauer, Andrew Gettelman, Yi Ming, Youtong Zheng, Po-Lun Ma, Hailong Wang, Kai Zhang, Matthew W. Christensen, Adam C. Varble, L. Ruby Leung, Xiaohong Liu, David Neubauer, Daniel G. Partridge, Philip Stier, and Toshihiko Takemura
Atmos. Chem. Phys., 24, 7331–7345, https://doi.org/10.5194/acp-24-7331-2024, https://doi.org/10.5194/acp-24-7331-2024, 2024
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Human activities release copious amounts of small particles called aerosols into the atmosphere. These particles change how much sunlight clouds reflect to space, an important human perturbation of the climate, whose magnitude is highly uncertain. We found that the latest climate models show a negative correlation but a positive causal relationship between aerosols and cloud water. This means we need to be very careful when we interpret observational studies that can only see correlation.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
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The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Kamil Mroz, Alessandro Battaglia, and Ann M. Fridlind
Atmos. Meas. Tech., 17, 1577–1597, https://doi.org/10.5194/amt-17-1577-2024, https://doi.org/10.5194/amt-17-1577-2024, 2024
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In this study, we examine the extent to which radar measurements from space can inform us about the properties of clouds and precipitation. Surprisingly, our analysis showed that the amount of ice turning into rain was lower than expected in the current product. To improve on this, we came up with a new way to extract information about the size and concentration of particles from radar data. As long as we use this method in the right conditions, we can even estimate how dense the ice is.
Rodanthi-Elisavet Mamouri, Albert Ansmann, Kevin Ohneiser, Daniel A. Knopf, Argyro Nisantzi, Johannes Bühl, Ronny Engelmann, Annett Skupin, Patric Seifert, Holger Baars, Dragos Ene, Ulla Wandinger, and Diofantos Hadjimitsis
Atmos. Chem. Phys., 23, 14097–14114, https://doi.org/10.5194/acp-23-14097-2023, https://doi.org/10.5194/acp-23-14097-2023, 2023
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For the first time, rather clear evidence is found that wildfire smoke particles can trigger strong cirrus formation. This finding is of importance because intensive and large wildfires may occur increasingly often in the future as climate change proceeds. Based on lidar observations in Cyprus in autumn 2020, we provide detailed insight into the cirrus formation at the tropopause in the presence of aged wildfire smoke (here, 8–9 day old Californian wildfire smoke).
Albert Ansmann, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Jessie M. Creamean, Matthew C. Boyer, Daniel A. Knopf, Sandro Dahlke, Marion Maturilli, Henriette Gebauer, Johannes Bühl, Cristofer Jimenez, Patric Seifert, and Ulla Wandinger
Atmos. Chem. Phys., 23, 12821–12849, https://doi.org/10.5194/acp-23-12821-2023, https://doi.org/10.5194/acp-23-12821-2023, 2023
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The 1-year MOSAiC (2019–2020) expedition with the German ice breaker Polarstern was the largest polar field campaign ever conducted. The Polarstern, with our lidar aboard, drifted with the pack ice north of 85° N for more than 7 months (October 2019 to mid-May 2020). We measured the full annual cycle of aerosol conditions in terms of aerosol optical and cloud-process-relevant properties. We observed a strong contrast between polluted winter and clean summer aerosol conditions.
McKenna W. Stanford, Ann M. Fridlind, Israel Silber, Andrew S. Ackerman, Greg Cesana, Johannes Mülmenstädt, Alain Protat, Simon Alexander, and Adrian McDonald
Atmos. Chem. Phys., 23, 9037–9069, https://doi.org/10.5194/acp-23-9037-2023, https://doi.org/10.5194/acp-23-9037-2023, 2023
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Clouds play an important role in the Earth’s climate system as they modulate the amount of radiation that either reaches the surface or is reflected back to space. This study demonstrates an approach to robustly evaluate surface-based observations against a large-scale model. We find that the large-scale model precipitates too infrequently relative to observations, contrary to literature documentation suggesting otherwise based on satellite measurements.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
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Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Sudipta Ghosh, Sagnik Dey, Sushant Das, Nicole Riemer, Graziano Giuliani, Dilip Ganguly, Chandra Venkataraman, Filippo Giorgi, Sachchida Nand Tripathi, Srikanthan Ramachandran, Thazhathakal Ayyappen Rajesh, Harish Gadhavi, and Atul Kumar Srivastava
Geosci. Model Dev., 16, 1–15, https://doi.org/10.5194/gmd-16-1-2023, https://doi.org/10.5194/gmd-16-1-2023, 2023
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Accurate representation of aerosols in climate models is critical for minimizing the uncertainty in climate projections. Here, we implement region-specific emission fluxes and a more accurate scheme for carbonaceous aerosol ageing processes in a regional climate model (RegCM4) and show that it improves model performance significantly against in situ, reanalysis, and satellite data over the Indian subcontinent. We recommend improving the model performance before using them for climate studies.
Frederic Tridon, Israel Silber, Alessandro Battaglia, Stefan Kneifel, Ann Fridlind, Petros Kalogeras, and Ranvir Dhillon
Atmos. Chem. Phys., 22, 12467–12491, https://doi.org/10.5194/acp-22-12467-2022, https://doi.org/10.5194/acp-22-12467-2022, 2022
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The role of ice precipitation in the Earth water budget is not well known because ice particles are complex, and their formation involves intricate processes. Riming of ice crystals by supercooled water droplets is an efficient process, but little is known about its importance at high latitudes. In this work, by exploiting the deployment of an unprecedented number of remote sensing systems in Antarctica, we find that riming occurs at much lower temperatures compared with the mid-latitudes.
Michael S. Diamond, Pablo E. Saide, Paquita Zuidema, Andrew S. Ackerman, Sarah J. Doherty, Ann M. Fridlind, Hamish Gordon, Calvin Howes, Jan Kazil, Takanobu Yamaguchi, Jianhao Zhang, Graham Feingold, and Robert Wood
Atmos. Chem. Phys., 22, 12113–12151, https://doi.org/10.5194/acp-22-12113-2022, https://doi.org/10.5194/acp-22-12113-2022, 2022
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Smoke from southern Africa blankets the southeast Atlantic from June-October, overlying a major transition region between overcast and scattered clouds. The smoke affects Earth's radiation budget by absorbing sunlight and changing cloud properties. We investigate these effects in regional climate and large eddy simulation models based on international field campaigns. We find that large-scale circulation changes more strongly affect cloud transitions than smoke microphysical effects in our case.
Albert Ansmann, Kevin Ohneiser, Alexandra Chudnovsky, Daniel A. Knopf, Edwin W. Eloranta, Diego Villanueva, Patric Seifert, Martin Radenz, Boris Barja, Félix Zamorano, Cristofer Jimenez, Ronny Engelmann, Holger Baars, Hannes Griesche, Julian Hofer, Dietrich Althausen, and Ulla Wandinger
Atmos. Chem. Phys., 22, 11701–11726, https://doi.org/10.5194/acp-22-11701-2022, https://doi.org/10.5194/acp-22-11701-2022, 2022
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For the first time we present a systematic study on the impact of wildfire smoke on ozone depletion in the Arctic (2020) and Antarctic stratosphere (2020, 2021). Two major fire events in Siberia and Australia were responsible for the observed record-breaking stratospheric smoke pollution. Our analyses were based on lidar observations of smoke parameters (Polarstern, Punta Arenas) and NDACC Arctic and Antarctic ozone profiles as well as on Antarctic OMI satellite observations of column ozone.
Yu Yao, Jeffrey H. Curtis, Joseph Ching, Zhonghua Zheng, and Nicole Riemer
Atmos. Chem. Phys., 22, 9265–9282, https://doi.org/10.5194/acp-22-9265-2022, https://doi.org/10.5194/acp-22-9265-2022, 2022
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Investigating the impacts of aerosol mixing state on aerosol optical properties has a long history from both the modeling and experimental perspective. In this study, we used particle-resolved simulations as a benchmark to determine the error in optical properties when using simplified aerosol representations. We found that errors in single scattering albedo due to the internal mixture assumptions can have substantial effects on calculating aerosol direct radiative forcing.
Kevin Ohneiser, Albert Ansmann, Bernd Kaifler, Alexandra Chudnovsky, Boris Barja, Daniel A. Knopf, Natalie Kaifler, Holger Baars, Patric Seifert, Diego Villanueva, Cristofer Jimenez, Martin Radenz, Ronny Engelmann, Igor Veselovskii, and Félix Zamorano
Atmos. Chem. Phys., 22, 7417–7442, https://doi.org/10.5194/acp-22-7417-2022, https://doi.org/10.5194/acp-22-7417-2022, 2022
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We present and discuss 2 years of long-term lidar observations of the largest stratospheric perturbation by wildfire smoke ever observed. The smoke originated from the record-breaking Australian fires in 2019–2020 and affects climate conditions and even the ozone layer in the Southern Hemisphere. The obvious link between dense smoke occurrence in the stratosphere and strong ozone depletion found in the Arctic and in the Antarctic in 2020 can be regarded as a new aspect of climate change.
Matthew L. Dawson, Christian Guzman, Jeffrey H. Curtis, Mario Acosta, Shupeng Zhu, Donald Dabdub, Andrew Conley, Matthew West, Nicole Riemer, and Oriol Jorba
Geosci. Model Dev., 15, 3663–3689, https://doi.org/10.5194/gmd-15-3663-2022, https://doi.org/10.5194/gmd-15-3663-2022, 2022
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Progress in identifying complex, mixed-phase physicochemical processes has resulted in an advanced understanding of the evolution of atmospheric systems but has also introduced a level of complexity that few atmospheric models were designed to handle. We present a flexible treatment for multiphase chemical processes for models of diverse scale, from box up to global models. This enables users to build a customized multiphase mechanism that is accessible to a much wider community.
Daniel A. Knopf, Joseph C. Charnawskas, Peiwen Wang, Benny Wong, Jay M. Tomlin, Kevin A. Jankowski, Matthew Fraund, Daniel P. Veghte, Swarup China, Alexander Laskin, Ryan C. Moffet, Mary K. Gilles, Josephine Y. Aller, Matthew A. Marcus, Shira Raveh-Rubin, and Jian Wang
Atmos. Chem. Phys., 22, 5377–5398, https://doi.org/10.5194/acp-22-5377-2022, https://doi.org/10.5194/acp-22-5377-2022, 2022
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Marine boundary layer aerosols collected in the remote region of the eastern North Atlantic induce immersion freezing and deposition ice nucleation under typical mixed-phase and cirrus cloud conditions. Corresponding ice nucleation parameterizations for model applications have been derived. Chemical imaging of ambient aerosol and ice-nucleating particles demonstrates that the latter is dominated by sea salt and organics while also representing a major particle type in the particle population.
Israel Silber, Robert C. Jackson, Ann M. Fridlind, Andrew S. Ackerman, Scott Collis, Johannes Verlinde, and Jiachen Ding
Geosci. Model Dev., 15, 901–927, https://doi.org/10.5194/gmd-15-901-2022, https://doi.org/10.5194/gmd-15-901-2022, 2022
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The Earth Model Column Collaboratory (EMC2) is an open-source ground-based (and air- or space-borne) lidar and radar simulator and subcolumn generator designed for large-scale models, in particular climate models, applicable also for high-resolution models. EMC2 emulates measurements while remaining faithful to large-scale models' physical assumptions implemented in their cloud or radiation schemes. We demonstrate the use of EMC2 to compare AWARE measurements with the NASA GISS ModelE3 and LES.
Daniel Hernandez-Deckers, Toshihisa Matsui, and Ann M. Fridlind
Atmos. Chem. Phys., 22, 711–724, https://doi.org/10.5194/acp-22-711-2022, https://doi.org/10.5194/acp-22-711-2022, 2022
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We investigate how the concentration of aerosols (small particles that serve as seeds for cloud droplets) affect the dynamics of simulated clouds using two different frameworks, i.e., the traditional selection of cloudy rising grid points and tracking small-scale coherent rising features (cumulus thermals). By doing so, we find that these cumulus thermals reveal useful information about the coupling between internal cloud circulations and cloud droplet and raindrop formation.
Jay M. Tomlin, Kevin A. Jankowski, Daniel P. Veghte, Swarup China, Peiwen Wang, Matthew Fraund, Johannes Weis, Guangjie Zheng, Yang Wang, Felipe Rivera-Adorno, Shira Raveh-Rubin, Daniel A. Knopf, Jian Wang, Mary K. Gilles, Ryan C. Moffet, and Alexander Laskin
Atmos. Chem. Phys., 21, 18123–18146, https://doi.org/10.5194/acp-21-18123-2021, https://doi.org/10.5194/acp-21-18123-2021, 2021
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Analysis of individual atmospheric particles shows that aerosol transported from North America during meteorological dry intrusion episodes may have a substantial impact on the mixing state and particle-type population over the mid-Atlantic, as organic contribution and particle-type diversity are significantly enhanced during these periods. These observations need to be considered in current atmospheric models.
Zhonghua Zheng, Matthew West, Lei Zhao, Po-Lun Ma, Xiaohong Liu, and Nicole Riemer
Atmos. Chem. Phys., 21, 17727–17741, https://doi.org/10.5194/acp-21-17727-2021, https://doi.org/10.5194/acp-21-17727-2021, 2021
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Aerosol mixing state is an important emergent property that affects aerosol radiative forcing and aerosol–cloud interactions, but it has not been easy to constrain this property globally. We present a framework for evaluating the error in aerosol mixing state induced by aerosol representation assumptions, which is one of the important contributors to structural uncertainty in aerosol models. Our study provides insights into potential improvements to model process representation for aerosols.
Daniel A. Knopf and Markus Ammann
Atmos. Chem. Phys., 21, 15725–15753, https://doi.org/10.5194/acp-21-15725-2021, https://doi.org/10.5194/acp-21-15725-2021, 2021
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Adsorption on and desorption of gas molecules from solid or liquid surfaces or interfaces represent the initial interaction of gas-to-condensed-phase processes that can define the physicochemical evolution of the condensed phase. We apply a thermodynamic and microscopic treatment of these multiphase processes to evaluate how adsorption and desorption rates and surface accommodation depend on the choice of adsorption model and standard states with implications for desorption energy and lifetimes.
Florian Tornow, Andrew S. Ackerman, and Ann M. Fridlind
Atmos. Chem. Phys., 21, 12049–12067, https://doi.org/10.5194/acp-21-12049-2021, https://doi.org/10.5194/acp-21-12049-2021, 2021
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Cold air outbreaks affect the local energy budget by forming bright boundary layer clouds that, once it rains, evolve into dimmer, broken cloud fields that are depleted of condensation nuclei – an evolution consistent with closed-to-open cell transitions. We find that cloud ice accelerates this evolution, primarily via riming prior to rain onset, which (1) reduces liquid water, (2) reduces condensation nuclei, and (3) leads to early precipitation cooling and moistening below cloud.
Yang Wang, Guangjie Zheng, Michael P. Jensen, Daniel A. Knopf, Alexander Laskin, Alyssa A. Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur J. Sedlacek, John E. Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria A. Zawadowicz, and Jian Wang
Atmos. Chem. Phys., 21, 11079–11098, https://doi.org/10.5194/acp-21-11079-2021, https://doi.org/10.5194/acp-21-11079-2021, 2021
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This paper reports the vertical profiles of trace gas and aerosol properties over the eastern North Atlantic, a region of persistent but diverse subtropical marine boundary layer (MBL) clouds. We examined the key processes that drive the cloud condensation nuclei (CCN) population and how it varies with season and synoptic conditions. This study helps improve the model representation of the aerosol processes in the remote MBL, reducing the simulated aerosol indirect effects.
Stefanie Kremser, Mike Harvey, Peter Kuma, Sean Hartery, Alexia Saint-Macary, John McGregor, Alex Schuddeboom, Marc von Hobe, Sinikka T. Lennartz, Alex Geddes, Richard Querel, Adrian McDonald, Maija Peltola, Karine Sellegri, Israel Silber, Cliff S. Law, Connor J. Flynn, Andrew Marriner, Thomas C. J. Hill, Paul J. DeMott, Carson C. Hume, Graeme Plank, Geoffrey Graham, and Simon Parsons
Earth Syst. Sci. Data, 13, 3115–3153, https://doi.org/10.5194/essd-13-3115-2021, https://doi.org/10.5194/essd-13-3115-2021, 2021
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Aerosol–cloud interactions over the Southern Ocean are poorly understood and remain a major source of uncertainty in climate models. This study presents ship-borne measurements, collected during a 6-week voyage into the Southern Ocean in 2018, that are an important supplement to satellite-based measurements. For example, these measurements include data on low-level clouds and aerosol composition in the marine boundary layer, which can be used in climate model evaluation efforts.
Albert Ansmann, Kevin Ohneiser, Rodanthi-Elisavet Mamouri, Daniel A. Knopf, Igor Veselovskii, Holger Baars, Ronny Engelmann, Andreas Foth, Cristofer Jimenez, Patric Seifert, and Boris Barja
Atmos. Chem. Phys., 21, 9779–9807, https://doi.org/10.5194/acp-21-9779-2021, https://doi.org/10.5194/acp-21-9779-2021, 2021
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We present retrievals of tropospheric and stratospheric height profiles of particle mass, volume, surface area concentration of wildfire smoke layers, and related cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations. The new analysis scheme is applied to ground-based lidar observations of stratospheric Australian smoke over southern South America and to spaceborne lidar observations of tropospheric North American smoke.
Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 14, 2501–2513, https://doi.org/10.5194/amt-14-2501-2021, https://doi.org/10.5194/amt-14-2501-2021, 2021
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We have developed an online method for speciated measurements of organic peroxy radicals and stabilized Criegee intermediates using chemical derivatization combined with chemical ionization mass spectrometry. Chemical derivatization prevents secondary radical reactions and eliminates potential interferences. Comparison between our measurements and results from numeric modeling shows that the method can be used for the quantification of a wide range of atmospheric radicals and intermediates.
Israel Silber, Ann M. Fridlind, Johannes Verlinde, Andrew S. Ackerman, Grégory V. Cesana, and Daniel A. Knopf
Atmos. Chem. Phys., 21, 3949–3971, https://doi.org/10.5194/acp-21-3949-2021, https://doi.org/10.5194/acp-21-3949-2021, 2021
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Long-term ground-based radar and sounding measurements over Alaska (Antarctica) indicate that more than 85 % (75 %) of supercooled clouds are precipitating at cloud base and that 75 % (50 %) are precipitating to the surface. Such high prevalence is reconciled with lesser spaceborne estimates by considering radar sensitivity. Results provide a strong observational constraint for polar cloud processes in large-scale models.
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Short summary
The role of Arctic clouds in the regional climate remains uncertain due to insufficient understanding of the amount of liquid droplets and ice crystals present in these clouds. An aerosol-cloud model is employed to examine the role of different aerosol types and freezing parameterizations on the number of ice crystals. The choice of freezing parameterization significantly changes the number of ice crystals impacting the interpretation of the evolution and warming effect of Arctic clouds.
The role of Arctic clouds in the regional climate remains uncertain due to insufficient...