Articles | Volume 26, issue 1
https://doi.org/10.5194/acp-26-269-2026
© 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/acp-26-269-2026
© Author(s) 2026. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
07 Jan 2026
Research article |
| 07 Jan 2026
| 07 Jan 2026
Uncertainty in aerosol effective radiative forcing from anthropogenic and natural aerosol parameters in ECHAM6.3-HAM2.3
SRON Space Research Organisation Netherlands, Leiden, the Netherlands
Duncan Watson-Parris
Scripps Institution of Oceanography and Halıcıoğlu Data Science Institute, University of California San Diego, La Jolla, CA, USA
Leighton A. Regayre
Met Office Hadley Centre, Exeter, UK
School of Earth and Environment, University of Leeds, Leeds, UK
Hailing Jia
SRON Space Research Organisation Netherlands, Leiden, the Netherlands
David Neubauer
ETH Zurich, Zurich, Switzerland
Aarhus University, Roskilde, Denmark
Carl Svenhag
Aarhus University, Roskilde, Denmark
Nick Schutgens
Vrije Universiteit Amsterdam, Amsterdam, the Netherlands
Athanasios Tsikerdekis
KNMI, Utrecht, the Netherlands
Athanasios Nenes
Institute of Chemical Engineering Sciences, FORTH/ICE-HT, Patras, Greece
School of Architecture, Civil and Environmental Engineering (ENAC), Laboratory of Atmospheric Processes and their Impacts (LAPI), Ecole Polytechnique Federale de Lausanne (EPFL), Lausanne, Switzerland
Muhammed Irfan
Institute of Chemical Engineering Sciences, FORTH/ICE-HT, Patras, Greece
School of Architecture, Civil and Environmental Engineering (ENAC), Laboratory of Atmospheric Processes and their Impacts (LAPI), Ecole Polytechnique Federale de Lausanne (EPFL), Lausanne, Switzerland
Department of Technical Physics, University of Eastern Finland, Kuopio, Finland
Bastiaan van Diedenhoven
SRON Space Research Organisation Netherlands, Leiden, the Netherlands
Ardit Arifi
SRON Space Research Organisation Netherlands, Leiden, the Netherlands
Guangliang Fu
SRON Space Research Organisation Netherlands, Leiden, the Netherlands
Otto P. Hasekamp
SRON Space Research Organisation Netherlands, Leiden, the Netherlands
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Clouds exist at scales that climate models struggle to represent, limiting our knowledge of how climate change may impact clouds. Here we use a new kilometer-scale global model representing an important step towards the necessary scale. We focus on how aerosol particles modify clouds, radiation, and precipitation. We find the magnitude and manner of responses tend to vary from region to region, highlighting the potential of global kilometer-scale simulations and a need to represent aerosols in climate models.
Kai Jeggle, David Neubauer, Hanin Binder, and Ulrike Lohmann
Atmos. Chem. Phys., 25, 7227–7243, https://doi.org/10.5194/acp-25-7227-2025, https://doi.org/10.5194/acp-25-7227-2025, 2025
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This work uncovers the formation regimes of cirrus clouds and how dust particles influence their properties. By applying machine learning to a combination of satellite and reanalysis data, cirrus clouds are classified into different formation regimes. Depending on the regime, increasing dust aerosol concentrations can either decrease or increase the number of ice crystals. This challenges the idea of using cloud seeding to cool the planet, as it may unintentionally lead to warming instead.
Sara M. Blichner, Theodore Khadir, Sini Talvinen, Paulo Artaxo, Liine Heikkinen, Harri Kokkola, Radovan Krejci, Muhammed Irfan, Twan van Noije, Tuukka Petäjä, Christopher Pöhlker, Øyvind Seland, Carl Svenhag, Antti Vartiainen, and Ilona Riipinen
EGUsphere, https://doi.org/10.5194/egusphere-2025-2559, https://doi.org/10.5194/egusphere-2025-2559, 2025
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This study looks at how well climate models capture the impact of rain on particles that help form cloud droplets. Using data from three measurement stations and applying both a correlation analysis and a machine learning approach, we found that models often miss how new particles form after rain and struggle in cold environments. This matters because these particles influence cloud formation and climate.
Jakob Boyd Pernov, William H. Aeberhard, Michele Volpi, Eliza Harris, Benjamin Hohermuth, Sakiko Ishino, Ragnhild B. Skeie, Stephan Henne, Ulas Im, Patricia K. Quinn, Lucia M. Upchurch, and Julia Schmale
Atmos. Chem. Phys., 25, 6497–6537, https://doi.org/10.5194/acp-25-6497-2025, https://doi.org/10.5194/acp-25-6497-2025, 2025
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Particulate methanesulfonic acid (MSAp) is vital for the Arctic climate system. Numerical models struggle to reproduce the MSAp seasonal cycle. We evaluate three numerical models and one reanalysis product’s ability to simulate MSAp. We develop data-driven models for MSAp at four Arctic stations. The data-driven models outperform the numerical models and reanalysis product and identified precursor source-, chemical-processing-, and removal-related features as being important for modeling MSAp.
Duncan Watson-Parris, Laura J. Wilcox, Camilla W. Stjern, Robert J. Allen, Geeta Persad, Massimo A. Bollasina, Annica M. L. Ekman, Carley E. Iles, Manoj Joshi, Marianne T. Lund, Daniel McCoy, Daniel M. Westervelt, Andrew I. L. Williams, and Bjørn H. Samset
Atmos. Chem. Phys., 25, 4443–4454, https://doi.org/10.5194/acp-25-4443-2025, https://doi.org/10.5194/acp-25-4443-2025, 2025
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In 2020, regulations by the International Maritime Organization aimed to reduce aerosol emissions from ships. These aerosols previously had a cooling effect, which the regulations might reduce, revealing more greenhouse gas warming. Here we find that, while there is regional warming, the global 2020–2040 temperature rise is only +0.03 °C. This small change is difficult to distinguish from natural climate variability, indicating the regulations have had a limited effect on observed warming to date.
Peer Nowack and Duncan Watson-Parris
Atmos. Chem. Phys., 25, 2365–2384, https://doi.org/10.5194/acp-25-2365-2025, https://doi.org/10.5194/acp-25-2365-2025, 2025
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In our article, we review uncertainties in global climate change projections and current methods using Earth observations as constraints, which is crucial for climate risk assessments and for informing society. We then discuss how machine learning can advance the field, discussing recent work that provides potentially stronger and more robust links between observed data and future climate projections. We further discuss the challenges of applying machine learning to climate science.
Yutao Chen, Ronald J. van der A, Jieying Ding, Henk Eskes, Jason E. Williams, Nicolas Theys, Athanasios Tsikerdekis, and Pieternel F. Levelt
Atmos. Chem. Phys., 25, 1851–1868, https://doi.org/10.5194/acp-25-1851-2025, https://doi.org/10.5194/acp-25-1851-2025, 2025
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There is a lack of local SO2 top-down emission inventories in India. With the improvement in the divergence method and the derivation of SO2 local lifetime, gridded SO2 emissions over a large area can be estimated efficiently. This method can be applied to any region in the world to derive SO2 emissions. Especially for regions with high latitudes, our methodology has the potential to significantly improve the top-down derivation of SO2 emissions.
Mariya Petrenko, Ralph Kahn, Mian Chin, Susanne E. Bauer, Tommi Bergman, Huisheng Bian, Gabriele Curci, Ben Johnson, Johannes W. Kaiser, Zak Kipling, Harri Kokkola, Xiaohong Liu, Keren Mezuman, Tero Mielonen, Gunnar Myhre, Xiaohua Pan, Anna Protonotariou, Samuel Remy, Ragnhild Bieltvedt Skeie, Philip Stier, Toshihiko Takemura, Kostas Tsigaridis, Hailong Wang, Duncan Watson-Parris, and Kai Zhang
Atmos. Chem. Phys., 25, 1545–1567, https://doi.org/10.5194/acp-25-1545-2025, https://doi.org/10.5194/acp-25-1545-2025, 2025
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We compared smoke plume simulations from 11 global models to each other and to satellite smoke amount observations aimed at constraining smoke source strength. In regions where plumes are thick and background aerosol is low, models and satellites compare well. However, the input emission inventory tends to underestimate in many places, and particle property and loss rate assumptions vary enormously among models, causing uncertainties that require systematic in situ measurements to resolve.
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Stephen R. Arnold, Leighton A. Regayre, Duseong S. Jo, Wenxiang Shen, Hao Wang, Man Yue, Jingyi Wang, Wenxin Zhang, and Ken S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2024-4135, https://doi.org/10.5194/egusphere-2024-4135, 2025
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This study uses a global chemistry-climate model to investigate how new particle formation (NPF) from highly oxygenated organic molecules (HOMs) contributes to cloud condensation nuclei (CCN) in both preindustrial (PI) and present-day (PD) environments, and its impact on aerosol indirect radiative forcing. The findings highlight the crucial role of biogenic emissions in climate change, providing new insights for carbon-neutral scenarios and enhancing understanding of aerosol-cloud interactions.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
Atmos. Chem. Phys., 25, 1333–1351, https://doi.org/10.5194/acp-25-1333-2025, https://doi.org/10.5194/acp-25-1333-2025, 2025
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This study investigates the impact of dust on the global radiative effect of nitrate aerosols. The results indicate both positive and negative regional shortwave and longwave radiative effects due to aerosol–radiation interactions and cloud adjustments. The global average net REari and REaci of nitrate aerosols are −0.11 and +0.17 W m−2, respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
Maria R. Russo, Sadie L. Bartholomew, David Hassell, Alex M. Mason, Erica Neininger, A. James Perman, David A. J. Sproson, Duncan Watson-Parris, and Nathan Luke Abraham
Geosci. Model Dev., 18, 181–191, https://doi.org/10.5194/gmd-18-181-2025, https://doi.org/10.5194/gmd-18-181-2025, 2025
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Observational data and modelling capabilities have expanded in recent years, but there are still barriers preventing these two data sources from being used in synergy. Proper comparison requires generating, storing, and handling a large amount of data. This work describes the first step in the development of a new set of software tools, the VISION toolkit, which can enable the easy and efficient integration of observational and model data required for model evaluation.
Pamela A. Dominutti, Jean-Luc Jaffrezo, Anouk Marsal, Takoua Mhadhbi, Rhabira Elazzouzi, Camille Rak, Fabrizia Cavalli, Jean-Philippe Putaud, Aikaterini Bougiatioti, Nikolaos Mihalopoulos, Despina Paraskevopoulou, Ian Mudway, Athanasios Nenes, Kaspar R. Daellenbach, Catherine Banach, Steven J. Campbell, Hana Cigánková, Daniele Contini, Greg Evans, Maria Georgopoulou, Manuella Ghanem, Drew A. Glencross, Maria Rachele Guascito, Hartmut Herrmann, Saima Iram, Maja Jovanović, Milena Jovašević-Stojanović, Markus Kalberer, Ingeborg M. Kooter, Suzanne E. Paulson, Anil Patel, Esperanza Perdrix, Maria Chiara Pietrogrande, Pavel Mikuška, Jean-Jacques Sauvain, Katerina Seitanidi, Pourya Shahpoury, Eduardo J. d. S. Souza, Sarah Steimer, Svetlana Stevanovic, Guillaume Suarez, P. S. Ganesh Subramanian, Battist Utinger, Marloes F. van Os, Vishal Verma, Xing Wang, Rodney J. Weber, Yuhan Yang, Xavier Querol, Gerard Hoek, Roy M. Harrison, and Gaëlle Uzu
Atmos. Meas. Tech., 18, 177–195, https://doi.org/10.5194/amt-18-177-2025, https://doi.org/10.5194/amt-18-177-2025, 2025
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In this work, 20 labs worldwide collaborated to evaluate the measurement of air pollution's oxidative potential (OP), a key indicator of its harmful effects. The study aimed to identify disparities in the widely used OP dithiothreitol assay and assess the consistency of OP among labs using the same protocol. The results showed that half of the labs achieved acceptable results. However, variability was also found, highlighting the need for standardisation in OP procedures.
Trude Eidhammer, Andrew Gettelman, Katherine Thayer-Calder, Duncan Watson-Parris, Gregory Elsaesser, Hugh Morrison, Marcus van Lier-Walqui, Ci Song, and Daniel McCoy
Geosci. Model Dev., 17, 7835–7853, https://doi.org/10.5194/gmd-17-7835-2024, https://doi.org/10.5194/gmd-17-7835-2024, 2024
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We describe a dataset where 45 parameters related to cloud processes in the Community Earth System Model version 2 (CESM2) Community Atmosphere Model version 6 (CAM6) are perturbed. Three sets of perturbed parameter ensembles (263 members) were created: current climate, preindustrial aerosol loading and future climate with sea surface temperature increased by 4 K.
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Wenxiang Shen, Stephen R. Arnold, Leighton A. Regayre, Meinrat O. Andreae, Mira L. Pöhlker, Duseong S. Jo, Man Yue, and Ken S. Carslaw
Atmos. Chem. Phys., 24, 11365–11389, https://doi.org/10.5194/acp-24-11365-2024, https://doi.org/10.5194/acp-24-11365-2024, 2024
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Highly oxygenated organic molecules (HOMs) play an important role in atmospheric new particle formation (NPF). By semi-explicitly coupling the chemical mechanism of HOMs and a comprehensive nucleation scheme in a global climate model, the updated model shows better agreement with measurements of nucleation rate, growth rate, and NPF event frequency. Our results reveal that HOM-driven NPF leads to a considerable increase in particle and cloud condensation nuclei burden globally.
Jiemei Liu, Jesper H. Christensen, Zhuyun Ye, Shikui Dong, Camilla Geels, Jørgen Brandt, Athanasios Nenes, Yuan Yuan, and Ulas Im
Atmos. Chem. Phys., 24, 10849–10867, https://doi.org/10.5194/acp-24-10849-2024, https://doi.org/10.5194/acp-24-10849-2024, 2024
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China was chosen as an example to conduct a quantitative analysis using the Danish Eulerian Hemispheric Model (DEHM) system with meteorological input from the Weather Research and Forecasting (WRF) model. Meteorological conditions and emission inventories contributed 46 % (65 %) and 54 % (35 %) to the variations in PM2.5 concentrations (oxidative potential – OP), respectively, highlighting secondary aerosol formation and biomass burning as the primary contributors to PM2.5 and OP levels.
Manu Anna Thomas, Klaus Wyser, Shiyu Wang, Marios Chatziparaschos, Paraskevi Georgakaki, Montserrat Costa-Surós, Maria Gonçalves Ageitos, Maria Kanakidou, Carlos Pérez García-Pando, Athanasios Nenes, Twan van Noije, Philippe Le Sager, and Abhay Devasthale
Geosci. Model Dev., 17, 6903–6927, https://doi.org/10.5194/gmd-17-6903-2024, https://doi.org/10.5194/gmd-17-6903-2024, 2024
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Aerosol–cloud interactions occur at a range of spatio-temporal scales. While evaluating recent developments in EC-Earth3-AerChem, this study aims to understand the extent to which the Twomey effect manifests itself at larger scales. We find a reduction in the warm bias over the Southern Ocean due to model improvements. While we see footprints of the Twomey effect at larger scales, the negative relationship between cloud droplet number and liquid water drives the shortwave radiative effect.
Kunfeng Gao, Franziska Vogel, Romanos Foskinis, Stergios Vratolis, Maria I. Gini, Konstantinos Granakis, Anne-Claire Billault-Roux, Paraskevi Georgakaki, Olga Zografou, Prodromos Fetfatzis, Alexis Berne, Alexandros Papayannis, Konstantinos Eleftheridadis, Ottmar Möhler, and Athanasios Nenes
Atmos. Chem. Phys., 24, 9939–9974, https://doi.org/10.5194/acp-24-9939-2024, https://doi.org/10.5194/acp-24-9939-2024, 2024
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Ice nucleating particle (INP) concentrations are required for correct predictions of clouds and precipitation in a changing climate, but they are poorly constrained in climate models. We unravel source contributions to INPs in the eastern Mediterranean and find that biological particles are important, regardless of their origin. The parameterizations developed exhibit superior performance and enable models to consider biological-particle effects on INPs.
Romanos Foskinis, Ghislain Motos, Maria I. Gini, Olga Zografou, Kunfeng Gao, Stergios Vratolis, Konstantinos Granakis, Ville Vakkari, Kalliopi Violaki, Andreas Aktypis, Christos Kaltsonoudis, Zongbo Shi, Mika Komppula, Spyros N. Pandis, Konstantinos Eleftheriadis, Alexandros Papayannis, and Athanasios Nenes
Atmos. Chem. Phys., 24, 9827–9842, https://doi.org/10.5194/acp-24-9827-2024, https://doi.org/10.5194/acp-24-9827-2024, 2024
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Analysis of modeling, in situ, and remote sensing measurements reveals the microphysical state of orographic clouds and their response to aerosol from the boundary layer and free troposphere. We show that cloud response to aerosol is robust, as predicted supersaturation and cloud droplet number levels agree with those determined from in-cloud measurements. The ability to determine if clouds are velocity- or aerosol-limited allows for novel model constraints and remote sensing products.
Henk Eskes, Athanasios Tsikerdekis, Melanie Ades, Mihai Alexe, Anna Carlin Benedictow, Yasmine Bennouna, Lewis Blake, Idir Bouarar, Simon Chabrillat, Richard Engelen, Quentin Errera, Johannes Flemming, Sebastien Garrigues, Jan Griesfeller, Vincent Huijnen, Luka Ilić, Antje Inness, John Kapsomenakis, Zak Kipling, Bavo Langerock, Augustin Mortier, Mark Parrington, Isabelle Pison, Mikko Pitkänen, Samuel Remy, Andreas Richter, Anja Schoenhardt, Michael Schulz, Valerie Thouret, Thorsten Warneke, Christos Zerefos, and Vincent-Henri Peuch
Atmos. Chem. Phys., 24, 9475–9514, https://doi.org/10.5194/acp-24-9475-2024, https://doi.org/10.5194/acp-24-9475-2024, 2024
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The Copernicus Atmosphere Monitoring Service (CAMS) provides global analyses and forecasts of aerosols and trace gases in the atmosphere. On 27 June 2023 a major upgrade, Cy48R1, became operational. Comparisons with in situ, surface remote sensing, aircraft, and balloon and satellite observations show that the new CAMS system is a significant improvement. The results quantify the skill of CAMS to forecast impactful events, such as wildfires, dust storms and air pollution peaks.
Jianqi Zhao, Xiaoyan Ma, Johannes Quaas, and Hailing Jia
Atmos. Chem. Phys., 24, 9101–9118, https://doi.org/10.5194/acp-24-9101-2024, https://doi.org/10.5194/acp-24-9101-2024, 2024
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We explore aerosol–cloud interactions in liquid-phase clouds over eastern China and its adjacent ocean in winter based on the WRF-Chem–SBM model, which couples a spectral-bin microphysics scheme and an online aerosol module. Our study highlights the differences in aerosol–cloud interactions between land and ocean and between precipitation clouds and non-precipitation clouds, and it differentiates and quantifies their underlying mechanisms.
Olga Zografou, Maria Gini, Prodromos Fetfatzis, Konstantinos Granakis, Romanos Foskinis, Manousos Ioannis Manousakas, Fotios Tsopelas, Evangelia Diapouli, Eleni Dovrou, Christina N. Vasilakopoulou, Alexandros Papayannis, Spyros N. Pandis, Athanasios Nenes, and Konstantinos Eleftheriadis
Atmos. Chem. Phys., 24, 8911–8926, https://doi.org/10.5194/acp-24-8911-2024, https://doi.org/10.5194/acp-24-8911-2024, 2024
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Characterization of PM1 and positive matrix factorization (PMF) source apportionment of organic and inorganic fractions were conducted at the high-altitude station (HAC)2. Cloud presence reduced PM1, affecting sulfate more than organics. Free-troposphere (FT) conditions showed more black carbon (eBC) than planetary boundary layer (PBL) conditions.
Emilie Fons, Ann Kristin Naumann, David Neubauer, Theresa Lang, and Ulrike Lohmann
Atmos. Chem. Phys., 24, 8653–8675, https://doi.org/10.5194/acp-24-8653-2024, https://doi.org/10.5194/acp-24-8653-2024, 2024
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Aerosols can modify the liquid water path (LWP) of stratocumulus and, thus, their radiative effect. We compare storm-resolving model and satellite data that disagree on the sign of LWP adjustments and diagnose this discrepancy with causal inference. We find that strong precipitation, the absence of wet scavenging, and cloud deepening under a weak inversion contribute to positive LWP adjustments to aerosols in the model, despite weak negative effects from cloud-top entrainment enhancement.
Muhammed Irfan, Thomas Kühn, Taina Yli-Juuti, Anton Laakso, Eemeli Holopainen, Douglas R. Worsnop, Annele Virtanen, and Harri Kokkola
Atmos. Chem. Phys., 24, 8489–8506, https://doi.org/10.5194/acp-24-8489-2024, https://doi.org/10.5194/acp-24-8489-2024, 2024
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The study examines how the volatility of semi-volatile organic compounds affects secondary organic aerosol (SOA) formation and climate. Our simulations show that uncertainties in these volatilities influence aerosol mass and climate impacts. Accurate representation of these compounds in climate models is crucial for predicting global climate patterns.
Alkiviadis Kalisoras, Aristeidis K. Georgoulias, Dimitris Akritidis, Robert J. Allen, Vaishali Naik, Chaincy Kuo, Sophie Szopa, Pierre Nabat, Dirk Olivié, Twan van Noije, Philippe Le Sager, David Neubauer, Naga Oshima, Jane Mulcahy, Larry W. Horowitz, and Prodromos Zanis
Atmos. Chem. Phys., 24, 7837–7872, https://doi.org/10.5194/acp-24-7837-2024, https://doi.org/10.5194/acp-24-7837-2024, 2024
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Effective radiative forcing (ERF) is a metric for estimating how human activities and natural agents change the energy flow into and out of the Earth’s climate system. We investigate the anthropogenic aerosol ERF, and we estimate the contribution of individual processes to the total ERF using simulations from Earth system models within the Coupled Model Intercomparison Project Phase 6 (CMIP6). Our findings highlight that aerosol–cloud interactions drive ERF variability during the last 150 years.
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.
Carl Svenhag, Moa K. Sporre, Tinja Olenius, Daniel Yazgi, Sara M. Blichner, Lars P. Nieradzik, and Pontus Roldin
Geosci. Model Dev., 17, 4923–4942, https://doi.org/10.5194/gmd-17-4923-2024, https://doi.org/10.5194/gmd-17-4923-2024, 2024
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Our research shows the importance of modeling new particle formation (NPF) and growth of particles in the atmosphere on a global scale, as they influence the outcomes of clouds and our climate. With the global model EC-Earth3 we show that using a new method for NPF modeling, which includes new detailed processes with NH3 and H2SO4, significantly impacts the number of particles in the air and clouds and changes the radiation balance of the same magnitude as anthropogenic greenhouse emissions.
Fangxuan Ren, Jintai Lin, Chenghao Xu, Jamiu A. Adeniran, Jingxu Wang, Randall V. Martin, Aaron van Donkelaar, Melanie S. Hammer, Larry W. Horowitz, Steven T. Turnock, Naga Oshima, Jie Zhang, Susanne Bauer, Kostas Tsigaridis, Øyvind Seland, Pierre Nabat, David Neubauer, Gary Strand, Twan van Noije, Philippe Le Sager, and Toshihiko Takemura
Geosci. Model Dev., 17, 4821–4836, https://doi.org/10.5194/gmd-17-4821-2024, https://doi.org/10.5194/gmd-17-4821-2024, 2024
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We evaluate the performance of 14 CMIP6 ESMs in simulating total PM2.5 and its 5 components over China during 2000–2014. PM2.5 and its components are underestimated in almost all models, except that black carbon (BC) and sulfate are overestimated in two models, respectively. The underestimation is the largest for organic carbon (OC) and the smallest for BC. Models reproduce the observed spatial pattern for OC, sulfate, nitrate and ammonium well, yet the agreement is poorer for BC.
Zane Dedekind, Ulrike Proske, Sylvaine Ferrachat, Ulrike Lohmann, and David Neubauer
Atmos. Chem. Phys., 24, 5389–5404, https://doi.org/10.5194/acp-24-5389-2024, https://doi.org/10.5194/acp-24-5389-2024, 2024
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Ice particles precipitating into lower clouds from an upper cloud, the seeder–feeder process, can enhance precipitation. A numerical modeling study conducted in the Swiss Alps found that 48 % of observed clouds were overlapping, with the seeder–feeder process occurring in 10 % of these clouds. Inhibiting the seeder–feeder process reduced the surface precipitation and ice particle growth rates, which were further reduced when additional ice multiplication processes were included in the model.
Zihao Yuan, Guangliang Fu, Bastiaan van Diedenhoven, Hai Xiang Lin, Jan Willem Erisman, and Otto P. Hasekamp
Atmos. Meas. Tech., 17, 2595–2610, https://doi.org/10.5194/amt-17-2595-2024, https://doi.org/10.5194/amt-17-2595-2024, 2024
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Currently, aerosol properties from spaceborne multi-angle polarimeter (MAP) instruments can only be retrieved in cloud-free areas or in areas where an aerosol layer is located above a cloud. Therefore, it is important to be able to identify cloud-free pixels for which an aerosol retrieval algorithm can provide meaningful output. The developed neural network cloud screening demonstrates that cloud masking for MAP aerosol retrieval can be based on the MAP measurements themselves.
Stephanie Fiedler, Vaishali Naik, Fiona M. O'Connor, Christopher J. Smith, Paul Griffiths, Ryan J. Kramer, Toshihiko Takemura, Robert J. Allen, Ulas Im, Matthew Kasoar, Angshuman Modak, Steven Turnock, Apostolos Voulgarakis, Duncan Watson-Parris, Daniel M. Westervelt, Laura J. Wilcox, Alcide Zhao, William J. Collins, Michael Schulz, Gunnar Myhre, and Piers M. Forster
Geosci. Model Dev., 17, 2387–2417, https://doi.org/10.5194/gmd-17-2387-2024, https://doi.org/10.5194/gmd-17-2387-2024, 2024
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Climate scientists want to better understand modern climate change. Thus, climate model experiments are performed and compared. The results of climate model experiments differ, as assessed in the latest Intergovernmental Panel on Climate Change (IPCC) assessment report. This article gives insights into the challenges and outlines opportunities for further improving the understanding of climate change. It is based on views of a group of experts in atmospheric composition–climate interactions.
Otto Hasekamp, Pavel Litvinov, Guangliang Fu, Cheng Chen, and Oleg Dubovik
Atmos. Meas. Tech., 17, 1497–1525, https://doi.org/10.5194/amt-17-1497-2024, https://doi.org/10.5194/amt-17-1497-2024, 2024
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Aerosols are particles in the atmosphere that cool the climate by reflecting and absorbing sunlight (direct effect) and changing cloud properties (indirect effect). The scale of aerosol cooling is uncertain, hampering accurate climate predictions. We compare two algorithms for the retrieval of aerosol properties from multi-angle polarimetric measurements: Generalized Retrieval of Atmosphere and Surface Properties (GRASP) and Remote sensing of Trace gas and Aerosol Products (RemoTAP).
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024, https://doi.org/10.5194/acp-24-1939-2024, 2024
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The 2014–15 Holuhraun eruption caused a huge aerosol plume in an otherwise unpolluted region, providing a chance to study how aerosol alters cloud properties. This two-part study uses observations and models to quantify this relationship’s impact on the Earth’s energy budget. Part 1 suggests the models capture the observed spatial and chemical evolution of the plume, yet no model plume is exact. Understanding these differences is key for Part 2, where changes to cloud properties are explored.
Alexandros Milousis, Alexandra P. Tsimpidi, Holger Tost, Spyros N. Pandis, Athanasios Nenes, Astrid Kiendler-Scharr, and Vlassis A. Karydis
Geosci. Model Dev., 17, 1111–1131, https://doi.org/10.5194/gmd-17-1111-2024, https://doi.org/10.5194/gmd-17-1111-2024, 2024
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This study aims to evaluate the newly developed ISORROPIA-lite aerosol thermodynamic module within the EMAC model and explore discrepancies in global atmospheric simulations of aerosol composition and acidity by utilizing different aerosol phase states. Even though local differences were found in regions where the RH ranged from 20 % to 60 %, on a global scale the results are similar. Therefore, ISORROPIA-lite can be a reliable and computationally effective alternative to ISORROPIA II in EMAC.
Zihan Zhang, Guangliang Fu, and Otto Hasekamp
Atmos. Meas. Tech., 16, 6051–6063, https://doi.org/10.5194/amt-16-6051-2023, https://doi.org/10.5194/amt-16-6051-2023, 2023
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In order to conduct accurate aerosol retrieval over snow, the Remote Sensing of Trace Gases and Aerosol Products (RemoTAP) algorithm is extended with a bi-directional reflection distribution function for snow surfaces. The experiments with both synthetic and real data show that the extended RemoTAP maintains capability for snow-free pixels and has obvious advantages in accuracy and the fraction of successful retrievals for retrieval over snow, especially over surfaces with snow cover > 75 %.
Yusuf A. Bhatti, Laura E. Revell, Alex J. Schuddeboom, Adrian J. McDonald, Alex T. Archibald, Jonny Williams, Abhijith U. Venugopal, Catherine Hardacre, and Erik Behrens
Atmos. Chem. Phys., 23, 15181–15196, https://doi.org/10.5194/acp-23-15181-2023, https://doi.org/10.5194/acp-23-15181-2023, 2023
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Aerosols are a large source of uncertainty over the Southern Ocean. A dominant source of sulfate aerosol in this region is dimethyl sulfide (DMS), which is poorly simulated by climate models. We show the sensitivity of simulated atmospheric DMS to the choice of oceanic DMS data set and emission scheme. We show that oceanic DMS has twice the influence on atmospheric DMS than the emission scheme. Simulating DMS more accurately in climate models will help to constrain aerosol uncertainty.
Meng Gao, Bryan A. Franz, Peng-Wang Zhai, Kirk Knobelspiesse, Andrew M. Sayer, Xiaoguang Xu, J. Vanderlei Martins, Brian Cairns, Patricia Castellanos, Guangliang Fu, Neranga Hannadige, Otto Hasekamp, Yongxiang Hu, Amir Ibrahim, Frederick Patt, Anin Puthukkudy, and P. Jeremy Werdell
Atmos. Meas. Tech., 16, 5863–5881, https://doi.org/10.5194/amt-16-5863-2023, https://doi.org/10.5194/amt-16-5863-2023, 2023
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This study evaluated the retrievability and uncertainty of aerosol and ocean properties from PACE's HARP2 instrument using enhanced neural network models with the FastMAPOL algorithm. A cascading retrieval method is developed to improve retrieval performance. A global set of simulated HARP2 data is generated and used for uncertainty evaluations. The performance assessment demonstrates that the FastMAPOL algorithm is a viable approach for operational application to HARP2 data after PACE launch.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
Atmos. Chem. Phys., 23, 14779–14799, https://doi.org/10.5194/acp-23-14779-2023, https://doi.org/10.5194/acp-23-14779-2023, 2023
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We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emission seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a
hiddensource of inter-model variability and may be leading to bias in some climate model results.
Ghislain Motos, Gabriel Freitas, Paraskevi Georgakaki, Jörg Wieder, Guangyu Li, Wenche Aas, Chris Lunder, Radovan Krejci, Julie Thérèse Pasquier, Jan Henneberger, Robert Oscar David, Christoph Ritter, Claudia Mohr, Paul Zieger, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13941–13956, https://doi.org/10.5194/acp-23-13941-2023, https://doi.org/10.5194/acp-23-13941-2023, 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 this information to the sources of aerosol found during each season and to processes of cloud glaciation.
Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg M. McFarquhar, James Podolske, Jens Redemann, Arthur J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema
Atmos. Chem. Phys., 23, 13911–13940, https://doi.org/10.5194/acp-23-13911-2023, https://doi.org/10.5194/acp-23-13911-2023, 2023
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To better understand smoke properties and its interactions with clouds, we compare the WRF-CAM5 model with observations from ORACLES, CLARIFY, and LASIC field campaigns in the southeastern Atlantic in August 2017. The model transports and mixes smoke well but does not fully capture some important processes. These include smoke chemical and physical aging over 4–12 days, smoke removal by rain, sulfate particle formation, aerosol activation into cloud droplets, and boundary layer turbulence.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
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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 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
Peter Manshausen, Duncan Watson-Parris, Matthew W. Christensen, Jukka-Pekka Jalkanen, and Philip Stier
Atmos. Chem. Phys., 23, 12545–12555, https://doi.org/10.5194/acp-23-12545-2023, https://doi.org/10.5194/acp-23-12545-2023, 2023
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Aerosol from burning fuel changes cloud properties, e.g., the number of droplets and the content of water. Here, we study how clouds respond to different amounts of shipping aerosol. Droplet numbers increase linearly with increasing aerosol over a broad range until they stop increasing, while the amount of liquid water always increases, independently of emission amount. These changes in cloud properties can make them reflect more or less sunlight, which is important for the earth's climate.
Guangyu Li, Elise K. Wilbourn, Zezhen Cheng, Jörg Wieder, Allison Fagerson, Jan Henneberger, Ghislain Motos, Rita Traversi, Sarah D. Brooks, Mauro Mazzola, Swarup China, Athanasios Nenes, Ulrike Lohmann, Naruki Hiranuma, and Zamin A. Kanji
Atmos. Chem. Phys., 23, 10489–10516, https://doi.org/10.5194/acp-23-10489-2023, https://doi.org/10.5194/acp-23-10489-2023, 2023
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In this work, we present results from an Arctic field campaign (NASCENT) in Ny-Ålesund, Svalbard, on the abundance, variability, physicochemical properties, and potential sources of ice-nucleating particles (INPs) relevant for mixed-phase cloud formation. This work improves the data coverage of Arctic INPs and aerosol properties, allowing for the validation of models predicting cloud microphysical and radiative properties of mixed-phase clouds in the rapidly warming Arctic.
Anne-Claire Billault-Roux, Paraskevi Georgakaki, Josué Gehring, Louis Jaffeux, Alfons Schwarzenboeck, Pierre Coutris, Athanasios Nenes, and Alexis Berne
Atmos. Chem. Phys., 23, 10207–10234, https://doi.org/10.5194/acp-23-10207-2023, https://doi.org/10.5194/acp-23-10207-2023, 2023
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Secondary ice production plays a key role in clouds and precipitation. In this study, we analyze radar measurements from a snowfall event in the Jura Mountains. Complex signatures are observed, which reveal that ice crystals were formed through various processes. An analysis of multi-sensor data suggests that distinct ice multiplication processes were taking place. Both the methods used and the insights gained through this case study contribute to a better understanding of snowfall microphysics.
Mária Lbadaoui-Darvas, Ari Laaksonen, and Athanasios Nenes
Atmos. Chem. Phys., 23, 10057–10074, https://doi.org/10.5194/acp-23-10057-2023, https://doi.org/10.5194/acp-23-10057-2023, 2023
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Heterogeneous ice nucleation is the main ice formation mechanism in clouds. The mechanism of different freezing modes is to date unknown, which results in large model biases. Experiments do not allow for direct observation of ice nucleation at its native resolution. This work uses first principles molecular simulations to determine the mechanism of the least-understood ice nucleation mode and link it to adsorption through a novel modeling framework that unites ice and droplet formation.
Athanasios Tsikerdekis, Otto P. Hasekamp, Nick A. J. Schutgens, and Qirui Zhong
Atmos. Chem. Phys., 23, 9495–9524, https://doi.org/10.5194/acp-23-9495-2023, https://doi.org/10.5194/acp-23-9495-2023, 2023
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Aerosols are tiny particles of different substances (species) that can be emitted into the atmosphere by natural processes or by anthropogenic activities. However, the actual aerosol emission amount per species is highly uncertain. Thus in this work we correct the aerosol emissions used to drive a global aerosol–climate model using satellite observations through a process called data assimilation. These more accurate aerosol emissions can lead to a more accurate weather and climate prediction.
Leighton A. Regayre, Lucia Deaconu, Daniel P. Grosvenor, David M. H. Sexton, Christopher Symonds, Tom Langton, Duncan Watson-Paris, Jane P. Mulcahy, Kirsty J. Pringle, Mark Richardson, Jill S. Johnson, John W. Rostron, Hamish Gordon, Grenville Lister, Philip Stier, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 8749–8768, https://doi.org/10.5194/acp-23-8749-2023, https://doi.org/10.5194/acp-23-8749-2023, 2023
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Aerosol forcing of Earth’s energy balance has persisted as a major cause of uncertainty in climate simulations over generations of climate model development. We show that structural deficiencies in a climate model are exposed by comprehensively exploring parametric uncertainty and that these deficiencies limit how much the model uncertainty can be reduced through observational constraint. This provides a future pathway towards building models with greater physical realism and lower uncertainty.
Armin Sorooshian, Mikhail D. Alexandrov, Adam D. Bell, Ryan Bennett, Grace Betito, Sharon P. Burton, Megan E. Buzanowicz, Brian Cairns, Eduard V. Chemyakin, Gao Chen, Yonghoon Choi, Brian L. Collister, Anthony L. Cook, Andrea F. Corral, Ewan C. Crosbie, Bastiaan van Diedenhoven, Joshua P. DiGangi, Glenn S. Diskin, Sanja Dmitrovic, Eva-Lou Edwards, Marta A. Fenn, Richard A. Ferrare, David van Gilst, Johnathan W. Hair, David B. Harper, Miguel Ricardo A. Hilario, Chris A. Hostetler, Nathan Jester, Michael Jones, Simon Kirschler, Mary M. Kleb, John M. Kusterer, Sean Leavor, Joseph W. Lee, Hongyu Liu, Kayla McCauley, Richard H. Moore, Joseph Nied, Anthony Notari, John B. Nowak, David Painemal, Kasey E. Phillips, Claire E. Robinson, Amy Jo Scarino, Joseph S. Schlosser, Shane T. Seaman, Chellappan Seethala, Taylor J. Shingler, Michael A. Shook, Kenneth A. Sinclair, William L. Smith Jr., Douglas A. Spangenberg, Snorre A. Stamnes, Kenneth L. Thornhill, Christiane Voigt, Holger Vömel, Andrzej P. Wasilewski, Hailong Wang, Edward L. Winstead, Kira Zeider, Xubin Zeng, Bo Zhang, Luke D. Ziemba, and Paquita Zuidema
Earth Syst. Sci. Data, 15, 3419–3472, https://doi.org/10.5194/essd-15-3419-2023, https://doi.org/10.5194/essd-15-3419-2023, 2023
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The NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) produced a unique dataset for research into aerosol–cloud–meteorology interactions. HU-25 Falcon and King Air aircraft conducted systematic and spatially coordinated flights over the northwest Atlantic Ocean. This paper describes the ACTIVATE flight strategy, instrument and complementary dataset products, data access and usage details, and data application notes.
Colin Tully, David Neubauer, Diego Villanueva, and Ulrike Lohmann
Atmos. Chem. Phys., 23, 7673–7698, https://doi.org/10.5194/acp-23-7673-2023, https://doi.org/10.5194/acp-23-7673-2023, 2023
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This study details the first attempt with a GCM to simulate a fully prognostic aerosol species specifically for cirrus climate intervention. The new approach is in line with the real-world delivery mechanism via aircraft. However, to achieve an appreciable signal from seeding, smaller particles were needed, and their mass emissions needed to be scaled by at least a factor of 100. These biases contributed to either overseeding or small and insignificant effects in response to seeding cirrus.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
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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.
Colin Tully, David Neubauer, and Ulrike Lohmann
Geosci. Model Dev., 16, 2957–2973, https://doi.org/10.5194/gmd-16-2957-2023, https://doi.org/10.5194/gmd-16-2957-2023, 2023
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A new method to simulate deterministic ice nucleation processes based on the differential activated fraction was evaluated against a cumulative approach. Box model simulations of heterogeneous-only ice nucleation within cirrus suggest that the latter approach likely underpredicts the ice crystal number concentration. Longer simulations with a GCM show that choosing between these two approaches impacts ice nucleation competition within cirrus but leads to small and insignificant climate effects.
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.
Edward Gryspeerdt, Adam C. Povey, Roy G. Grainger, Otto Hasekamp, N. Christina Hsu, Jane P. Mulcahy, Andrew M. Sayer, and Armin Sorooshian
Atmos. Chem. Phys., 23, 4115–4122, https://doi.org/10.5194/acp-23-4115-2023, https://doi.org/10.5194/acp-23-4115-2023, 2023
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The impact of aerosols on clouds is one of the largest uncertainties in the human forcing of the climate. Aerosol can increase the concentrations of droplets in clouds, but observational and model studies produce widely varying estimates of this effect. We show that these estimates can be reconciled if only polluted clouds are studied, but this is insufficient to constrain the climate impact of aerosol. The uncertainty in aerosol impact on clouds is currently driven by cases with little aerosol.
Anna Agustí-Panareda, Jérôme Barré, Sébastien Massart, Antje Inness, Ilse Aben, Melanie Ades, Bianca C. Baier, Gianpaolo Balsamo, Tobias Borsdorff, Nicolas Bousserez, Souhail Boussetta, Michael Buchwitz, Luca Cantarello, Cyril Crevoisier, Richard Engelen, Henk Eskes, Johannes Flemming, Sébastien Garrigues, Otto Hasekamp, Vincent Huijnen, Luke Jones, Zak Kipling, Bavo Langerock, Joe McNorton, Nicolas Meilhac, Stefan Noël, Mark Parrington, Vincent-Henri Peuch, Michel Ramonet, Miha Razinger, Maximilian Reuter, Roberto Ribas, Martin Suttie, Colm Sweeney, Jérôme Tarniewicz, and Lianghai Wu
Atmos. Chem. Phys., 23, 3829–3859, https://doi.org/10.5194/acp-23-3829-2023, https://doi.org/10.5194/acp-23-3829-2023, 2023
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We present a global dataset of atmospheric CO2 and CH4, the two most important human-made greenhouse gases, which covers almost 2 decades (2003–2020). It is produced by combining satellite data of CO2 and CH4 with a weather and air composition prediction model, and it has been carefully evaluated against independent observations to ensure validity and point out deficiencies to the user. This dataset can be used for scientific studies in the field of climate change and the global carbon cycle.
Jianqi Zhao, Xiaoyan Ma, Johannes Quaas, and Hailing Jia
EGUsphere, https://doi.org/10.5194/egusphere-2023-331, https://doi.org/10.5194/egusphere-2023-331, 2023
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We improve the ability of WRF-Chem model to simulate aerosol-cloud physical and chemical processes by coupling a spectral-bin cloud microphysics scheme and online aerosol module, and consequently explore the aerosol-cloud interactions over eastern China and its adjacent ocean in boreal winter. Our study highlights the differences in aerosol-cloud interactions between land and ocean, precipitation clouds and non-precipitation clouds, and differentiates and quantifies their underlying mechanisms.
Marine Bonazzola, Hélène Chepfer, Po-Lun Ma, Johannes Quaas, David M. Winker, Artem Feofilov, and Nick Schutgens
Geosci. Model Dev., 16, 1359–1377, https://doi.org/10.5194/gmd-16-1359-2023, https://doi.org/10.5194/gmd-16-1359-2023, 2023
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Aerosol has a large impact on climate. Using a lidar aerosol simulator ensures consistent comparisons between modeled and observed aerosol. We present a lidar aerosol simulator that applies a cloud masking and an aerosol detection threshold. We estimate the lidar signals that would be observed at 532 nm by the Cloud-Aerosol Lidar with Orthogonal Polarization overflying the atmosphere predicted by a climate model. Our comparison at the seasonal timescale shows a discrepancy in the Southern Ocean.
Andrew M. Sayer, Luca Lelli, Brian Cairns, Bastiaan van Diedenhoven, Amir Ibrahim, Kirk D. Knobelspiesse, Sergey Korkin, and P. Jeremy Werdell
Atmos. Meas. Tech., 16, 969–996, https://doi.org/10.5194/amt-16-969-2023, https://doi.org/10.5194/amt-16-969-2023, 2023
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This paper presents a method to estimate the height of the top of clouds above Earth's surface using satellite measurements. It is based on light absorption by oxygen in Earth's atmosphere, which darkens the signal that a satellite will see at certain wavelengths of light. Clouds "shield" the satellite from some of this darkening, dependent on cloud height (and other factors), because clouds scatter light at these wavelengths. The method will be applied to the future NASA PACE mission.
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.
Cynthia H. Whaley, Kathy S. Law, Jens Liengaard Hjorth, Henrik Skov, Stephen R. Arnold, Joakim Langner, Jakob Boyd Pernov, Garance Bergeron, Ilann Bourgeois, Jesper H. Christensen, Rong-You Chien, Makoto Deushi, Xinyi Dong, Peter Effertz, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Greg Huey, Ulas Im, Rigel Kivi, Louis Marelle, Tatsuo Onishi, Naga Oshima, Irina Petropavlovskikh, Jeff Peischl, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Tom Ryerson, Ragnhild Skeie, Sverre Solberg, Manu A. Thomas, Chelsea Thompson, Kostas Tsigaridis, Svetlana Tsyro, Steven T. Turnock, Knut von Salzen, and David W. Tarasick
Atmos. Chem. Phys., 23, 637–661, https://doi.org/10.5194/acp-23-637-2023, https://doi.org/10.5194/acp-23-637-2023, 2023
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This study summarizes recent research on ozone in the Arctic, a sensitive and rapidly warming region. We find that the seasonal cycles of near-surface atmospheric ozone are variable depending on whether they are near the coast, inland, or at high altitude. Several global model simulations were evaluated, and we found that because models lack some of the ozone chemistry that is important for the coastal Arctic locations, they do not accurately simulate ozone there.
Bastiaan van Diedenhoven, Otto P. Hasekamp, Brian Cairns, Gregory L. Schuster, Snorre Stamnes, Michael Shook, and Luke Ziemba
Atmos. Meas. Tech., 15, 7411–7434, https://doi.org/10.5194/amt-15-7411-2022, https://doi.org/10.5194/amt-15-7411-2022, 2022
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The strong variability in the chemistry of atmospheric particulate matter affects the amount of water aerosols absorb and their effect on climate. We present a remote sensing method to determine the amount of water in particulate matter. Its application to airborne instruments indicates that the observed aerosols have rather low water contents and low fractions of soluble particles. Future satellites will be able to yield global aerosol water uptake data.
Leighton A. Regayre, Lucia Deaconu, Daniel P. Grosvenor, David Sexton, Christopher C. Symonds, Tom Langton, Duncan Watson-Paris, Jane P. Mulcahy, Kirsty J. Pringle, Mark Richardson, Jill S. Johnson, John Rostron, Hamish Gordon, Grenville Lister, Philip Stier, and Ken S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2022-1330, https://doi.org/10.5194/egusphere-2022-1330, 2022
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We show that potential structural deficiencies in a climate model can be exposed by comprehensively exploring its parametric uncertainty, and that these deficiencies limit how much the model uncertainty can be reduced through observational constraint. Combined consideration of parametric and structural uncertainties provides a future pathway towards building models that have greater physical realism and lower uncertainty.
Alba Lorente, Tobias Borsdorff, Mari C. Martinez-Velarte, Andre Butz, Otto P. Hasekamp, Lianghai Wu, and Jochen Landgraf
Atmos. Meas. Tech., 15, 6585–6603, https://doi.org/10.5194/amt-15-6585-2022, https://doi.org/10.5194/amt-15-6585-2022, 2022
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The TROPOspheric Monitoring Instrument (TROPOMI) performs observations over ocean in every orbit, enhancing the monitoring capabilities of methane from space. In the sun glint geometry the mirror-like reflection at the water surface provides a signal that is high enough to retrieve methane with high accuracy and precision. We present 4 years of methane concentrations over the ocean, and we assess its quality. We also show the importance of ocean observations to quantify total CH4 emissions.
Johannes Quaas, Hailing Jia, Chris Smith, Anna Lea Albright, Wenche Aas, Nicolas Bellouin, Olivier Boucher, Marie Doutriaux-Boucher, Piers M. Forster, Daniel Grosvenor, Stuart Jenkins, Zbigniew Klimont, Norman G. Loeb, Xiaoyan Ma, Vaishali Naik, Fabien Paulot, Philip Stier, Martin Wild, Gunnar Myhre, and Michael Schulz
Atmos. Chem. Phys., 22, 12221–12239, https://doi.org/10.5194/acp-22-12221-2022, https://doi.org/10.5194/acp-22-12221-2022, 2022
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Pollution particles cool climate and offset part of the global warming. However, they are washed out by rain and thus their effect responds quickly to changes in emissions. We show multiple datasets to demonstrate that aerosol emissions and their concentrations declined in many regions influenced by human emissions, as did the effects on clouds. Consequently, the cooling impact on the Earth energy budget became smaller. This change in trend implies a relative warming.
Colin Tully, David Neubauer, Nadja Omanovic, and Ulrike Lohmann
Atmos. Chem. Phys., 22, 11455–11484, https://doi.org/10.5194/acp-22-11455-2022, https://doi.org/10.5194/acp-22-11455-2022, 2022
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The proposed geoengineering method, cirrus cloud thinning, was evaluated using a more physically based microphysics scheme coupled to a more realistic approach for calculating ice cloud fractions in the ECHAM-HAM GCM. Sensitivity tests reveal that using the new ice cloud fraction approach and increasing the critical ice saturation ratio for ice nucleation on seeding particles reduces warming from overseeding. However, this geoengineering method is unlikely to be feasible on a global scale.
Qirui Zhong, Nick Schutgens, Guido van der Werf, Twan van Noije, Kostas Tsigaridis, Susanne E. Bauer, Tero Mielonen, Alf Kirkevåg, Øyvind Seland, Harri Kokkola, Ramiro Checa-Garcia, David Neubauer, Zak Kipling, Hitoshi Matsui, Paul Ginoux, Toshihiko Takemura, Philippe Le Sager, Samuel Rémy, Huisheng Bian, Mian Chin, Kai Zhang, Jialei Zhu, Svetlana G. Tsyro, Gabriele Curci, Anna Protonotariou, Ben Johnson, Joyce E. Penner, Nicolas Bellouin, Ragnhild B. Skeie, and Gunnar Myhre
Atmos. Chem. Phys., 22, 11009–11032, https://doi.org/10.5194/acp-22-11009-2022, https://doi.org/10.5194/acp-22-11009-2022, 2022
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Aerosol optical depth (AOD) errors for biomass burning aerosol (BBA) are evaluated in 18 global models against satellite datasets. Notwithstanding biases in satellite products, they allow model evaluations. We observe large and diverse model biases due to errors in BBA. Further interpretations of AOD diversities suggest large biases exist in key processes for BBA which require better constraining. These results can contribute to further model improvement and development.
Amy H. Peace, Ben B. B. Booth, Leighton A. Regayre, Ken S. Carslaw, David M. H. Sexton, Céline J. W. Bonfils, and John W. Rostron
Earth Syst. Dynam., 13, 1215–1232, https://doi.org/10.5194/esd-13-1215-2022, https://doi.org/10.5194/esd-13-1215-2022, 2022
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Anthropogenic aerosol emissions have been linked to driving climate responses such as shifts in the location of tropical rainfall. However, the interaction of aerosols with climate remains one of the most uncertain aspects of climate modelling and limits our ability to predict future climate change. We use an ensemble of climate model simulations to investigate what impact the large uncertainty in how aerosols interact with climate has on predicting future tropical rainfall shifts.
Matthieu Dogniaux, Cyril Crevoisier, Silvère Gousset, Étienne Le Coarer, Yann Ferrec, Laurence Croizé, Lianghai Wu, Otto Hasekamp, Bojan Sic, and Laure Brooker
Atmos. Meas. Tech., 15, 4835–4858, https://doi.org/10.5194/amt-15-4835-2022, https://doi.org/10.5194/amt-15-4835-2022, 2022
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The Space Carbon Observatory (SCARBO) concept proposes a constellation of small satellites that would carry a miniaturized Fabry–Pérot imaging interferometer named NanoCarb and an aerosol instrument named SPEXone. In this work, we assess the performance of this concept for the retrieval of the total weighted columns of CO2 and CH4 and show the interest of adding the SPEXone aerosol instrument to improve the CO2 and CH4 column retrieval.
Haochi Che, Philip Stier, Duncan Watson-Parris, Hamish Gordon, and Lucia Deaconu
Atmos. Chem. Phys., 22, 10789–10807, https://doi.org/10.5194/acp-22-10789-2022, https://doi.org/10.5194/acp-22-10789-2022, 2022
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Extensive stratocumulus clouds over the south-eastern Atlantic (SEA) can lead to a cooling effect on the climate. A key pathway by which aerosols affect cloud properties is by acting as cloud condensation nuclei (CCN). Here, we investigated the source attribution of CCN in the SEA as well as the cloud responses. Our results show that aerosol nucleation contributes most to CCN in the marine boundary layer. In terms of emissions, anthropogenic sources contribute most to the CCN and cloud droplets.
Meng Gao, Kirk Knobelspiesse, Bryan A. Franz, Peng-Wang Zhai, Andrew M. Sayer, Amir Ibrahim, Brian Cairns, Otto Hasekamp, Yongxiang Hu, Vanderlei Martins, P. Jeremy Werdell, and Xiaoguang Xu
Atmos. Meas. Tech., 15, 4859–4879, https://doi.org/10.5194/amt-15-4859-2022, https://doi.org/10.5194/amt-15-4859-2022, 2022
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In this work, we assessed the pixel-wise retrieval uncertainties on aerosol and ocean color derived from multi-angle polarimetric measurements. Standard error propagation methods are used to compute the uncertainties. A flexible framework is proposed to evaluate how representative these uncertainties are compared with real retrieval errors. Meanwhile, to assist operational data processing, we optimized the computational speed to evaluate the retrieval uncertainties based on neural networks.
Bernd Heinold, Holger Baars, Boris Barja, Matthew Christensen, Anne Kubin, Kevin Ohneiser, Kerstin Schepanski, Nick Schutgens, Fabian Senf, Roland Schrödner, Diego Villanueva, and Ina Tegen
Atmos. Chem. Phys., 22, 9969–9985, https://doi.org/10.5194/acp-22-9969-2022, https://doi.org/10.5194/acp-22-9969-2022, 2022
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The extreme 2019–2020 Australian wildfires produced massive smoke plumes lofted into the lower stratosphere by pyrocumulonimbus convection. Most climate models do not adequately simulate the injection height of such intense fires. By combining aerosol-climate modeling with prescribed pyroconvective smoke injection and lidar observations, this study shows the importance of the representation of the most extreme wildfire events for estimating the atmospheric energy budget.
Roland Vernooij, Patrik Winiger, Martin Wooster, Tercia Strydom, Laurent Poulain, Ulrike Dusek, Mark Grosvenor, Gareth J. Roberts, Nick Schutgens, and Guido R. van der Werf
Atmos. Meas. Tech., 15, 4271–4294, https://doi.org/10.5194/amt-15-4271-2022, https://doi.org/10.5194/amt-15-4271-2022, 2022
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Landscape fires are a substantial emitter of greenhouse gases and aerosols. Previous studies have indicated savanna emission factors to be highly variable. Improving fire emission estimates, and understanding future climate- and human-induced changes in fire regimes, requires in situ measurements. We present a drone-based method that enables the collection of a large amount of high-quality emission factor measurements that do not have the biases of aircraft or surface measurements.
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.
Dongwei Fu, Larry Di Girolamo, Robert M. Rauber, Greg M. McFarquhar, Stephen W. Nesbitt, Jesse Loveridge, Yulan Hong, Bastiaan van Diedenhoven, Brian Cairns, Mikhail D. Alexandrov, Paul Lawson, Sarah Woods, Simone Tanelli, Sebastian Schmidt, Chris Hostetler, and Amy Jo Scarino
Atmos. Chem. Phys., 22, 8259–8285, https://doi.org/10.5194/acp-22-8259-2022, https://doi.org/10.5194/acp-22-8259-2022, 2022
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Satellite-retrieved cloud microphysics are widely used in climate research because of their central role in water and energy cycles. Here, we provide the first detailed investigation of retrieved cloud drop sizes from in situ and various satellite and airborne remote sensing techniques applied to real cumulus cloud fields. We conclude that the most widely used passive remote sensing method employed in climate research produces high biases of 6–8 µm (60 %–80 %) caused by 3-D radiative effects.
Enza Di Tomaso, Jerónimo Escribano, Sara Basart, Paul Ginoux, Francesca Macchia, Francesca Barnaba, Francesco Benincasa, Pierre-Antoine Bretonnière, Arnau Buñuel, Miguel Castrillo, Emilio Cuevas, Paola Formenti, María Gonçalves, Oriol Jorba, Martina Klose, Lucia Mona, Gilbert Montané Pinto, Michail Mytilinaios, Vincenzo Obiso, Miriam Olid, Nick Schutgens, Athanasios Votsis, Ernest Werner, and Carlos Pérez García-Pando
Earth Syst. Sci. Data, 14, 2785–2816, https://doi.org/10.5194/essd-14-2785-2022, https://doi.org/10.5194/essd-14-2785-2022, 2022
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MONARCH reanalysis of desert dust aerosols extends the existing observation-based information for mineral dust monitoring by providing 3-hourly upper-air, surface and total column key geophysical variables of the dust cycle over Northern Africa, the Middle East and Europe, at a 0.1° horizontal resolution in a rotated grid, from 2007 to 2016. This work provides evidence of the high accuracy of this data set and its suitability for air quality and health and climate service applications.
Hailing Jia, Johannes Quaas, Edward Gryspeerdt, Christoph Böhm, and Odran Sourdeval
Atmos. Chem. Phys., 22, 7353–7372, https://doi.org/10.5194/acp-22-7353-2022, https://doi.org/10.5194/acp-22-7353-2022, 2022
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Aerosol–cloud interaction is the most uncertain component of the anthropogenic forcing of the climate. By combining satellite and reanalysis data, we show that the strength of the Twomey effect (S) increases remarkably with vertical velocity. Both the confounding effect of aerosol–precipitation interaction and the lack of vertical co-location between aerosol and cloud are found to overestimate S, whereas the retrieval biases in aerosol and cloud appear to underestimate S.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys., 22, 5775–5828, https://doi.org/10.5194/acp-22-5775-2022, https://doi.org/10.5194/acp-22-5775-2022, 2022
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Air pollutants, like ozone and soot, play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the-art atmospheric models to measured air pollution in order to assess how well the models perform.
Athanasios Tsikerdekis, Nick A. J. Schutgens, Guangliang Fu, and Otto P. Hasekamp
Geosci. Model Dev., 15, 3253–3279, https://doi.org/10.5194/gmd-15-3253-2022, https://doi.org/10.5194/gmd-15-3253-2022, 2022
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In our study we quantify the ability of the future satellite sensor SPEXone, part of the NASA PACE mission, to estimate aerosol emissions. The sensor will be able to retrieve accurate information of aerosol light extinction and most importantly light absorption. We simulate SPEXone spatial coverage and combine it with an aerosol model. We found that SPEXone will be able to estimate species-specific (e.g. dust, sea salt, organic or black carbon, sulfates) aerosol emissions very accurately.
Ulrike Proske, Sylvaine Ferrachat, David Neubauer, Martin Staab, and Ulrike Lohmann
Atmos. Chem. Phys., 22, 4737–4762, https://doi.org/10.5194/acp-22-4737-2022, https://doi.org/10.5194/acp-22-4737-2022, 2022
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Cloud microphysical processes shape cloud properties and are therefore important to represent in climate models. Their parameterization has grown more complex, making the model results more difficult to interpret. Using sensitivity analysis we test how the global aerosol–climate model ECHAM-HAM reacts to changes to these parameterizations. The model is sensitive to the parameterization of ice crystal autoconversion but not to, e.g., self-collection, suggesting that it may be simplified.
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.
Patricia Tarín-Carrasco, Ulas Im, Camilla Geels, Laura Palacios-Peña, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 22, 3945–3965, https://doi.org/10.5194/acp-22-3945-2022, https://doi.org/10.5194/acp-22-3945-2022, 2022
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The evidence of the effects of atmospheric pollution (and particularly fine particulate matter, PM2.5) on human mortality is now unquestionable. Here, 895 000 annual premature deaths (PD) are estimated for the present (1991–2010), which increases to 1 540 000 in the year 2050 due to the ageing of the European population. The implementation of a mitigation scenario (80 % of the energy production in Europe from renewable sources) could lead to a decrease of over 60 000 annual PD for the year 2050.
Meloë S. F. Kacenelenbogen, Qian Tan, Sharon P. Burton, Otto P. Hasekamp, Karl D. Froyd, Yohei Shinozuka, Andreas J. Beyersdorf, Luke Ziemba, Kenneth L. Thornhill, Jack E. Dibb, Taylor Shingler, Armin Sorooshian, Reed W. Espinosa, Vanderlei Martins, Jose L. Jimenez, Pedro Campuzano-Jost, Joshua P. Schwarz, Matthew S. Johnson, Jens Redemann, and Gregory L. Schuster
Atmos. Chem. Phys., 22, 3713–3742, https://doi.org/10.5194/acp-22-3713-2022, https://doi.org/10.5194/acp-22-3713-2022, 2022
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The impact of aerosols on Earth's radiation budget and human health is important and strongly depends on their composition. One desire of our scientific community is to derive the composition of the aerosol from satellite sensors. However, satellites observe aerosol optical properties (and not aerosol composition) based on remote sensing instrumentation. This study assesses how much aerosol optical properties can tell us about aerosol composition.
Matthew S. Norgren, John Wood, K. Sebastian Schmidt, Bastiaan van Diedenhoven, Snorre A. Stamnes, Luke D. Ziemba, Ewan C. Crosbie, Michael A. Shook, A. Scott Kittelman, Samuel E. LeBlanc, Stephen Broccardo, Steffen Freitag, and Jeffrey S. Reid
Atmos. Meas. Tech., 15, 1373–1394, https://doi.org/10.5194/amt-15-1373-2022, https://doi.org/10.5194/amt-15-1373-2022, 2022
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A new spectral instrument (SPN-S), with the ability to partition solar radiation into direct and diffuse components, is used in airborne settings to study the optical properties of aerosols and cirrus. It is a low-cost and mechanically simple system but has higher measurement uncertainty than existing standards. This challenge is overcome by utilizing the unique measurement capabilities to develop new retrieval techniques. Validation is done with data from two NASA airborne research campaigns.
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.
Matthew W. Christensen, Andrew Gettelman, Jan Cermak, Guy Dagan, Michael Diamond, Alyson Douglas, Graham Feingold, Franziska Glassmeier, Tom Goren, Daniel P. Grosvenor, Edward Gryspeerdt, Ralph Kahn, Zhanqing Li, Po-Lun Ma, Florent Malavelle, Isabel L. McCoy, Daniel T. McCoy, Greg McFarquhar, Johannes Mülmenstädt, Sandip Pal, Anna Possner, Adam Povey, Johannes Quaas, Daniel Rosenfeld, Anja Schmidt, Roland Schrödner, Armin Sorooshian, Philip Stier, Velle Toll, Duncan Watson-Parris, Robert Wood, Mingxi Yang, and Tianle Yuan
Atmos. Chem. Phys., 22, 641–674, https://doi.org/10.5194/acp-22-641-2022, https://doi.org/10.5194/acp-22-641-2022, 2022
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Trace gases and aerosols (tiny airborne particles) are released from a variety of point sources around the globe. Examples include volcanoes, industrial chimneys, forest fires, and ship stacks. These sources provide opportunistic experiments with which to quantify the role of aerosols in modifying cloud properties. We review the current state of understanding on the influence of aerosol on climate built from the wide range of natural and anthropogenic laboratories investigated in recent decades.
Duncan Watson-Parris, Andrew Williams, Lucia Deaconu, and Philip Stier
Geosci. Model Dev., 14, 7659–7672, https://doi.org/10.5194/gmd-14-7659-2021, https://doi.org/10.5194/gmd-14-7659-2021, 2021
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The Earth System Emulator (ESEm) provides a fast and flexible framework for emulating a wide variety of Earth science datasets and tools for constraining (or tuning) models of any complexity. Three distinct use cases are presented that demonstrate the utility of ESEm and provide some insight into the use of machine learning for emulation in these different settings. The open-source Python package is freely available so that it might become a valuable tool for the community.
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.
Maria Sand, Bjørn H. Samset, Gunnar Myhre, Jonas Gliß, Susanne E. Bauer, Huisheng Bian, Mian Chin, Ramiro Checa-Garcia, Paul Ginoux, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Philippe Le Sager, Marianne T. Lund, Hitoshi Matsui, Twan van Noije, Dirk J. L. Olivié, Samuel Remy, Michael Schulz, Philip Stier, Camilla W. Stjern, Toshihiko Takemura, Kostas Tsigaridis, Svetlana G. Tsyro, and Duncan Watson-Parris
Atmos. Chem. Phys., 21, 15929–15947, https://doi.org/10.5194/acp-21-15929-2021, https://doi.org/10.5194/acp-21-15929-2021, 2021
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Absorption of shortwave radiation by aerosols can modify precipitation and clouds but is poorly constrained in models. A total of 15 different aerosol models from AeroCom phase III have reported total aerosol absorption, and for the first time, 11 of these models have reported in a consistent experiment the contributions to absorption from black carbon, dust, and organic aerosol. Here, we document the model diversity in aerosol absorption.
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.
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.
Paolo Pelucchi, David Neubauer, and Ulrike Lohmann
Geosci. Model Dev., 14, 5413–5434, https://doi.org/10.5194/gmd-14-5413-2021, https://doi.org/10.5194/gmd-14-5413-2021, 2021
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Stratocumulus are thin clouds whose cloud cover is underestimated in climate models partly due to overly low vertical resolution. We develop a scheme that locally refines the vertical grid based on a physical constraint for the cloud top. Global simulations show that the scheme, implemented only in the radiation routine, can increase stratocumulus cloud cover. However, this effect is poorly propagated to the simulated cloud cover. The scheme's limitations and possible ways forward are discussed.
Camilla Geels, Morten Winther, Camilla Andersson, Jukka-Pekka Jalkanen, Jørgen Brandt, Lise M. Frohn, Ulas Im, Wing Leung, and Jesper H. Christensen
Atmos. Chem. Phys., 21, 12495–12519, https://doi.org/10.5194/acp-21-12495-2021, https://doi.org/10.5194/acp-21-12495-2021, 2021
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In this study, we set up new shipping emissions scenarios and use two chemistry transport models and a health assessment model to assess the development of air quality and related health impacts in the Nordic region. Shipping alone is associated with about 850 premature deaths during present-day conditions, decreasing to approximately 550–600 cases in the 2050 scenarios.
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.
Ulas Im, Kostas Tsigaridis, Gregory Faluvegi, Peter L. Langen, Joshua P. French, Rashed Mahmood, Manu A. Thomas, Knut von Salzen, Daniel C. Thomas, Cynthia H. Whaley, Zbigniew Klimont, Henrik Skov, and Jørgen Brandt
Atmos. Chem. Phys., 21, 10413–10438, https://doi.org/10.5194/acp-21-10413-2021, https://doi.org/10.5194/acp-21-10413-2021, 2021
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Future (2015–2050) simulations of the aerosol burdens and their radiative forcing and climate impacts over the Arctic under various emission projections show that although the Arctic aerosol burdens are projected to decrease significantly by 10 to 60 %, regardless of the magnitude of aerosol reductions, surface air temperatures will continue to increase by 1.9–2.6 ℃, while sea-ice extent will continue to decrease, implying reductions of greenhouse gases are necessary to mitigate climate change.
Shipeng Zhang, Philip Stier, and Duncan Watson-Parris
Atmos. Chem. Phys., 21, 10179–10197, https://doi.org/10.5194/acp-21-10179-2021, https://doi.org/10.5194/acp-21-10179-2021, 2021
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The relationship between aerosol-induced changes in atmospheric energetics and precipitation responses across different scales is studied in terms of fast (radiatively or microphysically mediated) and slow (temperature-mediated) responses. We introduced a method to decompose rainfall changes into contributions from clouds, aerosols, and clear–clean sky from an energetic perspective. It provides a way to better interpret and quantify the precipitation changes caused by aerosol perturbations.
William G. K. McLean, Guangliang Fu, Sharon P. Burton, and Otto P. Hasekamp
Atmos. Meas. Tech., 14, 4755–4771, https://doi.org/10.5194/amt-14-4755-2021, https://doi.org/10.5194/amt-14-4755-2021, 2021
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In this study, we present results from aerosol retrievals using both synthetic and real lidar datasets, including measurements from the ACEPOL (Aerosol Characterization from Polarimeter and Lidar) campaign, a combined initiative between NASA and SRON (the Netherlands Institute for Space Research). Aerosol microphysical retrievals were performed using the High Spectral Resolution Lidar-2 (HSRL-2) setup, alongside several others, with the ACEPOL retrievals also compared to polarimeter retrievals.
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.
Meng Gao, Bryan A. Franz, Kirk Knobelspiesse, Peng-Wang Zhai, Vanderlei Martins, Sharon Burton, Brian Cairns, Richard Ferrare, Joel Gales, Otto Hasekamp, Yongxiang Hu, Amir Ibrahim, Brent McBride, Anin Puthukkudy, P. Jeremy Werdell, and Xiaoguang Xu
Atmos. Meas. Tech., 14, 4083–4110, https://doi.org/10.5194/amt-14-4083-2021, https://doi.org/10.5194/amt-14-4083-2021, 2021
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Multi-angle polarimetric measurements can retrieve accurate aerosol properties over complex atmosphere and ocean systems; however, most retrieval algorithms require high computational costs. We propose a deep neural network (NN) forward model to represent the radiative transfer simulation of coupled atmosphere and ocean systems and then conduct simultaneous aerosol and ocean color retrievals on AirHARP measurements. The computational acceleration is 103 times with CPU or 104 times with GPU.
Nick Schutgens, Oleg Dubovik, Otto Hasekamp, Omar Torres, Hiren Jethva, Peter J. T. Leonard, Pavel Litvinov, Jens Redemann, Yohei Shinozuka, Gerrit de Leeuw, Stefan Kinne, Thomas Popp, Michael Schulz, and Philip Stier
Atmos. Chem. Phys., 21, 6895–6917, https://doi.org/10.5194/acp-21-6895-2021, https://doi.org/10.5194/acp-21-6895-2021, 2021
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Absorptive aerosol has a potentially large impact on climate change. We evaluate and intercompare four global satellite datasets of absorptive aerosol optical depth (AAOD) and single-scattering albedo (SSA). We show that these datasets show reasonable correlations with the AErosol RObotic NETwork (AERONET) reference, although significant biases remain. In a follow-up paper we show that these observations nevertheless can be used for model evaluation.
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.
Andrew M. Dzambo, Tristan L'Ecuyer, Kenneth Sinclair, Bastiaan van Diedenhoven, Siddhant Gupta, Greg McFarquhar, Joseph R. O'Brien, Brian Cairns, Andrzej P. Wasilewski, and Mikhail Alexandrov
Atmos. Chem. Phys., 21, 5513–5532, https://doi.org/10.5194/acp-21-5513-2021, https://doi.org/10.5194/acp-21-5513-2021, 2021
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This work highlights a new algorithm using data collected from the 2016–2018 NASA ORACLES field campaign. This algorithm synthesizes cloud and rain measurements to attain estimates of cloud and precipitation properties over the southeast Atlantic Ocean. Estimates produced by this algorithm compare well against in situ estimates. Increased rain fractions and rain rates are found in regions of atmospheric instability. This dataset can be used to explore aerosol–cloud–precipitation interactions.
Ulrike Proske, Verena Bessenbacher, Zane Dedekind, Ulrike Lohmann, and David Neubauer
Atmos. Chem. Phys., 21, 5195–5216, https://doi.org/10.5194/acp-21-5195-2021, https://doi.org/10.5194/acp-21-5195-2021, 2021
Short summary
Short summary
Ice crystals falling out of one cloud can initiate freezing in a second cloud below. We estimate the occurrence frequency of this natural cloud seeding over Switzerland from satellite data and sublimation calculations. We find that such situations with an ice cloud above another cloud are frequent and that the falling crystals survive the fall between two clouds in a significant number of cases, suggesting that natural cloud seeding is an important phenomenon over Switzerland.
Cited articles
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Short summary
Aerosols (small airborne particles) impact Earth's climate, but their extent is unknown. By running climate model simulations and using machine learning to emulate millions of additional variants with different settings, we found that natural emissions like sea spray and sulfur are key sources of uncertainty in climate predictions. Our work shows that understanding these natural processes better can help improve climate models and make future climate projections more accurate.
Aerosols (small airborne particles) impact Earth's climate, but their extent is unknown. By...
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