Articles | Volume 23, issue 7
https://doi.org/10.5194/acp-23-4431-2023
© Author(s) 2023. 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-23-4431-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
14 Apr 2023
Research article |
| 14 Apr 2023
| 14 Apr 2023
Contribution of regional aerosol nucleation to low-level CCN in an Amazonian deep convective environment: results from a regionally nested global model
Xuemei Wang
School of Earth and Environment, University of Leeds, LS2 9JT, Leeds, UK
Hamish Gordon
Department of Chemical Engineering and Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA
Daniel P. Grosvenor
School of Earth and Environment, University of Leeds, LS2 9JT, Leeds, UK
Meinrat O. Andreae
Biogeochemistry, Multiphase Chemistry, and Particle Chemistry Departments, Max Planck Institute for Chemistry, Mainz, Germany
School of Earth and Environment, University of Leeds, LS2 9JT, Leeds, UK
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Organic aerosols (OAs), their sources and their processes remain poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem, can be a useful tool to describe primary OA (POA) production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and to estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations made at Delhi, India, in 2018.
Ruth Price, Andrea Baccarini, Julia Schmale, Paul Zieger, Ian M. Brooks, Paul Field, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 2927–2961, https://doi.org/10.5194/acp-23-2927-2023, https://doi.org/10.5194/acp-23-2927-2023, 2023
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Arctic clouds can control how much energy is absorbed by the surface or reflected back to space. Using a computer model of the atmosphere we investigated the formation of atmospheric particles that allow cloud droplets to form. We found that particles formed aloft are transported to the lowest part of the Arctic atmosphere and that this is a key source of particles. Our results have implications for the way Arctic clouds will behave in the future as climate change continues to impact the region.
Haley M. Royer, Mira L. Pöhlker, Ovid Krüger, Edmund Blades, Peter Sealy, Nurun Nahar Lata, Zezhen Cheng, Swarup China, Andrew P. Ault, Patricia K. Quinn, Paquita Zuidema, Christopher Pöhlker, Ulrich Pöschl, Meinrat Andreae, and Cassandra J. Gaston
Atmos. Chem. Phys., 23, 981–998, https://doi.org/10.5194/acp-23-981-2023, https://doi.org/10.5194/acp-23-981-2023, 2023
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This paper presents atmospheric particle chemical composition and measurements of aerosol water uptake properties collected at Ragged Point, Barbados, during the winter of 2020. The result of this study indicates the importance of small African smoke particles for cloud droplet formation in the tropical North Atlantic and highlights the large spatial and temporal pervasiveness of smoke over the Atlantic Ocean.
Yunfan Liu, Hang Su, Siwen Wang, Chao Wei, Wei Tao, Mira L. Pöhlker, Christopher Pöhlker, Bruna A. Holanda, Ovid O. Krüger, Thorsten Hoffmann, Manfred Wendisch, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Yafang Cheng
Atmos. Chem. Phys., 23, 251–272, https://doi.org/10.5194/acp-23-251-2023, https://doi.org/10.5194/acp-23-251-2023, 2023
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The origins of the abundant cloud condensation nuclei (CCN) in the upper troposphere (UT) of the Amazon remain unclear. With model developments of new secondary organic aerosol schemes and constrained by observation, we show that strong aerosol nucleation and condensation in the UT is triggered by biogenic organics, and organic condensation is key for UT CCN production. This UT CCN-producing mechanism may prevail over broader vegetation canopies and deserves emphasis in aerosol–climate feedback.
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.
Ville Leinonen, Harri Kokkola, Taina Yli-Juuti, Tero Mielonen, Thomas Kühn, Tuomo Nieminen, Simo Heikkinen, Tuuli Miinalainen, Tommi Bergman, Ken Carslaw, Stefano Decesari, Markus Fiebig, Tareq Hussein, Niku Kivekäs, Radovan Krejci, Markku Kulmala, Ari Leskinen, Andreas Massling, Nikos Mihalopoulos, Jane P. Mulcahy, Steffen M. Noe, Twan van Noije, Fiona M. O'Connor, Colin O'Dowd, Dirk Olivie, Jakob B. Pernov, Tuukka Petäjä, Øyvind Seland, Michael Schulz, Catherine E. Scott, Henrik Skov, Erik Swietlicki, Thomas Tuch, Alfred Wiedensohler, Annele Virtanen, and Santtu Mikkonen
Atmos. Chem. Phys., 22, 12873–12905, https://doi.org/10.5194/acp-22-12873-2022, https://doi.org/10.5194/acp-22-12873-2022, 2022
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We provide the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five different earth system models. We investigated aerosol modes (nucleation, Aitken, and accumulation) separately and were able to show the differences between measured and modeled trends and especially their seasonal patterns. The differences in model results are likely due to complex effects of several processes instead of certain specific model features.
Charlotte M. Beall, Thomas C. J. Hill, Paul J. DeMott, Tobias Köneman, Michael Pikridas, Frank Drewnick, Hartwig Harder, Christopher Pöhlker, Jos Lelieveld, Bettina Weber, Minas Iakovides, Roman Prokeš, Jean Sciare, Meinrat O. Andreae, M. Dale Stokes, and Kimberly A. Prather
Atmos. Chem. Phys., 22, 12607–12627, https://doi.org/10.5194/acp-22-12607-2022, https://doi.org/10.5194/acp-22-12607-2022, 2022
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Ice-nucleating particles (INPs) are rare aerosols that can trigger ice formation in clouds and affect climate-relevant cloud properties such as phase, reflectivity and lifetime. Dust is the dominant INP source, yet few measurements have been reported near major dust sources. We report INP observations within hundreds of kilometers of the biggest dust source regions globally: the Sahara and the Arabian Peninsula. Results show that at temperatures > −15 °C, INPs are dominated by organics.
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.
Michael S. Diamond, Pablo E. Saide, Paquita Zuidema, Andrew S. Ackerman, Sarah J. Doherty, Ann M. Fridlind, Hamish Gordon, Calvin Howes, Jan Kazil, Takanobu Yamaguchi, Jianhao Zhang, Graham Feingold, and Robert Wood
Atmos. Chem. Phys., 22, 12113–12151, https://doi.org/10.5194/acp-22-12113-2022, https://doi.org/10.5194/acp-22-12113-2022, 2022
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Smoke from southern Africa blankets the southeast Atlantic from June-October, overlying a major transition region between overcast and scattered clouds. The smoke affects Earth's radiation budget by absorbing sunlight and changing cloud properties. We investigate these effects in regional climate and large eddy simulation models based on international field campaigns. We find that large-scale circulation changes more strongly affect cloud transitions than smoke microphysical effects in our case.
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.
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.
Alexander D. Harrison, Daniel O'Sullivan, Michael P. Adams, Grace C. E. Porter, Edmund Blades, Cherise Brathwaite, Rebecca Chewitt-Lucas, Cassandra Gaston, Rachel Hawker, Ovid O. Krüger, Leslie Neve, Mira L. Pöhlker, Christopher Pöhlker, Ulrich Pöschl, Alberto Sanchez-Marroquin, Andrea Sealy, Peter Sealy, Mark D. Tarn, Shanice Whitehall, James B. McQuaid, Kenneth S. Carslaw, Joseph M. Prospero, and Benjamin J. Murray
Atmos. Chem. Phys., 22, 9663–9680, https://doi.org/10.5194/acp-22-9663-2022, https://doi.org/10.5194/acp-22-9663-2022, 2022
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The formation of ice in clouds fundamentally alters cloud properties; hence it is important we understand the special aerosol particles that can nucleate ice when immersed in supercooled cloud droplets. In this paper we show that African desert dust that has travelled across the Atlantic to the Caribbean nucleates ice much less well than we might have expected.
Hanna K. Lappalainen, Tuukka Petäjä, Timo Vihma, Jouni Räisänen, Alexander Baklanov, Sergey Chalov, Igor Esau, Ekaterina Ezhova, Matti Leppäranta, Dmitry Pozdnyakov, Jukka Pumpanen, Meinrat O. Andreae, Mikhail Arshinov, Eija Asmi, Jianhui Bai, Igor Bashmachnikov, Boris Belan, Federico Bianchi, Boris Biskaborn, Michael Boy, Jaana Bäck, Bin Cheng, Natalia Chubarova, Jonathan Duplissy, Egor Dyukarev, Konstantinos Eleftheriadis, Martin Forsius, Martin Heimann, Sirkku Juhola, Vladimir Konovalov, Igor Konovalov, Pavel Konstantinov, Kajar Köster, Elena Lapshina, Anna Lintunen, Alexander Mahura, Risto Makkonen, Svetlana Malkhazova, Ivan Mammarella, Stefano Mammola, Stephany Buenrostro Mazon, Outi Meinander, Eugene Mikhailov, Victoria Miles, Stanislav Myslenkov, Dmitry Orlov, Jean-Daniel Paris, Roberta Pirazzini, Olga Popovicheva, Jouni Pulliainen, Kimmo Rautiainen, Torsten Sachs, Vladimir Shevchenko, Andrey Skorokhod, Andreas Stohl, Elli Suhonen, Erik S. Thomson, Marina Tsidilina, Veli-Pekka Tynkkynen, Petteri Uotila, Aki Virkkula, Nadezhda Voropay, Tobias Wolf, Sayaka Yasunaka, Jiahua Zhang, Yubao Qiu, Aijun Ding, Huadong Guo, Valery Bondur, Nikolay Kasimov, Sergej Zilitinkevich, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 22, 4413–4469, https://doi.org/10.5194/acp-22-4413-2022, https://doi.org/10.5194/acp-22-4413-2022, 2022
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We summarize results during the last 5 years in the northern Eurasian region, especially from Russia, and introduce recent observations of the air quality in the urban environments in China. Although the scientific knowledge in these regions has increased, there are still gaps in our understanding of large-scale climate–Earth surface interactions and feedbacks. This arises from limitations in research infrastructures and integrative data analyses, hindering a comprehensive system analysis.
Marco A. Franco, Florian Ditas, Leslie A. Kremper, Luiz A. T. Machado, Meinrat O. Andreae, Alessandro Araújo, Henrique M. J. Barbosa, Joel F. de Brito, Samara Carbone, Bruna A. Holanda, Fernando G. Morais, Janaína P. Nascimento, Mira L. Pöhlker, Luciana V. Rizzo, Marta Sá, Jorge Saturno, David Walter, Stefan Wolff, Ulrich Pöschl, Paulo Artaxo, and Christopher Pöhlker
Atmos. Chem. Phys., 22, 3469–3492, https://doi.org/10.5194/acp-22-3469-2022, https://doi.org/10.5194/acp-22-3469-2022, 2022
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In Central Amazonia, new particle formation in the planetary boundary layer is rare. Instead, there is the appearance of sub-50 nm aerosols with diameters larger than about 20 nm that eventually grow to cloud condensation nuclei size range. Here, 254 growth events were characterized which have higher predominance in the wet season. About 70 % of them showed direct relation to convective downdrafts, while 30 % occurred partly under clear-sky conditions, evidencing still unknown particle sources.
Meinrat O. Andreae, Tracey W. Andreae, Florian Ditas, and Christopher Pöhlker
Atmos. Chem. Phys., 22, 2487–2505, https://doi.org/10.5194/acp-22-2487-2022, https://doi.org/10.5194/acp-22-2487-2022, 2022
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Atmospheric aerosol particles are key players in the Earth’s climate system, but there is still considerable uncertainty about where and how these particles are initially formed. We present the first study of new particle formation (NPF) at a pristine site in a subboreal forest region of North America. Our data suggest that, in this environment, there is frequent NPF from biogenic organic precursor compounds, which was likely the predominant source of particles in the preindustrial environment.
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.
Sarah J. Doherty, Pablo E. Saide, Paquita Zuidema, Yohei Shinozuka, Gonzalo A. Ferrada, Hamish Gordon, Marc Mallet, Kerry Meyer, David Painemal, Steven G. Howell, Steffen Freitag, Amie Dobracki, James R. Podolske, Sharon P. Burton, Richard A. Ferrare, Calvin Howes, Pierre Nabat, Gregory R. Carmichael, Arlindo da Silva, Kristina Pistone, Ian Chang, Lan Gao, Robert Wood, and Jens Redemann
Atmos. Chem. Phys., 22, 1–46, https://doi.org/10.5194/acp-22-1-2022, https://doi.org/10.5194/acp-22-1-2022, 2022
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Between July and October, biomass burning smoke is advected over the southeastern Atlantic Ocean, leading to climate forcing. Model calculations of forcing by this plume vary significantly in both magnitude and sign. This paper compares aerosol and cloud properties observed during three NASA ORACLES field campaigns to the same in four models. It quantifies modeled biases in properties key to aerosol direct radiative forcing and evaluates how these biases propagate to biases in forcing.
Luiz A. T. Machado, Marco A. Franco, Leslie A. Kremper, Florian Ditas, Meinrat O. Andreae, Paulo Artaxo, Micael A. Cecchini, Bruna A. Holanda, Mira L. Pöhlker, Ivan Saraiva, Stefan Wolff, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Chem. Phys., 21, 18065–18086, https://doi.org/10.5194/acp-21-18065-2021, https://doi.org/10.5194/acp-21-18065-2021, 2021
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Several studies evaluate aerosol–cloud interactions, but only a few attempted to describe how clouds modify aerosol properties. This study evaluates the effect of weather events on the particle size distribution at the ATTO, combining remote sensing and in situ data. Ultrafine, Aitken and accumulation particles modes have different behaviors for the diurnal cycle and for rainfall events. This study opens up new scientific questions that need to be pursued in detail in new field campaigns.
Ramon Campos Braga, Barbara Ervens, Daniel Rosenfeld, Meinrat O. Andreae, Jan-David Förster, Daniel Fütterer, Lianet Hernández Pardo, Bruna A. Holanda, Tina Jurkat-Witschas, Ovid O. Krüger, Oliver Lauer, Luiz A. T. Machado, Christopher Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Manfred Wendisch, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 17513–17528, https://doi.org/10.5194/acp-21-17513-2021, https://doi.org/10.5194/acp-21-17513-2021, 2021
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Interactions of aerosol particles with clouds represent a large uncertainty in estimates of climate change. Properties of aerosol particles control their ability to act as cloud condensation nuclei. Using aerosol measurements in the Amazon, we performed model studies to compare predicted and measured cloud droplet number concentrations at cloud bases. Our results confirm previous estimates of particle hygroscopicity in this region.
Rachel E. Hawker, Annette K. Miltenberger, Jill S. Johnson, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Paul R. Field, Benjamin J. Murray, and Ken S. Carslaw
Atmos. Chem. Phys., 21, 17315–17343, https://doi.org/10.5194/acp-21-17315-2021, https://doi.org/10.5194/acp-21-17315-2021, 2021
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We find that ice-nucleating particles (INPs), aerosols that can initiate the freezing of cloud droplets, cause substantial changes to the properties of radiatively important convectively generated anvil cirrus. The number concentration of INPs had a large effect on ice crystal number concentration while the INP temperature dependence controlled ice crystal size and cloud fraction. The results indicate information on INP number and source is necessary for the representation of cloud glaciation.
Igor B. Konovalov, Nikolai A. Golovushkin, Matthias Beekmann, Mikhail V. Panchenko, and Meinrat O. Andreae
Atmos. Meas. Tech., 14, 6647–6673, https://doi.org/10.5194/amt-14-6647-2021, https://doi.org/10.5194/amt-14-6647-2021, 2021
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The absorption of solar light by organic matter, known as brown carbon (BrC), contributes significantly to the radiative budget of the Earth’s atmosphere, but its representation in atmospheric models is uncertain. This paper advances a methodology to constrain model parameters characterizing BrC absorption of atmospheric aerosol originating from biomass burning with the available remote ground-based observations of atmospheric aerosol.
Heather Guy, Ian M. Brooks, Ken S. Carslaw, Benjamin J. Murray, Von P. Walden, Matthew D. Shupe, Claire Pettersen, David D. Turner, Christopher J. Cox, William D. Neff, Ralf Bennartz, and Ryan R. Neely III
Atmos. Chem. Phys., 21, 15351–15374, https://doi.org/10.5194/acp-21-15351-2021, https://doi.org/10.5194/acp-21-15351-2021, 2021
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We present the first full year of surface aerosol number concentration measurements from the central Greenland Ice Sheet. Aerosol concentrations here have a distinct seasonal cycle from those at lower-altitude Arctic sites, which is driven by large-scale atmospheric circulation. Our results can be used to help understand the role aerosols might play in Greenland surface melt through the modification of cloud properties. This is crucial in a rapidly changing region where observations are sparse.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Ramon Campos Braga, Daniel Rosenfeld, Ovid O. Krüger, Barbara Ervens, Bruna A. Holanda, Manfred Wendisch, Trismono Krisna, Ulrich Pöschl, Meinrat O. Andreae, Christiane Voigt, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 14079–14088, https://doi.org/10.5194/acp-21-14079-2021, https://doi.org/10.5194/acp-21-14079-2021, 2021
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Quantifying the precipitation within clouds is crucial for our understanding of the Earth's hydrological cycle. Using in situ measurements of cloud and rain properties over the Amazon Basin and Atlantic Ocean, we show here a linear relationship between the effective radius (re) and precipitation water content near the tops of convective clouds for different pollution states and temperature levels. Our results emphasize the role of re to determine both initiation and amount of precipitation.
Maria Prass, Meinrat O. Andreae, Alessandro C. de Araùjo, Paulo Artaxo, Florian Ditas, Wolfgang Elbert, Jan-David Förster, Marco Aurélio Franco, Isabella Hrabe de Angelis, Jürgen Kesselmeier, Thomas Klimach, Leslie Ann Kremper, Eckhard Thines, David Walter, Jens Weber, Bettina Weber, Bernhard M. Fuchs, Ulrich Pöschl, and Christopher Pöhlker
Biogeosciences, 18, 4873–4887, https://doi.org/10.5194/bg-18-4873-2021, https://doi.org/10.5194/bg-18-4873-2021, 2021
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Bioaerosols in the atmosphere over the Amazon rain forest were analyzed by molecular biological staining and microscopy. Eukaryotic, bacterial, and archaeal aerosols were quantified in time series and altitude profiles which exhibited clear differences in number concentrations and vertical distributions. Our results provide insights into the sources and dispersion of different Amazonian bioaerosol types as a basis for a better understanding of biosphere–atmosphere interactions.
Ramiro Checa-Garcia, Yves Balkanski, Samuel Albani, Tommi Bergman, Ken Carslaw, Anne Cozic, Chris Dearden, Beatrice Marticorena, Martine Michou, Twan van Noije, Pierre Nabat, Fiona M. O'Connor, Dirk Olivié, Joseph M. Prospero, Philippe Le Sager, Michael Schulz, and Catherine Scott
Atmos. Chem. Phys., 21, 10295–10335, https://doi.org/10.5194/acp-21-10295-2021, https://doi.org/10.5194/acp-21-10295-2021, 2021
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Thousands of tons of dust are emitted into the atmosphere every year, producing important impacts on the Earth system. However, current global climate models are not yet able to reproduce dust emissions, transport and depositions with the desirable accuracy. Our study analyses five different Earth system models to report aspects to be improved to reproduce better available observations, increase the consistency between models and therefore decrease the current uncertainties.
Robbie Ramsay, Chiara F. Di Marco, Mathew R. Heal, Matthias Sörgel, Paulo Artaxo, Meinrat O. Andreae, and Eiko Nemitz
Biogeosciences, 18, 2809–2825, https://doi.org/10.5194/bg-18-2809-2021, https://doi.org/10.5194/bg-18-2809-2021, 2021
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The exchange of the gas ammonia between the atmosphere and the surface is an important biogeochemical process, but little is known of this exchange for certain ecosystems, such as the Amazon rainforest. This study took measurements of ammonia exchange over an Amazon rainforest site and subsequently modelled the observed deposition and emission patterns. We observed emissions of ammonia from the rainforest, which can be simulated accurately by using a canopy resistance modelling approach.
Rachel E. Hawker, Annette K. Miltenberger, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Zhiqiang Cui, Richard J. Cotton, Ken S. Carslaw, Paul R. Field, and Benjamin J. Murray
Atmos. Chem. Phys., 21, 5439–5461, https://doi.org/10.5194/acp-21-5439-2021, https://doi.org/10.5194/acp-21-5439-2021, 2021
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The impact of aerosols on clouds is a large source of uncertainty for future climate projections. Our results show that the radiative properties of a complex convective cloud field in the Saharan outflow region are sensitive to the temperature dependence of ice-nucleating particle concentrations. This means that differences in the aerosol source or composition, for the same aerosol size distribution, can cause differences in the outgoing radiation from regions dominated by tropical convection.
Ananth Ranjithkumar, Hamish Gordon, Christina Williamson, Andrew Rollins, Kirsty Pringle, Agnieszka Kupc, Nathan Luke Abraham, Charles Brock, and Ken Carslaw
Atmos. Chem. Phys., 21, 4979–5014, https://doi.org/10.5194/acp-21-4979-2021, https://doi.org/10.5194/acp-21-4979-2021, 2021
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The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
Kamalika Sengupta, Kirsty Pringle, Jill S. Johnson, Carly Reddington, Jo Browse, Catherine E. Scott, and Ken Carslaw
Atmos. Chem. Phys., 21, 2693–2723, https://doi.org/10.5194/acp-21-2693-2021, https://doi.org/10.5194/acp-21-2693-2021, 2021
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Global models consistently underestimate atmospheric secondary organic aerosol (SOA), which has significant climatic implications. We use a perturbed parameter model ensemble and ground-based observations to reduce the uncertainty in modelling SOA formation from oxidation of volatile organic compounds. We identify plausible parameter spaces for the yields of extremely low-volatility, low-volatility, and semi-volatile organic compounds based on model–observation match for three key model outputs.
Jim M. Haywood, Steven J. Abel, Paul A. Barrett, Nicolas Bellouin, Alan Blyth, Keith N. Bower, Melissa Brooks, Ken Carslaw, Haochi Che, Hugh Coe, Michael I. Cotterell, Ian Crawford, Zhiqiang Cui, Nicholas Davies, Beth Dingley, Paul Field, Paola Formenti, Hamish Gordon, Martin de Graaf, Ross Herbert, Ben Johnson, Anthony C. Jones, Justin M. Langridge, Florent Malavelle, Daniel G. Partridge, Fanny Peers, Jens Redemann, Philip Stier, Kate Szpek, Jonathan W. Taylor, Duncan Watson-Parris, Robert Wood, Huihui Wu, and Paquita Zuidema
Atmos. Chem. Phys., 21, 1049–1084, https://doi.org/10.5194/acp-21-1049-2021, https://doi.org/10.5194/acp-21-1049-2021, 2021
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Every year, the seasonal cycle of biomass burning from agricultural practices in Africa creates a huge plume of smoke that travels many thousands of kilometres over the Atlantic Ocean. This study provides an overview of a measurement campaign called the cloud–aerosol–radiation interaction and forcing for year 2017 (CLARIFY-2017) and documents the rationale, deployment strategy, observations, and key results from the campaign which utilized the heavily equipped FAAM atmospheric research aircraft.
Benjamin J. Murray, Kenneth S. Carslaw, and Paul R. Field
Atmos. Chem. Phys., 21, 665–679, https://doi.org/10.5194/acp-21-665-2021, https://doi.org/10.5194/acp-21-665-2021, 2021
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The balance between the amounts of ice and supercooled water in clouds over the world's oceans strongly influences how much these clouds can dampen or amplify global warming. Aerosol particles which catalyse ice formation can dramatically reduce the amount of supercooled water in clouds; hence we argue that we need a concerted effort to improve our understanding of these ice-nucleating particles if we are to improve our predictions of climate change.
Igor B. Konovalov, Nikolai A. Golovushkin, Matthias Beekmann, and Meinrat O. Andreae
Atmos. Chem. Phys., 21, 357–392, https://doi.org/10.5194/acp-21-357-2021, https://doi.org/10.5194/acp-21-357-2021, 2021
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A lack of consistent observational constraints on the atmospheric evolution of the optical properties of biomass burning (BB) aerosol limits the accuracy of assessments of the aerosol radiative and climate effects. We show that useful insights into the evolution of the BB aerosol optical properties can be inferred from a combination of satellite observations and 3D modeling. We report major changes that occurred in the optical properties of Siberian BB aerosol during its long-range transport.
Haochi Che, Philip Stier, Hamish Gordon, Duncan Watson-Parris, and Lucia Deaconu
Atmos. Chem. Phys., 21, 17–33, https://doi.org/10.5194/acp-21-17-2021, https://doi.org/10.5194/acp-21-17-2021, 2021
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The south-eastern Atlantic is semi-permanently covered by some of the largest stratocumulus clouds and is influenced by one-third of the biomass burning emissions from African fires. A UKEMS1 model simulation shows that the absorption effect of biomass burning aerosols is the most significant on clouds and radiation. The dominate cooling and rapid adjustments induced by the radiative effects of biomass burning aerosols result in an overall cooling in the south-eastern Atlantic.
Robert B. Chatfield, Meinrat O. Andreae, ARCTAS Science Team, and SEAC4RS Science Team
Atmos. Meas. Tech., 13, 7069–7096, https://doi.org/10.5194/amt-13-7069-2020, https://doi.org/10.5194/amt-13-7069-2020, 2020
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Forest burning affects air pollution and global climate. A NASA aircraft studied fire emissions including the Rim Fire near Yosemite. We found frequent confusions between the actual fire emission factors and other effects on the air samples. Effects on CO2 and CO can originate far upwind; the gases can mix variably into a smoke plume. We devised a theory of constant features in plumes. A statistical mixed-effects analysis of a co-emitted tracers model disentangles such mixing from fire effects.
Jane P. Mulcahy, Colin Johnson, Colin G. Jones, Adam C. Povey, Catherine E. Scott, Alistair Sellar, Steven T. Turnock, Matthew T. Woodhouse, Nathan Luke Abraham, Martin B. Andrews, Nicolas Bellouin, Jo Browse, Ken S. Carslaw, Mohit Dalvi, Gerd A. Folberth, Matthew Glover, Daniel P. Grosvenor, Catherine Hardacre, Richard Hill, Ben Johnson, Andy Jones, Zak Kipling, Graham Mann, James Mollard, Fiona M. O'Connor, Julien Palmiéri, Carly Reddington, Steven T. Rumbold, Mark Richardson, Nick A. J. Schutgens, Philip Stier, Marc Stringer, Yongming Tang, Jeremy Walton, Stephanie Woodward, and Andrew Yool
Geosci. Model Dev., 13, 6383–6423, https://doi.org/10.5194/gmd-13-6383-2020, https://doi.org/10.5194/gmd-13-6383-2020, 2020
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Aerosols are an important component of the Earth system. Here, we comprehensively document and evaluate the aerosol schemes as implemented in the physical and Earth system models, HadGEM3-GC3.1 and UKESM1. This study provides a useful characterisation of the aerosol climatology in both models, facilitating the understanding of the numerous aerosol–climate interaction studies that will be conducted for CMIP6 and beyond.
Daniel P. Grosvenor and Kenneth S. Carslaw
Atmos. Chem. Phys., 20, 15681–15724, https://doi.org/10.5194/acp-20-15681-2020, https://doi.org/10.5194/acp-20-15681-2020, 2020
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Particles arising from human activity interact with clouds and affect how much of the Sun's energy is reflected away. Lack of understanding about how to represent this in models leads to large uncertainties in climate predictions. We quantify cloud responses to particles in the latest UK Met Office climate model over the North Atlantic Ocean, showing that, in contrast to suggestions elsewhere, increases in cloud coverage and thickness are important over large areas.
Robbie Ramsay, Chiara F. Di Marco, Matthias Sörgel, Mathew R. Heal, Samara Carbone, Paulo Artaxo, Alessandro C. de Araùjo, Marta Sá, Christopher Pöhlker, Jost Lavric, Meinrat O. Andreae, and Eiko Nemitz
Atmos. Chem. Phys., 20, 15551–15584, https://doi.org/10.5194/acp-20-15551-2020, https://doi.org/10.5194/acp-20-15551-2020, 2020
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The Amazon rainforest is a unique
laboratoryto study the processes which govern the exchange of gases and aerosols to and from the atmosphere. This study investigated these processes by measuring the atmospheric concentrations of trace gases and particles at the Amazon Tall Tower Observatory. We found that the long-range transport of pollutants can affect the atmospheric composition above the Amazon rainforest and that the gases ammonia and nitrous acid can be emitted from the rainforest.
Zhuang Wang, Cheng Liu, Zhouqing Xie, Qihou Hu, Meinrat O. Andreae, Yunsheng Dong, Chun Zhao, Ting Liu, Yizhi Zhu, Haoran Liu, Chengzhi Xing, Wei Tan, Xiangguang Ji, Jinan Lin, and Jianguo Liu
Atmos. Chem. Phys., 20, 14917–14932, https://doi.org/10.5194/acp-20-14917-2020, https://doi.org/10.5194/acp-20-14917-2020, 2020
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Significant stratification of aerosols was observed in North China. Polluted dust dominated above the PBL, and anthropogenic aerosols prevailed within the PBL, which is mainly driven by meteorological conditions. The key role of the elevated dust is to alter atmospheric thermodynamics and stability, causing the suppression of turbulence exchange and a decrease in PBL height, especially during the dissipation stage, thereby inhibiting dissipation of persistent heavy surface haze pollution.
Sandip S. Dhomse, Graham W. Mann, Juan Carlos Antuña Marrero, Sarah E. Shallcross, Martyn P. Chipperfield, Kenneth S. Carslaw, Lauren Marshall, N. Luke Abraham, and Colin E. Johnson
Atmos. Chem. Phys., 20, 13627–13654, https://doi.org/10.5194/acp-20-13627-2020, https://doi.org/10.5194/acp-20-13627-2020, 2020
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We confirm downward adjustment of SO2 emission to simulate the Pinatubo aerosol cloud with aerosol microphysics models. Similar adjustment is also needed to simulate the El Chichón and Agung volcanic cloud, indicating potential missing removal or vertical redistribution process in models. Important inhomogeneities in the CMIP6 forcing datasets after Agung and El Chichón eruptions are difficult to reconcile. Quasi-biennial oscillation plays an important role in modifying stratospheric warming.
Nina Löbs, David Walter, Cybelli G. G. Barbosa, Sebastian Brill, Rodrigo P. Alves, Gabriela R. Cerqueira, Marta de Oliveira Sá, Alessandro C. de Araújo, Leonardo R. de Oliveira, Florian Ditas, Daniel Moran-Zuloaga, Ana Paula Pires Florentino, Stefan Wolff, Ricardo H. M. Godoi, Jürgen Kesselmeier, Sylvia Mota de Oliveira, Meinrat O. Andreae, Christopher Pöhlker, and Bettina Weber
Biogeosciences, 17, 5399–5416, https://doi.org/10.5194/bg-17-5399-2020, https://doi.org/10.5194/bg-17-5399-2020, 2020
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Cryptogamic organisms, such as bryophytes, lichens, and algae, cover major parts of vegetation in the Amazonian rain forest, but their relevance in biosphere–atmosphere exchange, climate processes, and nutrient cycling is largely unknown.
Over the duration of 2 years we measured their water content, temperature, and light conditions to get better insights into their physiological activity patterns and thus their potential impact on local, regional, and even global biogeochemical processes.
Lixia Liu, Yafang Cheng, Siwen Wang, Chao Wei, Mira L. Pöhlker, Christopher Pöhlker, Paulo Artaxo, Manish Shrivastava, Meinrat O. Andreae, Ulrich Pöschl, and Hang Su
Atmos. Chem. Phys., 20, 13283–13301, https://doi.org/10.5194/acp-20-13283-2020, https://doi.org/10.5194/acp-20-13283-2020, 2020
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This modeling paper reveals how aerosol–cloud interactions (ACIs) and aerosol–radiation interactions (ARIs) induced by biomass burning (BB) aerosols act oppositely on radiation, cloud, and precipitation in the Amazon during the dry season. The varying relative significance of ACIs and ARIs with BB aerosol concentration leads to a nonlinear dependence of the total climate response on BB aerosol loading and features the growing importance of ARIs at high aerosol loading.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Yohei Shinozuka, Pablo E. Saide, Gonzalo A. Ferrada, Sharon P. Burton, Richard Ferrare, Sarah J. Doherty, Hamish Gordon, Karla Longo, Marc Mallet, Yan Feng, Qiaoqiao Wang, Yafang Cheng, Amie Dobracki, Steffen Freitag, Steven G. Howell, Samuel LeBlanc, Connor Flynn, Michal Segal-Rosenhaimer, Kristina Pistone, James R. Podolske, Eric J. Stith, Joseph Ryan Bennett, Gregory R. Carmichael, Arlindo da Silva, Ravi Govindaraju, Ruby Leung, Yang Zhang, Leonhard Pfister, Ju-Mee Ryoo, Jens Redemann, Robert Wood, and Paquita Zuidema
Atmos. Chem. Phys., 20, 11491–11526, https://doi.org/10.5194/acp-20-11491-2020, https://doi.org/10.5194/acp-20-11491-2020, 2020
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In the southeast Atlantic, well-defined smoke plumes from Africa advect over marine boundary layer cloud decks; both are most extensive around September, when most of the smoke resides in the free troposphere. A framework is put forth for evaluating the performance of a range of global and regional atmospheric composition models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016.
Hamish Gordon, Paul R. Field, Steven J. Abel, Paul Barrett, Keith Bower, Ian Crawford, Zhiqiang Cui, Daniel P. Grosvenor, Adrian A. Hill, Jonathan Taylor, Jonathan Wilkinson, Huihui Wu, and Ken S. Carslaw
Atmos. Chem. Phys., 20, 10997–11024, https://doi.org/10.5194/acp-20-10997-2020, https://doi.org/10.5194/acp-20-10997-2020, 2020
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The Met Office's Unified Model is widely used both for weather forecasting and climate prediction. We present the first version of the model in which both aerosol and cloud particle mass and number concentrations are allowed to evolve separately and independently, which is important for studying how aerosols affect weather and climate. We test the model against aircraft observations near Ascension Island in the Atlantic, focusing on how aerosols can "activate" to become cloud droplets.
James Weber, Scott Archer-Nicholls, Paul Griffiths, Torsten Berndt, Michael Jenkin, Hamish Gordon, Christoph Knote, and Alexander T. Archibald
Atmos. Chem. Phys., 20, 10889–10910, https://doi.org/10.5194/acp-20-10889-2020, https://doi.org/10.5194/acp-20-10889-2020, 2020
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Highly oxygenated organic molecules (HOMs) are important for aerosol growth and new particle formation, particularly in air masses with less sulphuric acid. This new chemical mechanism reproduces measured [HOM] and [HOM precursors] and is concise enough for use in global climate models. The mechanism also reproduces the observed suppression of HOMs by isoprene, suggesting enhanced emissions may not necessarily lead to more aerosols. Greater HOM importance in the pre-industrial era is also shown.
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Short summary
New particle formation in the upper troposphere is important for the global boundary layer aerosol population, and they can be transported downward in Amazonia. We use a global and a regional model to quantify the number of aerosols that are formed at high altitude and transported downward in a 1000 km region. We find that the majority of the aerosols are from outside the region. This suggests that the 1000 km region is unlikely to be a
closed loopfor aerosol formation, transport and growth.
New particle formation in the upper troposphere is important for the global boundary layer...
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