Articles | Volume 16, issue 17
https://doi.org/10.5194/acp-16-10941-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-10941-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
06 Sep 2016
Research article |
| 06 Sep 2016
Inverse modelling of Köhler theory – Part 1: A response surface analysis of CCN spectra with respect to surface-active organic species
Samuel Lowe
Department of Environmental Science and Analytical Chemistry, Stockholm University, Stockholm, Sweden
Bert Bolin Centre for Climate Research, Stockholm University, Stockholm, Sweden
Atmospheric, Oceanic and Planetary Physics, Department of Physics, University of Oxford, Oxford, UK
Daniel G. Partridge
CORRESPONDING AUTHOR
Atmospheric, Oceanic and Planetary Physics, Department of Physics, University of Oxford, Oxford, UK
Department of Environmental Science and Analytical Chemistry, Stockholm University, Stockholm, Sweden
Bert Bolin Centre for Climate Research, Stockholm University, Stockholm, Sweden
David Topping
School of Earth Atmospheric and Environmental Science, University of Manchester, Manchester, UK
National Centre for Atmospheric Science (NCAS), University of Manchester, Manchester, UK
Philip Stier
Atmospheric, Oceanic and Planetary Physics, Department of Physics, University of Oxford, Oxford, UK
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Sarah Wilson Kemsley, Paulo Ceppi, Hendrik Andersen, Jan Cermak, Philip Stier, and Peer Nowack
EGUsphere, https://doi.org/10.5194/egusphere-2024-226, https://doi.org/10.5194/egusphere-2024-226, 2024
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Aiming to inform parameter selection for future observational constraint analyses, we incorporate five candidate meteorological drivers specifically targeting high clouds, into a cloud controlling factor framework within a range of spatial domain sizes. We find a discrepancy between optimal domain size for predicting local and globally-aggregated cloud radiative anomalies, and identify upper tropospheric static stability as an important high-cloud controlling factor.
Karoline Block, Mahnoosh Haghighatnasab, Daniel G. Partridge, Philip Stier, and Johannes Quaas
Earth Syst. Sci. Data, 16, 443–470, https://doi.org/10.5194/essd-16-443-2024, https://doi.org/10.5194/essd-16-443-2024, 2024
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Aerosols being able to act as condensation nuclei for cloud droplets (CCNs) are a key element in cloud formation but very difficult to determine. In this study we present a new global vertically resolved CCN dataset for various humidity conditions and aerosols. It is obtained using an atmospheric model (CAMS reanalysis) that is fed by satellite observations of light extinction (AOD). We investigate and evaluate the abundance of CCNs in the atmosphere and their temporal and spatial occurrence.
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
EGUsphere, https://doi.org/10.5194/egusphere-2024-4, https://doi.org/10.5194/egusphere-2024-4, 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.
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.
William K. Jones, Martin Stengel, and Philip Stier
EGUsphere, https://doi.org/10.5194/egusphere-2023-2059, https://doi.org/10.5194/egusphere-2023-2059, 2023
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Storm clouds cover large areas of the tropics. These clouds both reflect incoming sunlight and trap heat from the atmosphere below, regulating the temperature of the tropics. Over land, storm clouds occur in the late afternoon and evening, and so exist both during the daytime and at night. Changes in this timing could upset the balance of the respective cooling and heating effects of these clouds. We find that isolated storms have a larger effect on this balance than their small size suggests.
Hendrik Andersen, Jan Cermak, Alyson Douglas, Timothy A. Myers, Peer Nowack, Philip Stier, Casey J. Wall, and Sarah Wilson Kemsley
Atmos. Chem. Phys., 23, 10775–10794, https://doi.org/10.5194/acp-23-10775-2023, https://doi.org/10.5194/acp-23-10775-2023, 2023
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This study uses an observation-based cloud-controlling factor framework to study near-global sensitivities of cloud radiative effects to a large number of meteorological and aerosol controls. We present near-global sensitivity patterns to selected thermodynamic, dynamic, and aerosol factors and discuss the physical mechanisms underlying the derived sensitivities. Our study hopes to guide future analyses aimed at constraining cloud feedbacks and aerosol–cloud interactions.
G. Alexander Sokolowsky, Sean W. Freeman, William K. Jones, Julia Kukulies, Fabian Senf, Peter J. Marinescu, Max Heikenfeld, Kelcy N. Brunner, Eric C. Bruning, Scott M. Collis, Robert C. Jackson, Gabrielle R. Leung, Nils Pfeifer, Bhupendra A. Raut, Stephen M. Saleeby, Philip Stier, and Susan C. van den Heever
EGUsphere, https://doi.org/10.5194/egusphere-2023-1722, https://doi.org/10.5194/egusphere-2023-1722, 2023
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Building on previous analysis tools developed for atmospheric science, the original release of the Tracking and Object-Based Analysis (tobac) Python package, v1.2, was open-source, modular, and insensitive to the type of gridded input data. Here, we present the latest version of tobac, v1.5, which substantially improves scientific capabilities and computational efficiency from the previous version. These enhancements permit new uses for tobac in atmospheric science and potentially other fields.
Bjorn Stevens, Stefan Adami, Tariq Ali, Hartwig Anzt, Zafer Aslan, Sabine Attinger, Jaana Bäck, Johanna Baehr, Peter Bauer, Natacha Bernier, Bob Bishop, Hendryk Bockelmann, Sandrine Bony, Veronique Bouchet, Guy Brasseur, David N. Bresch, Sean Breyer, Gilbert Brunet, Pier Luigi Buttigieg, Junji Cao, Christelle Castet, Yafang Cheng, Ayantika Dey Choudhury, Deborah Coen, Susanne Crewell, Atish Dabholkar, Qing Dai, Francisco Doblas-Reyes, Dale Durran, Ayoub El Gaidi, Charlie Ewen, Eleftheria Exarchou, Veronika Eyring, Florencia Falkinhoff, David Farrell, Piers M. Forster, Ariane Frassoni, Claudia Frauen, Oliver Fuhrer, Shahzad Gani, Edwin Gerber, Debra Goldfarb, Jens Grieger, Nicolas Gruber, Wilco Hazeleger, Rolf Herken, Chris Hewitt, Torsten Hoefler, Huang-Hsiung Hsu, Daniela Jacob, Alexandra Jahn, Christian Jakob, Thomas Jung, Christopher Kadow, In-Sik Kang, Sarah Kang, Karthik Kashinath, Katharina Kleinen-von Königslöw, Daniel Klocke, Uta Kloenne, Milan Klöwer, Chihiro Kodama, Stefan Kollet, Tobias Kölling, Jenni Kontkanen, Steve Kopp, Michal Koran, Markku Kulmala, Hanna Lappalainen, Fakhria Latifi, Bryan Lawrence, June Yi Lee, Quentin Lejeun, Christian Lessig, Chao Li, Thomas Lippert, Jürg Luterbacher, Pekka Manninen, Jochem Marotzke, Satoshi Matsouoka, Charlotte Merchant, Peter Messmer, Gero Michel, Kristel Michielsen, Tomoki Miyakawa, Jens Müller, Ramsha Munir, Sandeep Narayanasetti, Ousmane Ndiaye, Carlos Nobre, Achim Oberg, Riko Oki, Tuba Özkan-Haller, Tim Palmer, Stan Posey, Andreas Prein, Odessa Primus, Mike Pritchard, Julie Pullen, Dian Putrasahan, Johannes Quaas, Krishnan Raghavan, Venkatachalam Ramaswamy, Markus Rapp, Florian Rauser, Markus Reichstein, Aromar Revi, Sonakshi Saluja, Masaki Satoh, Vera Schemann, Sebastian Schemm, Christina Schnadt Poberaj, Thomas Schulthess, Cath Senior, Jagadish Shukla, Manmeet Singh, Julia Slingo, Adam Sobel, Silvina Solman, Jenna Spitzer, Detlef Stammer, Philip Stier, Thomas Stocker, Sarah Strock, Hang Su, Petteri Taalas, John Taylor, Susann Tegtmeier, Georg Teutsch, Adrian Tompkins, Uwe Ulbrich, Pier-Luigi Vidale, Chien-Ming Wu, Hao Xu, Najibullah Zaki, Laure Zanna, Tianjun Zhou, and Florian Ziemen
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2023-376, https://doi.org/10.5194/essd-2023-376, 2023
Revised manuscript accepted for ESSD
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To manage Earth in the Anthropocene, new tools, new institutions, and new forms of international cooperation will be required. Earth Virtualization Engines are proposed as international federation of centers of excellence to empower all people to respond to the immense and urgent challenges posed by climate change.
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.
Ross Herbert and Philip Stier
Atmos. Chem. Phys., 23, 4595–4616, https://doi.org/10.5194/acp-23-4595-2023, https://doi.org/10.5194/acp-23-4595-2023, 2023
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We provide robust evidence from multiple sources showing that smoke from fires in the Amazon rainforest significantly modifies the diurnal cycle of convection and cools the climate. Low to moderate amounts of smoke increase deep convective clouds and rain, whilst beyond a threshold amount, the smoke starts to suppress the convection and rain. We are currently at this threshold, suggesting increases in fires from agricultural practices or droughts will reduce cloudiness and rain over the region.
William K. Jones, Matthew W. Christensen, and Philip Stier
Atmos. Meas. Tech., 16, 1043–1059, https://doi.org/10.5194/amt-16-1043-2023, https://doi.org/10.5194/amt-16-1043-2023, 2023
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Geostationary weather satellites have been used to detect storm clouds since their earliest applications. However, this task remains difficult as imaging satellites cannot observe the strong vertical winds that are characteristic of storm clouds. Here we introduce a new method that allows us to detect the early development of storms and continue to track them throughout their lifetime, allowing us to study how their early behaviour affects subsequent weather.
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
Preprint archived
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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.
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.
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.
Matthias Karl, Liisa Pirjola, Tiia Grönholm, Mona Kurppa, Srinivasan Anand, Xiaole Zhang, Andreas Held, Rolf Sander, Miikka Dal Maso, David Topping, Shuai Jiang, Leena Kangas, and Jaakko Kukkonen
Geosci. Model Dev., 15, 3969–4026, https://doi.org/10.5194/gmd-15-3969-2022, https://doi.org/10.5194/gmd-15-3969-2022, 2022
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The community aerosol dynamics model MAFOR includes several advanced features: coupling with an up-to-date chemistry mechanism for volatile organic compounds, a revised Brownian coagulation kernel that takes into account the fractal geometry of soot particles, a multitude of nucleation parameterizations, size-resolved partitioning of semi-volatile inorganics, and a hybrid method for the formation of secondary organic aerosols within the framework of condensation and evaporation.
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.
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.
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.
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.
Langwen Huang and David Topping
Geosci. Model Dev., 14, 2187–2203, https://doi.org/10.5194/gmd-14-2187-2021, https://doi.org/10.5194/gmd-14-2187-2021, 2021
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As our knowledge and understanding of atmospheric aerosol particle evolution and impact grows, designing community mechanistic models requires an ability to capture increasing chemical, physical and therefore numerical complexity. As the landscape of computing software and hardware evolves, it is important to profile the usefulness of emerging platforms in tackling this complexity. With this in mind we present JlBox v1.1, written in Julia.
Jens Redemann, Robert Wood, Paquita Zuidema, Sarah J. Doherty, Bernadette Luna, Samuel E. LeBlanc, Michael S. Diamond, Yohei Shinozuka, Ian Y. Chang, Rei Ueyama, Leonhard Pfister, Ju-Mee Ryoo, Amie N. Dobracki, Arlindo M. da Silva, Karla M. Longo, Meloë S. Kacenelenbogen, Connor J. Flynn, Kristina Pistone, Nichola M. Knox, Stuart J. Piketh, James M. Haywood, Paola Formenti, Marc Mallet, Philip Stier, Andrew S. Ackerman, Susanne E. Bauer, Ann M. Fridlind, Gregory R. Carmichael, Pablo E. Saide, Gonzalo A. Ferrada, Steven G. Howell, Steffen Freitag, Brian Cairns, Brent N. Holben, Kirk D. Knobelspiesse, Simone Tanelli, Tristan S. L'Ecuyer, Andrew M. Dzambo, Ousmane O. Sy, Greg M. McFarquhar, Michael R. Poellot, Siddhant Gupta, Joseph R. O'Brien, Athanasios Nenes, Mary Kacarab, Jenny P. S. Wong, Jennifer D. Small-Griswold, Kenneth L. Thornhill, David Noone, James R. Podolske, K. Sebastian Schmidt, Peter Pilewskie, Hong Chen, Sabrina P. Cochrane, Arthur J. Sedlacek, Timothy J. Lang, Eric Stith, Michal Segal-Rozenhaimer, Richard A. Ferrare, Sharon P. Burton, Chris A. Hostetler, David J. Diner, Felix C. Seidel, Steven E. Platnick, Jeffrey S. Myers, Kerry G. Meyer, Douglas A. Spangenberg, Hal Maring, and Lan Gao
Atmos. Chem. Phys., 21, 1507–1563, https://doi.org/10.5194/acp-21-1507-2021, https://doi.org/10.5194/acp-21-1507-2021, 2021
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Southern Africa produces significant biomass burning emissions whose impacts on regional and global climate are poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA investigation designed to study the key processes that determine these climate impacts. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project, the dataset it produced, and the most important initial findings.
Simon Patrick O'Meara, Shuxuan Xu, David Topping, M. Rami Alfarra, Gerard Capes, Douglas Lowe, Yunqi Shao, and Gordon McFiggans
Geosci. Model Dev., 14, 675–702, https://doi.org/10.5194/gmd-14-675-2021, https://doi.org/10.5194/gmd-14-675-2021, 2021
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User-friendly and open-source software for simulating aerosol chambers is a valuable tool for research scientists in designing and analysing their experiments. This paper describes a new version of such software and will therefore provide a useful reference for those applying it. Central to the paper is an assessment of the software's accuracy through comparison against previously published simulations.
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.
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.
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.
Johannes Quaas, Antti Arola, Brian Cairns, Matthew Christensen, Hartwig Deneke, Annica M. L. Ekman, Graham Feingold, Ann Fridlind, Edward Gryspeerdt, Otto Hasekamp, Zhanqing Li, Antti Lipponen, Po-Lun Ma, Johannes Mülmenstädt, Athanasios Nenes, Joyce E. Penner, Daniel Rosenfeld, Roland Schrödner, Kenneth Sinclair, Odran Sourdeval, Philip Stier, Matthias Tesche, Bastiaan van Diedenhoven, and Manfred Wendisch
Atmos. Chem. Phys., 20, 15079–15099, https://doi.org/10.5194/acp-20-15079-2020, https://doi.org/10.5194/acp-20-15079-2020, 2020
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Anthropogenic pollution particles – aerosols – serve as cloud condensation nuclei and thus increase cloud droplet concentration and the clouds' reflection of sunlight (a cooling effect on climate). This Twomey effect is poorly constrained by models and requires satellite data for better quantification. The review summarizes the challenges in properly doing so and outlines avenues for progress towards a better use of aerosol retrievals and better retrievals of droplet concentrations.
Douglas Morrison, Ian Crawford, Nicholas Marsden, Michael Flynn, Katie Read, Luis Neves, Virginia Foot, Paul Kaye, Warren Stanley, Hugh Coe, David Topping, and Martin Gallagher
Atmos. Chem. Phys., 20, 14473–14490, https://doi.org/10.5194/acp-20-14473-2020, https://doi.org/10.5194/acp-20-14473-2020, 2020
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We provide conservative estimates of the concentrations of bacteria within transatlantic dust clouds, originating from the African continent. We observe significant seasonal differences in the overall concentrations of particles but no seasonal variation in the ratio between bacteria and dust. With bacteria contributing to ice formation at warmer temperatures than dust, our observations should improve the accuracy of climate models.
Nick Schutgens, Andrew M. Sayer, Andreas Heckel, Christina Hsu, Hiren Jethva, Gerrit de Leeuw, Peter J. T. Leonard, Robert C. Levy, Antti Lipponen, Alexei Lyapustin, Peter North, Thomas Popp, Caroline Poulsen, Virginia Sawyer, Larisa Sogacheva, Gareth Thomas, Omar Torres, Yujie Wang, Stefan Kinne, Michael Schulz, and Philip Stier
Atmos. Chem. Phys., 20, 12431–12457, https://doi.org/10.5194/acp-20-12431-2020, https://doi.org/10.5194/acp-20-12431-2020, 2020
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We intercompare 14 different datasets of satellite observations of aerosol. Such measurements are challenging but also provide the best opportunity to globally observe an atmospheric component strongly related to air pollution and climate change. Our study shows that most datasets perform similarly well on a global scale but that locally errors can be quite different. We develop a technique to estimate satellite errors everywhere, even in the absence of surface reference data.
David Topping, David Watts, Hugh Coe, James Evans, Thomas J. Bannan, Douglas Lowe, Caroline Jay, and Jonathan W. Taylor
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-270, https://doi.org/10.5194/gmd-2020-270, 2020
Publication in GMD not foreseen
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Time-series forecasting methods have often been used to mitigate some of the challenges associated with deploying chemical transport models. In this study we deploy and evaluate Facebook’s Prophetmodel v0.6 in predicting hourly concentrations of Nitrogen Dioxide [NO2]. et. Overall we find the Prophet model offers a relatively effective and simple way to make predictions about NO2 at local levels.
Laura Palacios-Peña, Philip Stier, Raquel Lorente-Plazas, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 20, 9679–9700, https://doi.org/10.5194/acp-20-9679-2020, https://doi.org/10.5194/acp-20-9679-2020, 2020
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It is widely known that the impact of aerosol–radiation and aerosol–cloud interactions on the radiative forcing is subject to large uncertainties. This is mainly due to the lack of understanding of aerosol optical properties and vertical distribution, whose uncertainties come from different processes. This work attempts to quantify the sensitivity of aerosol optical properties and their vertical distribution to key physico-chemical processes.
Gunnar Myhre, Bjørn H. Samset, Christian W. Mohr, Kari Alterskjær, Yves Balkanski, Nicolas Bellouin, Mian Chin, James Haywood, Øivind Hodnebrog, Stefan Kinne, Guangxing Lin, Marianne T. Lund, Joyce E. Penner, Michael Schulz, Nick Schutgens, Ragnhild B. Skeie, Philip Stier, Toshihiko Takemura, and Kai Zhang
Atmos. Chem. Phys., 20, 8855–8865, https://doi.org/10.5194/acp-20-8855-2020, https://doi.org/10.5194/acp-20-8855-2020, 2020
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The radiative forcing of the direct aerosol effects can be decomposed into clear-sky and cloudy-sky portions. In this study we use observational methods and two sets of multi-model global aerosol simulations over the industrial era to show that the contribution from cloudy-sky regions is likely weak.
Petroc D. Shelley, Thomas J. Bannan, Stephen D. Worrall, M. Rami Alfarra, Ulrich K. Krieger, Carl J. Percival, Arthur Garforth, and David Topping
Atmos. Chem. Phys., 20, 8293–8314, https://doi.org/10.5194/acp-20-8293-2020, https://doi.org/10.5194/acp-20-8293-2020, 2020
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The methods used to estimate the vapour pressures of compounds in the atmosphere typically perform poorly when applied to organic compounds found in the atmosphere. New measurements have been made and compared to previous experimental data and estimated values so that the limitations within the estimation methods can be identified and in the future be rectified.
Guy Dagan and Philip Stier
Atmos. Chem. Phys., 20, 6291–6303, https://doi.org/10.5194/acp-20-6291-2020, https://doi.org/10.5194/acp-20-6291-2020, 2020
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Ensemble daily simulations for two separate month-long periods over a region near Barbados were conducted to investigate aerosol effects on cloud properties and the atmospheric energy budget. For each day, two simulations were conducted with low and high cloud droplet number concentrations representing clean and polluted conditions, respectively. These simulations are used to distinguish between properties that are robustly affected by changes in aerosol concentrations and those that are not.
Zak Kipling, Laurent Labbouz, and Philip Stier
Atmos. Chem. Phys., 20, 4445–4460, https://doi.org/10.5194/acp-20-4445-2020, https://doi.org/10.5194/acp-20-4445-2020, 2020
Guy Dagan, Philip Stier, Matthew Christensen, Guido Cioni, Daniel Klocke, and Axel Seifert
Atmos. Chem. Phys., 20, 4523–4544, https://doi.org/10.5194/acp-20-4523-2020, https://doi.org/10.5194/acp-20-4523-2020, 2020
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In order to better understand the physical processes behind aerosol effects on the atmospheric energy budget, we analyse numerical simulations of tropical cloud systems. Two sets of simulations, at different dates during the NARVAL 2 field campaign, are simulated with different dominant cloud modes. Our results demonstrate that under different environmental conditions, the response of the atmospheric energy budget to aerosol perturbation could be different.
Natalie R. Gervasi, David O. Topping, and Andreas Zuend
Atmos. Chem. Phys., 20, 2987–3008, https://doi.org/10.5194/acp-20-2987-2020, https://doi.org/10.5194/acp-20-2987-2020, 2020
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Organic aerosols have been shown to exist often in a semi-solid or amorphous, glassy state. Highly viscous particles behave differently than their well-mixed liquid analogues with consequences for a variety of aerosol processes. Here, we introduce a new predictive mixture viscosity model called AIOMFAC-VISC. It enables us to predict the viscosity of aqueous organic mixtures as a function of temperature and chemical composition, covering the full range of liquid, semi-solid, and glassy states.
Parya Broomandi, Xueyu Geng, Weisi Guo, Jong Ryeol Kim, Alessio Pagani, and David Topping
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2019-342, https://doi.org/10.5194/gmd-2019-342, 2020
Revised manuscript not accepted
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As a result of our novel graph-based reduced modeling, we are able to represent high-dimensional knowledge into a causal inference and stability framework.
Kathryn Fowler, Paul Connolly, and David Topping
Atmos. Chem. Phys., 20, 683–698, https://doi.org/10.5194/acp-20-683-2020, https://doi.org/10.5194/acp-20-683-2020, 2020
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Observations of low–temperature cirrus clouds have found unexpectedly low ice crystal numbers and high supersaturations, suggesting an incomplete understanding of the freezing mechanisms under these conditions. The existence of viscous organic aerosol has offered alternative ice nucleation pathways, which have been observed in laboratory studies. We have developed the first cloud parcel model to investigate the effect of viscosity on ice nucleation.
Edward Gryspeerdt, Johannes Mülmenstädt, Andrew Gettelman, Florent F. Malavelle, Hugh Morrison, David Neubauer, Daniel G. Partridge, Philip Stier, Toshihiko Takemura, Hailong Wang, Minghuai Wang, and Kai Zhang
Atmos. Chem. Phys., 20, 613–623, https://doi.org/10.5194/acp-20-613-2020, https://doi.org/10.5194/acp-20-613-2020, 2020
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Aerosol radiative forcing is a key uncertainty in our understanding of the human forcing of the climate, with much of this uncertainty coming from aerosol impacts on clouds. Observation-based estimates of the radiative forcing are typically smaller than those from global models, but it is not clear if they are more reliable. This work shows how the forcing components in global climate models can be identified, highlighting similarities between the two methods and areas for future investigation.
George Spill, Philip Stier, Paul R. Field, and Guy Dagan
Atmos. Chem. Phys., 19, 13507–13517, https://doi.org/10.5194/acp-19-13507-2019, https://doi.org/10.5194/acp-19-13507-2019, 2019
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Shallow convective clouds are among the most common and least understood clouds in the atmosphere. Here we present simulations of realistic, shallow cloud fields in a large domain, in contrast to typical idealised simulations, and find that in these simulations the response to aerosol perturbations is different.
Max Heikenfeld, Peter J. Marinescu, Matthew Christensen, Duncan Watson-Parris, Fabian Senf, Susan C. van den Heever, and Philip Stier
Geosci. Model Dev., 12, 4551–4570, https://doi.org/10.5194/gmd-12-4551-2019, https://doi.org/10.5194/gmd-12-4551-2019, 2019
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We present tobac (Tracking and Object-Based Analysis of Clouds), a newly developed framework for tracking and analysing clouds in different types of datasets. It provides a flexible new way to include the evolution of individual clouds in a wide range of analyses. It is developed as a community project to provide a common basis for the inclusion of existing tracking algorithms and the development of new analyses that involve tracking clouds and other features in geoscientific research.
Øivind Hodnebrog, Gunnar Myhre, Bjørn H. Samset, Kari Alterskjær, Timothy Andrews, Olivier Boucher, Gregory Faluvegi, Dagmar Fläschner, Piers M. Forster, Matthew Kasoar, Alf Kirkevåg, Jean-Francois Lamarque, Dirk Olivié, Thomas B. Richardson, Dilshad Shawki, Drew Shindell, Keith P. Shine, Philip Stier, Toshihiko Takemura, Apostolos Voulgarakis, and Duncan Watson-Parris
Atmos. Chem. Phys., 19, 12887–12899, https://doi.org/10.5194/acp-19-12887-2019, https://doi.org/10.5194/acp-19-12887-2019, 2019
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Different greenhouse gases (e.g. CO2) and aerosols (e.g. black carbon) impact the Earth’s water cycle differently. Here we investigate how various gases and particles impact atmospheric water vapour and its lifetime, i.e., the average number of days that water vapour stays in the atmosphere after evaporation and before precipitation. We find that this lifetime could increase substantially by the end of this century, indicating that important changes in precipitation patterns are excepted.
Duncan Watson-Parris, Nick Schutgens, Carly Reddington, Kirsty J. Pringle, Dantong Liu, James D. Allan, Hugh Coe, Ken S. Carslaw, and Philip Stier
Atmos. Chem. Phys., 19, 11765–11790, https://doi.org/10.5194/acp-19-11765-2019, https://doi.org/10.5194/acp-19-11765-2019, 2019
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The vertical distribution of aerosol in the atmosphere affects its ability to act as cloud condensation nuclei and changes the amount of sunlight it absorbs or reflects. Common global measurements of aerosol provide no information about this vertical distribution. Using a global collection of in situ aircraft measurements to compare with an aerosol–climate model (ECHAM-HAM), we explore the key processes controlling this distribution and find that wet removal plays a key role.
David Neubauer, Sylvaine Ferrachat, Colombe Siegenthaler-Le Drian, Philip Stier, Daniel G. Partridge, Ina Tegen, Isabelle Bey, Tanja Stanelle, Harri Kokkola, and Ulrike Lohmann
Geosci. Model Dev., 12, 3609–3639, https://doi.org/10.5194/gmd-12-3609-2019, https://doi.org/10.5194/gmd-12-3609-2019, 2019
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The global aerosol–climate model ECHAM6.3–HAM2.3 as well as the previous model versions ECHAM5.5–HAM2.0 and ECHAM6.1–HAM2.2 are evaluated. The simulation of clouds has improved in ECHAM6.3–HAM2.3. This has an impact on effective radiative forcing due to aerosol–radiation and aerosol–cloud interactions and equilibrium climate sensitivity, which are weaker in ECHAM6.3–HAM2.3 than in the previous model versions.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Stephanie Fiedler, Stefan Kinne, Wan Ting Katty Huang, Petri Räisänen, Declan O'Donnell, Nicolas Bellouin, Philip Stier, Joonas Merikanto, Twan van Noije, Risto Makkonen, and Ulrike Lohmann
Atmos. Chem. Phys., 19, 6821–6841, https://doi.org/10.5194/acp-19-6821-2019, https://doi.org/10.5194/acp-19-6821-2019, 2019
Ina Tegen, David Neubauer, Sylvaine Ferrachat, Colombe Siegenthaler-Le Drian, Isabelle Bey, Nick Schutgens, Philip Stier, Duncan Watson-Parris, Tanja Stanelle, Hauke Schmidt, Sebastian Rast, Harri Kokkola, Martin Schultz, Sabine Schroeder, Nikos Daskalakis, Stefan Barthel, Bernd Heinold, and Ulrike Lohmann
Geosci. Model Dev., 12, 1643–1677, https://doi.org/10.5194/gmd-12-1643-2019, https://doi.org/10.5194/gmd-12-1643-2019, 2019
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We describe a new version of the aerosol–climate model ECHAM–HAM and show tests of the model performance by comparing different aspects of the aerosol distribution with different datasets. The updated version of HAM contains improved descriptions of aerosol processes, including updated emission fields and cloud processes. While there are regional deviations between the model and observations, the model performs well overall.
Thomas J. Bannan, Michael Le Breton, Michael Priestley, Stephen D. Worrall, Asan Bacak, Nicholas A. Marsden, Archit Mehra, Julia Hammes, Mattias Hallquist, M. Rami Alfarra, Ulrich K. Krieger, Jonathan P. Reid, John Jayne, Wade Robinson, Gordon McFiggans, Hugh Coe, Carl J. Percival, and Dave Topping
Atmos. Meas. Tech., 12, 1429–1439, https://doi.org/10.5194/amt-12-1429-2019, https://doi.org/10.5194/amt-12-1429-2019, 2019
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The Filter Inlet for Gases and AEROsols (FIGAERO) is an inlet designed to be coupled with a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) and provides simultaneous molecular information relating to both the gas- and particle-phase samples. This method has been used to extract vapour pressures of compounds whilst giving quantitative concentrations in the particle phase. Here we detail an ideal set of benchmark compounds for characterization of the FIGAERO.
Max Heikenfeld, Bethan White, Laurent Labbouz, and Philip Stier
Atmos. Chem. Phys., 19, 2601–2627, https://doi.org/10.5194/acp-19-2601-2019, https://doi.org/10.5194/acp-19-2601-2019, 2019
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Aerosols can affect the evolution of deep convective clouds by controlling the cloud droplet number concentration. We perform a detailed analysis of the pathways of such aerosol perturbations through the cloud microphysics in numerical model simulations. By focussing on individually tracked convective cells, we can reveal consistent changes to individual process rates, such as a lifting of freezing and riming, but also major differences between the three different microphysics schemes used.
Elizabeth Forde, Martin Gallagher, Virginia Foot, Roland Sarda-Esteve, Ian Crawford, Paul Kaye, Warren Stanley, and David Topping
Atmos. Chem. Phys., 19, 1665–1684, https://doi.org/10.5194/acp-19-1665-2019, https://doi.org/10.5194/acp-19-1665-2019, 2019
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The abundance and diversity of airborne biological particles in different environments remains poorly constrained. Measurements of such particles were conducted at four sites in the United Kingdom, using real-time fluorescence instrumentation. Using local land cover types, sources of suspected particle types were identified and compared. Most sites exhibited a wet-discharged fungal spore dominance, with the exception of one site, which was inferred to be influenced by a local dairy farm.
Simon Ruske, David O. Topping, Virginia E. Foot, Andrew P. Morse, and Martin W. Gallagher
Atmos. Meas. Tech., 11, 6203–6230, https://doi.org/10.5194/amt-11-6203-2018, https://doi.org/10.5194/amt-11-6203-2018, 2018
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Pollen, bacteria and fungal spores are common in the environment, can have very important implications for public health and may influence the weather. Biological sensors potentially could be used to monitor quantities of these types of particles. However, it is important to transform the measurements from these instruments into counts of these biological particles. The paper tests a variety of approaches for achieving this aim on data collected in a laboratory.
Dawei Hu, David Topping, and Gordon McFiggans
Atmos. Chem. Phys., 18, 14925–14937, https://doi.org/10.5194/acp-18-14925-2018, https://doi.org/10.5194/acp-18-14925-2018, 2018
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Co-condensation of inorganic or organic vapours on growing droplets could significantly enhance both CCN and cloud droplet number concentration, thereby influencing climate. Until now, there has been very few direct observational evidence of this process. We exposed involatile inorganic particles to a moist atmosphere containing a controlled amount of an organic semi-volatile vapour. We measured a much greater growth of the particles than if they had only been exposed to water vapour.
Harri Kokkola, Thomas Kühn, Anton Laakso, Tommi Bergman, Kari E. J. Lehtinen, Tero Mielonen, Antti Arola, Scarlet Stadtler, Hannele Korhonen, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Ina Tegen, Colombe Siegenthaler-Le Drian, Martin G. Schultz, Isabelle Bey, Philip Stier, Nikos Daskalakis, Colette L. Heald, and Sami Romakkaniemi
Geosci. Model Dev., 11, 3833–3863, https://doi.org/10.5194/gmd-11-3833-2018, https://doi.org/10.5194/gmd-11-3833-2018, 2018
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In this paper we present a global aerosol–chemistry–climate model with the focus on its representation for atmospheric aerosol particles. In the model, aerosols are simulated using the aerosol module SALSA2.0, which in this paper is compared to satellite, ground, and aircraft-based observations of the properties of atmospheric aerosol. Based on this study, the model simulated aerosol properties compare well with the observations.
Michael Le Breton, Yujue Wang, Åsa M. Hallquist, Ravi Kant Pathak, Jing Zheng, Yudong Yang, Dongjie Shang, Marianne Glasius, Thomas J. Bannan, Qianyun Liu, Chak K. Chan, Carl J. Percival, Wenfei Zhu, Shengrong Lou, David Topping, Yuchen Wang, Jianzhen Yu, Keding Lu, Song Guo, Min Hu, and Mattias Hallquist
Atmos. Chem. Phys., 18, 10355–10371, https://doi.org/10.5194/acp-18-10355-2018, https://doi.org/10.5194/acp-18-10355-2018, 2018
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This paper utilizes a chemical ionisation mass spectrometer measuring gas and particle-phase organosulfates (OS) simultaneously during a field campaign in Beijing, China, and highlights how high time frequency online measurements enable a detailed analysis of dominant production mechanisms. We find that high aerosol acidity, organic precursor concentration and relative humidity promote the production of OS. The thermogram desorption reveals the potential for semi-volatile gas-phase OS.
Martin G. Schultz, Scarlet Stadtler, Sabine Schröder, Domenico Taraborrelli, Bruno Franco, Jonathan Krefting, Alexandra Henrot, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Colombe Siegenthaler-Le Drian, Sebastian Wahl, Harri Kokkola, Thomas Kühn, Sebastian Rast, Hauke Schmidt, Philip Stier, Doug Kinnison, Geoffrey S. Tyndall, John J. Orlando, and Catherine Wespes
Geosci. Model Dev., 11, 1695–1723, https://doi.org/10.5194/gmd-11-1695-2018, https://doi.org/10.5194/gmd-11-1695-2018, 2018
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The chemistry–climate model ECHAM-HAMMOZ contains a detailed representation of tropospheric and stratospheric reactive chemistry and state-of-the-art parameterizations of aerosols. It thus allows for detailed investigations of chemical processes in the climate system. Evaluation of the model with various observational data yields good results, but the model has a tendency to produce too much OH in the tropics. This highlights the important interplay between atmospheric chemistry and dynamics.
Stefano Decesari, Simona Kovarich, Manuela Pavan, Arianna Bassan, Andrea Ciacci, and David Topping
Atmos. Chem. Phys., 18, 2329–2340, https://doi.org/10.5194/acp-18-2329-2018, https://doi.org/10.5194/acp-18-2329-2018, 2018
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Particulate matter (PM) chemical composition includes thousands of individual organic compounds that have never been tested for their toxicological potential. Computational (in silico) screenings represent a promising approach to identify new target compounds for more in-depth toxicological analyses. We provide here a proof-of-concept evaluation based on ca. 100 aerosol organic compounds. Reliable toxicological predictions were obtained for more than 80 % of them.
Kathryn Fowler, Paul J. Connolly, David O. Topping, and Simon O'Meara
Atmos. Chem. Phys., 18, 1629–1642, https://doi.org/10.5194/acp-18-1629-2018, https://doi.org/10.5194/acp-18-1629-2018, 2018
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This is the first time the Maxwell–Stefan framework has been applied to an atmospheric aerosol core–shell model and shows that there is a complex interplay between the viscous and solubility effects on aerosol composition. Understanding aerosol composition is essential to accurately model their interactions within atmospheric systems. We use simple binary systems to demonstrate how viscosity and solubility both play a role in affecting the rate of diffusion through aerosol particles.
Ulrich K. Krieger, Franziska Siegrist, Claudia Marcolli, Eva U. Emanuelsson, Freya M. Gøbel, Merete Bilde, Aleksandra Marsh, Jonathan P. Reid, Andrew J. Huisman, Ilona Riipinen, Noora Hyttinen, Nanna Myllys, Theo Kurtén, Thomas Bannan, Carl J. Percival, and David Topping
Atmos. Meas. Tech., 11, 49–63, https://doi.org/10.5194/amt-11-49-2018, https://doi.org/10.5194/amt-11-49-2018, 2018
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Vapor pressures of low-volatility organic molecules at atmospheric temperatures reported in the literature often differ by several orders of magnitude between measurement techniques. These discrepancies exceed the stated uncertainty of each technique, which is generally reported to be smaller than a factor of 2. We determined saturation vapor pressures for the homologous series of polyethylene glycols ranging in vapor pressure at 298 K from 1E−7 Pa to 5E−2 Pa as a reference set.
Maria Sand, Bjørn H. Samset, Yves Balkanski, Susanne Bauer, Nicolas Bellouin, Terje K. Berntsen, Huisheng Bian, Mian Chin, Thomas Diehl, Richard Easter, Steven J. Ghan, Trond Iversen, Alf Kirkevåg, Jean-François Lamarque, Guangxing Lin, Xiaohong Liu, Gan Luo, Gunnar Myhre, Twan van Noije, Joyce E. Penner, Michael Schulz, Øyvind Seland, Ragnhild B. Skeie, Philip Stier, Toshihiko Takemura, Kostas Tsigaridis, Fangqun Yu, Kai Zhang, and Hua Zhang
Atmos. Chem. Phys., 17, 12197–12218, https://doi.org/10.5194/acp-17-12197-2017, https://doi.org/10.5194/acp-17-12197-2017, 2017
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The role of aerosols in the changing polar climate is not well understood and the aerosols are poorly constrained in the models. In this study we have compared output from 16 different aerosol models with available observations at both poles. We show that the model median is representative of the observations, but the model spread is large. The Arctic direct aerosol radiative effect over the industrial area is positive during spring due to black carbon and negative during summer due to sulfate.
Bethan White, Edward Gryspeerdt, Philip Stier, Hugh Morrison, Gregory Thompson, and Zak Kipling
Atmos. Chem. Phys., 17, 12145–12175, https://doi.org/10.5194/acp-17-12145-2017, https://doi.org/10.5194/acp-17-12145-2017, 2017
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Aerosols influence cloud and precipitation by modifying cloud droplet number concentrations (CDNCs). We simulate three different types of convective cloud using two different cloud microphysics parameterisations. The simulated cloud and precipitation depends much more strongly on the choice of microphysics scheme than on CDNC. The uncertainty differs between types of convection. Our results highlight a large uncertainty in cloud and precipitation responses to aerosol in current models.
Simon O'Meara, David O. Topping, Rahul A. Zaveri, and Gordon McFiggans
Atmos. Chem. Phys., 17, 10477–10494, https://doi.org/10.5194/acp-17-10477-2017, https://doi.org/10.5194/acp-17-10477-2017, 2017
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To simulate particle-phase diffusion, an analytical expression is desired because it takes less calculation time than a differential equation. Here a correction is found for the analytical solution for when diffusivity is dependent on composition, thereby making it more widely applicable than before. Consequently, we are able to more realistically evaluate the rate limitation (if any) imposed by particle-phase diffusion on component partitioning between the gas and particle phase.
Nick Schutgens, Svetlana Tsyro, Edward Gryspeerdt, Daisuke Goto, Natalie Weigum, Michael Schulz, and Philip Stier
Atmos. Chem. Phys., 17, 9761–9780, https://doi.org/10.5194/acp-17-9761-2017, https://doi.org/10.5194/acp-17-9761-2017, 2017
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We estimate representativeness errors in observations due to mismatching spatio-temporal sampling, on timescales of hours to a year and length scales of 50 to 200 km, for a variety of observing systems (in situ or remote sensing ground sites, satellites with imagers or lidar, etc.) and develop strategies to reduce them. This study is relevant to the use of observations in constructing satellite L3 products, observational intercomparison and model evaluation.
David O. Topping, James Allan, M. Rami Alfarra, and Bernard Aumont
Geosci. Model Dev., 10, 2365–2377, https://doi.org/10.5194/gmd-10-2365-2017, https://doi.org/10.5194/gmd-10-2365-2017, 2017
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Our ability to model the chemical and thermodynamic processes that lead to secondary organic aerosol (SOA) formation is thought to be hampered by the complexity of the system. In this proof of concept study, the ability to train supervised methods to predict electron impact ionisation (EI) mass spectra for the AMS is evaluated to facilitate improved model evaluation. The study demonstrates the use of a methodology that would be improved with more training data and data from simple mixed systems.
Sarah Taylor, Philip Stier, Bethan White, Stephan Finkensieper, and Martin Stengel
Atmos. Chem. Phys., 17, 7035–7053, https://doi.org/10.5194/acp-17-7035-2017, https://doi.org/10.5194/acp-17-7035-2017, 2017
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Variability of convective cloud spans a wide range of temporal and spatial scales and is important for global weather and climate. This study uses satellite data from SEVIRI to quantify the diurnal cycle of cloud top temperatures over a large area. Results indicate that in some regions the diurnal cycle apparent in the observations may be significantly impacted by diurnal variability in the accuracy of the retrieval. These results may interest both the observation and modelling communities.
Simon Ruske, David O. Topping, Virginia E. Foot, Paul H. Kaye, Warren R. Stanley, Ian Crawford, Andrew P. Morse, and Martin W. Gallagher
Atmos. Meas. Tech., 10, 695–708, https://doi.org/10.5194/amt-10-695-2017, https://doi.org/10.5194/amt-10-695-2017, 2017
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Particles such as bacteria, pollen and fungal spores have important implications within the environment and public health sectors. Here we evaluate the performance of various different methods for distinguishing between these different types of particles using a new instrument. We demonstrate that there may be better alternatives to the currently used methods which can be further investigated in future research.
Zak Kipling, Philip Stier, Laurent Labbouz, and Till Wagner
Atmos. Chem. Phys., 17, 327–342, https://doi.org/10.5194/acp-17-327-2017, https://doi.org/10.5194/acp-17-327-2017, 2017
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We present the first evaluation of the convective cloud field model (CCFM) in the context of a global climate model. CCFM attempts to address some of the shortcomings of commonly used representations of convection, in particular allowing for physically based aerosol effects on different types of convective cloud. We show that the model performs well overall in the context of the climate model and is thus well placed to study aerosol–convection–climate interactions at the global scale.
Natalie Weigum, Nick Schutgens, and Philip Stier
Atmos. Chem. Phys., 16, 13619–13639, https://doi.org/10.5194/acp-16-13619-2016, https://doi.org/10.5194/acp-16-13619-2016, 2016
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We introduce a novel technique to isolate the effect of aerosol variability in models from other sources of variability by varying the resolution of aerosol and trace gas fields while maintaining a constant resolution in the rest of the model.
Our results show that aerosol variability has a large impact on simulating aerosol climate effects, even when meteorology and dynamics are fixed. Processes most affected are gas-phase chemistry and aerosol uptake of water through equilibrium reactions.
Our results show that aerosol variability has a large impact on simulating aerosol climate effects, even when meteorology and dynamics are fixed. Processes most affected are gas-phase chemistry and aerosol uptake of water through equilibrium reactions.
François Benduhn, Graham W. Mann, Kirsty J. Pringle, David O. Topping, Gordon McFiggans, and Kenneth S. Carslaw
Geosci. Model Dev., 9, 3875–3906, https://doi.org/10.5194/gmd-9-3875-2016, https://doi.org/10.5194/gmd-9-3875-2016, 2016
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We present a new mathematical formalism that serves to represent exchanges of inorganic matter between the atmosphere gas phase and the aerosol aqueous phase. In a global modelling framework, taking into account these processes may help represent many important features more accurately, such as the formation of cloud droplets or the radiative properties of the atmosphere. The formalism strives to keep an appropriate balance between accuracy and computation efficiency requirements.
Matthew Crooks, Paul Connolly, David Topping, and Gordon McFiggans
Geosci. Model Dev., 9, 3617–3637, https://doi.org/10.5194/gmd-9-3617-2016, https://doi.org/10.5194/gmd-9-3617-2016, 2016
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Semi-volatile compounds, like water, can exist in both vapour phases and condensed phases within a system. This paper presents a method of calculating the condensed and vapour phases of semi-volatile compounds at equilibrium, in particular, when the condensed mass occurs within particles of different sizes and chemical composition. The applications of interest to the authors are those of atmospheric importance such as cloud droplet formation and reflection or absorption of solar radiation.
Duncan Watson-Parris, Nick Schutgens, Nicholas Cook, Zak Kipling, Philip Kershaw, Edward Gryspeerdt, Bryan Lawrence, and Philip Stier
Geosci. Model Dev., 9, 3093–3110, https://doi.org/10.5194/gmd-9-3093-2016, https://doi.org/10.5194/gmd-9-3093-2016, 2016
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In this paper we describe CIS, a new command line tool for the easy visualization, analysis and comparison of a wide variety of gridded and ungridded data sets used in Earth sciences. Users can now use a single tool to not only view plots of satellite, aircraft, station or model data, but also bring them onto the same spatio-temporal sampling. This allows robust, quantitative comparisons to be made easily. CIS is an open-source project and welcomes input from the community.
Philip Stier
Atmos. Chem. Phys., 16, 6595–6607, https://doi.org/10.5194/acp-16-6595-2016, https://doi.org/10.5194/acp-16-6595-2016, 2016
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Cloud droplets form on suitable nuclei from aerosol emissions. Clouds with more droplets have higher reflectance so that aerosol emissions have a cooling climate effect. Numerous publications of these effects rely on passive satellite remote sensing. In this work I use a self consistent global aerosol model to show that a commonly used assumption (passively retrieved aerosol extinction is a suitable proxy for cloud condensation nuclei) is violated for a significant fraction of the Earth.
Nick A. J. Schutgens, Edward Gryspeerdt, Natalie Weigum, Svetlana Tsyro, Daisuke Goto, Michael Schulz, and Philip Stier
Atmos. Chem. Phys., 16, 6335–6353, https://doi.org/10.5194/acp-16-6335-2016, https://doi.org/10.5194/acp-16-6335-2016, 2016
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We show that evaluating global aerosol model data with observations of very different spatial scales (200 vs. 10 km) can lead to large discrepancies, solely due to different spatial sampling. Strategies for reducing these sampling errors are developed and tested using a set of high-resolution model simulations.
Simon O'Meara, David O. Topping, and Gordon McFiggans
Atmos. Chem. Phys., 16, 5299–5313, https://doi.org/10.5194/acp-16-5299-2016, https://doi.org/10.5194/acp-16-5299-2016, 2016
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To understand the effect of atmospheric particulate matter on climate and human health we need to know how it evolves. We investigate how best to estimate diffusion of components through particles by comparing diffusion times from three approaches to solving Fick's Law and find that they agree. This means that scientists can simulate Fickian diffusion through atmospheric particles using the approach best suited to their requirements and have confidence that their model is mathematically sound.
Shipeng Zhang, Minghuai Wang, Steven J. Ghan, Aijun Ding, Hailong Wang, Kai Zhang, David Neubauer, Ulrike Lohmann, Sylvaine Ferrachat, Toshihiko Takeamura, Andrew Gettelman, Hugh Morrison, Yunha Lee, Drew T. Shindell, Daniel G. Partridge, Philip Stier, Zak Kipling, and Congbin Fu
Atmos. Chem. Phys., 16, 2765–2783, https://doi.org/10.5194/acp-16-2765-2016, https://doi.org/10.5194/acp-16-2765-2016, 2016
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The variation of aerosol indirect effects (AIE) in several climate models is investigated across different dynamical regimes. Regimes with strong large-scale ascent are shown to be as important as stratocumulus regimes in studying AIE. AIE over regions with high monthly large-scale surface precipitation rate contributes the most to the total aerosol indirect forcing. These results point to the need to reduce the uncertainty in AIE in different dynamical regimes.
David Topping, Mark Barley, Michael K. Bane, Nicholas Higham, Bernard Aumont, Nicholas Dingle, and Gordon McFiggans
Geosci. Model Dev., 9, 899–914, https://doi.org/10.5194/gmd-9-899-2016, https://doi.org/10.5194/gmd-9-899-2016, 2016
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In this paper we describe the development and application of a new web-based and open-source facility, UManSysProp (http://umansysprop .seaes.manchester.ac.uk), for automating predictions of molecular and atmospheric aerosol properties. Current facilities include pure component vapour pressures, critical properties, and sub-cooled densities of organic molecules; activity coefficient predictions for mixed inorganic-organic liquid systems; hygroscopic growth factors and CCN activation potential.
Zak Kipling, Philip Stier, Colin E. Johnson, Graham W. Mann, Nicolas Bellouin, Susanne E. Bauer, Tommi Bergman, Mian Chin, Thomas Diehl, Steven J. Ghan, Trond Iversen, Alf Kirkevåg, Harri Kokkola, Xiaohong Liu, Gan Luo, Twan van Noije, Kirsty J. Pringle, Knut von Salzen, Michael Schulz, Øyvind Seland, Ragnhild B. Skeie, Toshihiko Takemura, Kostas Tsigaridis, and Kai Zhang
Atmos. Chem. Phys., 16, 2221–2241, https://doi.org/10.5194/acp-16-2221-2016, https://doi.org/10.5194/acp-16-2221-2016, 2016
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The vertical distribution of atmospheric aerosol is an important factor in its effects on climate. In this study we use a sophisticated model of the many interacting processes affecting aerosol in the atmosphere to show that the vertical distribution is typically dominated by only a few of these processes. Constraining these physical processes may help to reduce the large differences between models. However, the important processes are not always the same for different types of aerosol.
N. A. J. Schutgens, D. G. Partridge, and P. Stier
Atmos. Chem. Phys., 16, 1065–1079, https://doi.org/10.5194/acp-16-1065-2016, https://doi.org/10.5194/acp-16-1065-2016, 2016
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When comparing models against observations, researchers often use long-term averages without due regard for the temporal sampling of the underlying data sets.
We study the errors introduced by this practice and show they are often larger than observational errors and comparable to model errors. We further analyse what causes these errors and suggest best practices for eliminating them.
I. Crawford, S. Ruske, D. O. Topping, and M. W. Gallagher
Atmos. Meas. Tech., 8, 4979–4991, https://doi.org/10.5194/amt-8-4979-2015, https://doi.org/10.5194/amt-8-4979-2015, 2015
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HCA analysis methods were evaluated for the purpose of identifying primary biological aerosol sampled with a WIBS. The ward linkage with z-score normalisation could discriminate between five test particles with 98% accuracy. We applied these methods to a previously studied ambient data set, where both methods produced similar results with some minor differences in cluster partitioning. Finally we compared to previous approaches and found our new method offered improved quantification of PBA.
E. Gryspeerdt, P. Stier, B. A. White, and Z. Kipling
Atmos. Chem. Phys., 15, 7557–7570, https://doi.org/10.5194/acp-15-7557-2015, https://doi.org/10.5194/acp-15-7557-2015, 2015
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Wet scavenging generates differences between the aerosol properties in clear-sky scenes (observed by satellites) and cloudy scenes, leading to different
aerosol-precipitation relationships in satellite data and global models. Convective systems usually draw in air from clear-sky regions, but global models have difficulty separating this aerosol from the aerosol in cloudy scenes within a model gridbox. This may prevent models from reproducing the observed aerosol-precipitation relationships.
B. H. Samset, G. Myhre, A. Herber, Y. Kondo, S.-M. Li, N. Moteki, M. Koike, N. Oshima, J. P. Schwarz, Y. Balkanski, S. E. Bauer, N. Bellouin, T. K. Berntsen, H. Bian, M. Chin, T. Diehl, R. C. Easter, S. J. Ghan, T. Iversen, A. Kirkevåg, J.-F. Lamarque, G. Lin, X. Liu, J. E. Penner, M. Schulz, Ø. Seland, R. B. Skeie, P. Stier, T. Takemura, K. Tsigaridis, and K. Zhang
Atmos. Chem. Phys., 14, 12465–12477, https://doi.org/10.5194/acp-14-12465-2014, https://doi.org/10.5194/acp-14-12465-2014, 2014
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Far from black carbon (BC) emission sources, present climate models are unable to reproduce flight measurements. By comparing recent models with data, we find that the atmospheric lifetime of BC may be overestimated in models. By adjusting modeled BC concentrations to measurements in remote regions - over oceans and at high altitudes - we arrive at a reduced estimate for BC radiative forcing over the industrial era.
N. A. J. Schutgens and P. Stier
Atmos. Chem. Phys., 14, 11657–11686, https://doi.org/10.5194/acp-14-11657-2014, https://doi.org/10.5194/acp-14-11657-2014, 2014
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The complexity of the physical and chemical processes effectively turns global aerosol models into black boxes. In an attempt to lift the veil, we present a detailed budget of process contributions (emissions, nucleation, sulfate condensation, coagulation, aging, deposition) in ECHAM5.5-HAM2 across varying length- and timescales. We show a clear hierarchy exists in process importance, that can be used in improving and simplifying the model and for understanding discrepancies with observation.
E. Gryspeerdt, P. Stier, and D. G. Partridge
Atmos. Chem. Phys., 14, 9677–9694, https://doi.org/10.5194/acp-14-9677-2014, https://doi.org/10.5194/acp-14-9677-2014, 2014
R. E. L. West, P. Stier, A. Jones, C. E. Johnson, G. W. Mann, N. Bellouin, D. G. Partridge, and Z. Kipling
Atmos. Chem. Phys., 14, 6369–6393, https://doi.org/10.5194/acp-14-6369-2014, https://doi.org/10.5194/acp-14-6369-2014, 2014
G. W. Mann, K. S. Carslaw, C. L. Reddington, K. J. Pringle, M. Schulz, A. Asmi, D. V. Spracklen, D. A. Ridley, M. T. Woodhouse, L. A. Lee, K. Zhang, S. J. Ghan, R. C. Easter, X. Liu, P. Stier, Y. H. Lee, P. J. Adams, H. Tost, J. Lelieveld, S. E. Bauer, K. Tsigaridis, T. P. C. van Noije, A. Strunk, E. Vignati, N. Bellouin, M. Dalvi, C. E. Johnson, T. Bergman, H. Kokkola, K. von Salzen, F. Yu, G. Luo, A. Petzold, J. Heintzenberg, A. Clarke, J. A. Ogren, J. Gras, U. Baltensperger, U. Kaminski, S. G. Jennings, C. D. O'Dowd, R. M. Harrison, D. C. S. Beddows, M. Kulmala, Y. Viisanen, V. Ulevicius, N. Mihalopoulos, V. Zdimal, M. Fiebig, H.-C. Hansson, E. Swietlicki, and J. S. Henzing
Atmos. Chem. Phys., 14, 4679–4713, https://doi.org/10.5194/acp-14-4679-2014, https://doi.org/10.5194/acp-14-4679-2014, 2014
C. Jiao, M. G. Flanner, Y. Balkanski, S. E. Bauer, N. Bellouin, T. K. Berntsen, H. Bian, K. S. Carslaw, M. Chin, N. De Luca, T. Diehl, S. J. Ghan, T. Iversen, A. Kirkevåg, D. Koch, X. Liu, G. W. Mann, J. E. Penner, G. Pitari, M. Schulz, Ø. Seland, R. B. Skeie, S. D. Steenrod, P. Stier, T. Takemura, K. Tsigaridis, T. van Noije, Y. Yun, and K. Zhang
Atmos. Chem. Phys., 14, 2399–2417, https://doi.org/10.5194/acp-14-2399-2014, https://doi.org/10.5194/acp-14-2399-2014, 2014
P. J. Connolly, D. O. Topping, F. Malavelle, and G. McFiggans
Atmos. Chem. Phys., 14, 2289–2302, https://doi.org/10.5194/acp-14-2289-2014, https://doi.org/10.5194/acp-14-2289-2014, 2014
E. Gryspeerdt, P. Stier, and D. G. Partridge
Atmos. Chem. Phys., 14, 1141–1158, https://doi.org/10.5194/acp-14-1141-2014, https://doi.org/10.5194/acp-14-1141-2014, 2014
B. S. Grandey, P. Stier, R. G. Grainger, and T. M. Wagner
Atmos. Chem. Phys., 13, 10689–10701, https://doi.org/10.5194/acp-13-10689-2013, https://doi.org/10.5194/acp-13-10689-2013, 2013
L. A. Lee, K. J. Pringle, C. L. Reddington, G. W. Mann, P. Stier, D. V. Spracklen, J. R. Pierce, and K. S. Carslaw
Atmos. Chem. Phys., 13, 8879–8914, https://doi.org/10.5194/acp-13-8879-2013, https://doi.org/10.5194/acp-13-8879-2013, 2013
Z. Kipling, P. Stier, J. P. Schwarz, A. E. Perring, J. R. Spackman, G. W. Mann, C. E. Johnson, and P. J. Telford
Atmos. Chem. Phys., 13, 5969–5986, https://doi.org/10.5194/acp-13-5969-2013, https://doi.org/10.5194/acp-13-5969-2013, 2013
P. Stier, N. A. J. Schutgens, N. Bellouin, H. Bian, O. Boucher, M. Chin, S. Ghan, N. Huneeus, S. Kinne, G. Lin, X. Ma, G. Myhre, J. E. Penner, C. A. Randles, B. Samset, M. Schulz, T. Takemura, F. Yu, H. Yu, and C. Zhou
Atmos. Chem. Phys., 13, 3245–3270, https://doi.org/10.5194/acp-13-3245-2013, https://doi.org/10.5194/acp-13-3245-2013, 2013
B. S. Grandey, P. Stier, and T. M. Wagner
Atmos. Chem. Phys., 13, 3177–3184, https://doi.org/10.5194/acp-13-3177-2013, https://doi.org/10.5194/acp-13-3177-2013, 2013
C. A. Randles, S. Kinne, G. Myhre, M. Schulz, P. Stier, J. Fischer, L. Doppler, E. Highwood, C. Ryder, B. Harris, J. Huttunen, Y. Ma, R. T. Pinker, B. Mayer, D. Neubauer, R. Hitzenberger, L. Oreopoulos, D. Lee, G. Pitari, G. Di Genova, J. Quaas, F. G. Rose, S. Kato, S. T. Rumbold, I. Vardavas, N. Hatzianastassiou, C. Matsoukas, H. Yu, F. Zhang, H. Zhang, and P. Lu
Atmos. Chem. Phys., 13, 2347–2379, https://doi.org/10.5194/acp-13-2347-2013, https://doi.org/10.5194/acp-13-2347-2013, 2013
B. H. Samset, G. Myhre, M. Schulz, Y. Balkanski, S. Bauer, T. K. Berntsen, H. Bian, N. Bellouin, T. Diehl, R. C. Easter, S. J. Ghan, T. Iversen, S. Kinne, A. Kirkevåg, J.-F. Lamarque, G. Lin, X. Liu, J. E. Penner, Ø. Seland, R. B. Skeie, P. Stier, T. Takemura, K. Tsigaridis, and K. Zhang
Atmos. Chem. Phys., 13, 2423–2434, https://doi.org/10.5194/acp-13-2423-2013, https://doi.org/10.5194/acp-13-2423-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface
Weakened aerosol–radiation interaction exacerbating ozone pollution in eastern China since China's clean air actions
Uncertainties from biomass burning aerosols in air quality models obscure public health impacts in Southeast Asia
Oxidative potential apportionment of atmospheric PM1: a new approach combining high-sensitive online analysers for chemical composition and offline OP measurement technique
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon
An updated modeling framework to simulate Los Angeles air quality – Part 1: Model development, evaluation, and source apportionment
Frequent haze events associated with transport and stagnation over the corridor between the North China Plain and Yangtze River Delta
Evaluation of WRF-Chem-simulated meteorology and aerosols over northern India during the severe pollution episode of 2016
How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption
pH regulates the formation of organosulfates and inorganic sulfate from organic peroxide reaction with dissolved SO2 in aquatic media
Technical note: Accurate, reliable, and high-resolution air quality predictions by improving the Copernicus Atmosphere Monitoring Service using a novel statistical post-processing method
Contribution of intermediate-volatility organic compounds from on-road transport to secondary organic aerosol levels in Europe
Secondary Organic Aerosols Derived from Intermediate Volatility n-Alkanes Adopt Low Viscous Phase State
Development of an integrated model framework for multi-air-pollutant exposure assessments in high-density cities
CAMx–UNIPAR simulation of secondary organic aerosol mass formed from multiphase reactions of hydrocarbons under the Central Valley urban atmospheres of California
Impact of urbanization on fine particulate matter concentrations over central Europe
Measurement report: Assessing the impacts of emission uncertainty on aerosol optical properties and radiative forcing from biomass burning in peninsular Southeast Asia
Significant impact of urban-tree biogenic emissions on air quality estimated by a bottom-up inventory and chemistry-transport modeling
The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics
Dynamics-based estimates of decline trend with fine temporal variations in China's PM2.5 emissions
Modeling atmospheric brown carbon in the GISS ModelE Earth system model
Dual roles of inorganic aqueous phase on SOA growth from benzene and phenol
Effects of simulated secondary organic aerosol water on PM1 levels and composition over the US
Reactive organic carbon air emissions from mobile sources in the United States
Development and evaluation of processes affecting simulation of diel fine particulate matter variation in the GEOS-Chem model
Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements
Evolution of atmospheric age of particles and its implications for the formation of a severe haze event in eastern China
A multimodel evaluation of the potential impact of shipping on particle species in the Mediterranean Sea
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying pre-existing particles – Part 2: Modeling chemical drivers and 3-D NPF occurrence
How does tropospheric VOC chemistry affect climate? An investigation of preindustrial control simulations using the Community Earth System Model version 2
Anthropogenic amplification of biogenic secondary organic aerosol production
A dynamic parameterization of sulfuric acid–dimethylamine nucleation and its application in three-dimensional modeling
Modeling dust mineralogical composition: sensitivity to soil mineralogy atlases and their expected climate impacts
Assessment of the impacts of cloud chemistry on surface SO2 and sulfate levels in typical regions of China
Impact of Landes forest fires on air quality in France during the 2022 summer
Global nitrogen and sulfur deposition mapping using a measurement–model fusion approach
Comprehensive simulations of new particle formation events in Beijing with a cluster dynamics–multicomponent sectional model
Implications of differences between recent anthropogenic aerosol emission inventories for diagnosed AOD and radiative forcing from 1990 to 2019
Unbalanced emission reductions of different species and sectors in China during COVID-19 lockdown derived by multi-species surface observation assimilation
Simulating organic aerosol in Delhi with WRF-Chem using the volatility-basis-set approach: exploring model uncertainty with a Gaussian process emulator
Modelling wintertime sea-spray aerosols under Arctic haze conditions
Impact of solar geoengineering on wildfires in the 21st century in CESM2/WACCM6
Linking gas, particulate, and toxic endpoints to air emissions in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Contribution of regional aerosol nucleation to low-level CCN in an Amazonian deep convective environment: results from a regionally nested global model
Coarse particulate matter air quality in East Asia: implications for fine particulate nitrate
Foreign emissions exacerbate PM2.5 pollution in China through nitrate chemistry
Analysis of new particle formation events and comparisons to simulations of particle number concentrations based on GEOS-Chem–advanced particle microphysics in Beijing, China
Simulation of organic aerosol, its precursors, and related oxidants in the Landes pine forest in southwestern France: accounting for domain-specific land use and physical conditions
Modelling the European wind-blown dust emissions and their impact on particulate matter (PM) concentrations
Rui Wang, Yang Cheng, Shasha Chen, Rongrong Li, Yue Hu, Xiaokai Guo, Tianlei Zhang, Fengmin Song, and Hao Li
Atmos. Chem. Phys., 24, 4029–4046, https://doi.org/10.5194/acp-24-4029-2024, https://doi.org/10.5194/acp-24-4029-2024, 2024
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We used quantum chemical calculations, Born–Oppenheimer molecular dynamics simulations, and the ACDC kinetic model to characterize SO3–H2SO4 interaction in the gas phase and at the air–water interface and to study the effect of H2S2O7 on H2SO4–NH3-based clusters. The work expands our understanding of new pathways for the loss of SO3 in acidic polluted areas and helps reveal some missing sources of NPF in metropolitan industrial regions and understand the atmospheric organic–sulfur cycle better.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 24, 4001–4015, https://doi.org/10.5194/acp-24-4001-2024, https://doi.org/10.5194/acp-24-4001-2024, 2024
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The present study quantifies the response of aerosol–radiation interaction (ARI) to anthropogenic emission reduction from 2013 to 2017, with the main focus on the contribution to changed O3 concentrations over eastern China both in summer and winter using the WRF-Chem model. The weakened ARI due to decreased anthropogenic emission aggravates the summer (winter) O3 pollution by +0.81 ppb (+0.63 ppb), averaged over eastern China.
Margaret R. Marvin, Paul I. Palmer, Fei Yao, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 24, 3699–3715, https://doi.org/10.5194/acp-24-3699-2024, https://doi.org/10.5194/acp-24-3699-2024, 2024
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We use an atmospheric chemistry model to investigate aerosols emitted from fire activity across Southeast Asia. We find that the limited nature of measurements in this region leads to large uncertainties that significantly hinder the model representation of these aerosols and their impacts on air quality. As a result, the number of monthly attributable deaths is underestimated by as many as 4500, particularly in March at the peak of the mainland burning season.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
Yuemeng Ji, Zhang Shi, Wenjian Li, Jiaxin Wang, Qiuju Shi, Yixin Li, Lei Gao, Ruize Ma, Weijun Lu, Lulu Xu, Yanpeng Gao, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 3079–3091, https://doi.org/10.5194/acp-24-3079-2024, https://doi.org/10.5194/acp-24-3079-2024, 2024
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The formation mechanisms for secondary brown carbon (SBrC) contributed by multifunctional reduced nitrogen compounds (RNCs) remain unclear. Hence, from combined laboratory experiments and quantum chemical calculations, we investigated the heterogeneous reactions of glyoxal (GL) with multifunctional RNCs, which are driven by four-step indirect nucleophilic addition reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Feifan Yan, Hang Su, Yafang Cheng, Rujin Huang, Hong Liao, Ting Yang, Yuanyuan Zhu, Shaoqing Zhang, Lifang Sheng, Wenbin Kou, Xinran Zeng, Shengnan Xiang, Xiaohong Yao, Huiwang Gao, and Yang Gao
Atmos. Chem. Phys., 24, 2365–2376, https://doi.org/10.5194/acp-24-2365-2024, https://doi.org/10.5194/acp-24-2365-2024, 2024
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PM2.5 pollution is a major air quality issue deteriorating human health, and previous studies mostly focus on regions like the North China Plain and Yangtze River Delta. However, the characteristics of PM2.5 concentrations between these two regions are studied less often. Focusing on the transport corridor region, we identify an interesting seesaw transport phenomenon with stagnant weather conditions, conducive to PM2.5 accumulation over this region, resulting in large health effects.
Prerita Agarwal, David S. Stevenson, and Mathew R. Heal
Atmos. Chem. Phys., 24, 2239–2266, https://doi.org/10.5194/acp-24-2239-2024, https://doi.org/10.5194/acp-24-2239-2024, 2024
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Air pollution levels across northern India are amongst some of the worst in the world, with episodic and hazardous haze events. Here, the ability of the WRF-Chem model to predict air quality over northern India is assessed against several datasets. Whilst surface wind speed and particle pollution peaks are over- and underestimated, respectively, meteorology and aerosol trends are adequately captured, and we conclude it is suitable for investigating severe particle pollution events.
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.
Lin Du, Xiaofan Lv, Makroni Lily, Kun Li, and Narcisse Tsona Tchinda
Atmos. Chem. Phys., 24, 1841–1853, https://doi.org/10.5194/acp-24-1841-2024, https://doi.org/10.5194/acp-24-1841-2024, 2024
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This study explores the pH effect on the reaction of dissolved SO2 with selected organic peroxides. Results show that the formation of organic and/or inorganic sulfate from these peroxides strongly depends on their electronic structures, and these processes are likely to alter the chemical composition of dissolved organic matter in different ways. The rate constants of these reactions exhibit positive pH and temperature dependencies within pH 1–10 and 240–340 K ranges.
Angelo Riccio and Elena Chianese
Atmos. Chem. Phys., 24, 1673–1689, https://doi.org/10.5194/acp-24-1673-2024, https://doi.org/10.5194/acp-24-1673-2024, 2024
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Starting from the Copernicus Atmosphere Monitoring Service (CAMS), we provided a novel ensemble statistical post-processing approach to improve their air quality predictions. Our approach is able to provide reliable short-term forecasts of pollutant concentrations, which is a key challenge in supporting national authorities in their tasks related to EU Air Quality Directives, such as planning and reporting the state of air quality to the citizens.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
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Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
EGUsphere, https://doi.org/10.5194/egusphere-2024-51, https://doi.org/10.5194/egusphere-2024-51, 2024
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SOA derived from n-alkanes is a major component of anthropogenic particulate matter. We provide a comprehensive analysis of n-alkane SOA by explicit chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopt low viscous semisolid or liquid states. Our results indicate little kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Zhiyuan Li, Kin-Fai Ho, Harry Fung Lee, and Steve Hung Lam Yim
Atmos. Chem. Phys., 24, 649–661, https://doi.org/10.5194/acp-24-649-2024, https://doi.org/10.5194/acp-24-649-2024, 2024
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This study developed an integrated model framework for accurate multi-air-pollutant exposure assessments in high-density and high-rise cities. Following the proposed integrated model framework, we established multi-air-pollutant exposure models for four major PM10 chemical species as well as four criteria air pollutants with R2 values ranging from 0.73 to 0.93. The proposed framework serves as an important tool for combined exposure assessment in epidemiological studies.
Yujin Jo, Myoseon Jang, Sanghee Han, Azad Madhu, Bonyoung Koo, Yiqin Jia, Zechen Yu, Soontae Kim, and Jinsoo Park
Atmos. Chem. Phys., 24, 487–508, https://doi.org/10.5194/acp-24-487-2024, https://doi.org/10.5194/acp-24-487-2024, 2024
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The CAMx–UNIPAR model simulated the SOA budget formed via multiphase reactions of hydrocarbons and the impact of emissions and climate on SOA characteristics under California’s urban environments during winter 2018. SOA growth was dominated by daytime oxidation of long-chain alkanes and nighttime terpene oxidation with O3 and NO−3 radicals. The spatial distributions of anthropogenic SOA were affected by the northwesterly wind, whereas those of biogenic SOA were insensitive to wind directions.
Peter Huszar, Alvaro Patricio Prieto Perez, Lukáš Bartík, Jan Karlický, and Anahi Villalba-Pradas
Atmos. Chem. Phys., 24, 397–425, https://doi.org/10.5194/acp-24-397-2024, https://doi.org/10.5194/acp-24-397-2024, 2024
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Urbanization transforms rural land into artificial land, while due to human activities, it also introduces a great quantity of emissions. We quantify the impact of urbanization on the final particulate matter pollutant levels by looking not only at these emissions, but also at the way urban land cover influences meteorological conditions, how the removal of pollutants changes due to urban land cover, and how biogenic emissions from vegetation change due to less vegetation in urban areas.
Yinbao Jin, Yiming Liu, Xiao Lu, Xiaoyang Chen, Ao Shen, Haofan Wang, Yinping Cui, Yifei Xu, Siting Li, Jian Liu, Ming Zhang, Yingying Ma, and Qi Fan
Atmos. Chem. Phys., 24, 367–395, https://doi.org/10.5194/acp-24-367-2024, https://doi.org/10.5194/acp-24-367-2024, 2024
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This study aims to address these issues by evaluating eight independent biomass burning (BB) emission inventories (GFED, FINN1.5, FINN2.5 MOS, FINN2.5 MOSVIS, GFAS, FEER, QFED, and IS4FIRES) using the WRF-Chem model and analyzing their impact on aerosol optical properties (AOPs) and direct radiative forcing (DRF) during wildfire events in peninsular Southeast Asia (PSEA) that occurred in March 2019.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
EGUsphere, https://doi.org/10.5194/egusphere-2023-2786, https://doi.org/10.5194/egusphere-2023-2786, 2023
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This study presents the development of a bottom-up inventory of urban-tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air-quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 % and of ozone by 1.0 % on average over the two months.
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.
Zhen Peng, Lili Lei, Zhe-Min Tan, Meigen Zhang, Aijun Ding, and Xingxia Kou
Atmos. Chem. Phys., 23, 14505–14520, https://doi.org/10.5194/acp-23-14505-2023, https://doi.org/10.5194/acp-23-14505-2023, 2023
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Annual PM2.5 emissions in China consistently decreased by about 3% to 5% from 2017 to 2020 with spatial variations and seasonal dependencies. High-temporal-resolution and dynamics-based PM2.5 emission estimates provide quantitative diurnal variations for each season. Significant reductions in PM2.5 emissions in the North China Plain and northeast of China in 2020 were caused by COVID-19.
Maegan A. DeLessio, Kostas Tsigaridis, Susanne E. Bauer, Jacek Chowdhary, and Gregory L. Schuster
EGUsphere, https://doi.org/10.5194/egusphere-2023-2472, https://doi.org/10.5194/egusphere-2023-2472, 2023
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This study presents the first explicit representation of brown carbon aerosols in the GISS ModelE Earth system model (ESM). Model sensitivity to a range of brown carbon parameters, as well as model performance compared to AERONET and MODIS retrievals of total aerosol properties, was assessed. General recommendations for incorporating brown carbon into ESMs are also included.
Jiwon Choi, Myoseon Jang, and Spencer Blau
EGUsphere, https://doi.org/10.5194/egusphere-2023-2461, https://doi.org/10.5194/egusphere-2023-2461, 2023
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A persistent phenoxy radical (PPR) effectively forms via a heterogeneous reaction of phenol and phenol-related products in the presence of wet-inorganic aerosol. These PPR can catalytically consume ozone during a NOx cycle and negatively influence SOA formation. SOA formation from phenol or benzene is simulated using the UNIPAR model which predicted SOA formation via multiphase reactions of hydrocarbons and compared with chamber data obtained under varying NOx levels, humidity, and seed types.
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.
Benjamin N. Murphy, Darrell Sonntag, Karl M. Seltzer, Havala O. T. Pye, Christine Allen, Evan Murray, Claudia Toro, Drew R. Gentner, Cheng Huang, Shantanu Jathar, Li Li, Andrew A. May, and Allen L. Robinson
Atmos. Chem. Phys., 23, 13469–13483, https://doi.org/10.5194/acp-23-13469-2023, https://doi.org/10.5194/acp-23-13469-2023, 2023
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We update methods for calculating organic particle and vapor emissions from mobile sources in the USA. Conventionally, particulate matter (PM) and volatile organic carbon (VOC) are speciated without consideration of primary semivolatile emissions. Our methods integrate state-of-the-science speciation profiles and correct for common artifacts when sampling emissions in a laboratory. We quantify impacts of the emission updates on ambient pollution with the Community Multiscale Air Quality model.
Yanshun Li, Randall V. Martin, Chi Li, Brian L. Boys, Aaron van Donkelaar, Jun Meng, and Jeffrey R. Pierce
Atmos. Chem. Phys., 23, 12525–12543, https://doi.org/10.5194/acp-23-12525-2023, https://doi.org/10.5194/acp-23-12525-2023, 2023
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We developed and evaluated processes affecting within-day (diel) variability in PM2.5 concentrations in a chemical transport model over the contiguous US. Diel variability in PM2.5 for the contiguous US is driven by early-morning accumulation into a shallow mixed layer, decreases from mid-morning through afternoon with mixed-layer growth, increases from mid-afternoon through evening as the mixed-layer collapses, and decreases overnight as emissions decrease.
Chupeng Zhang, Shangfei Hai, Yang Gao, Yuhang Wang, Shaoqing Zhang, Lifang Sheng, Bin Zhao, Shuxiao Wang, Jingkun Jiang, Xin Huang, Xiaojing Shen, Junying Sun, Aura Lupascu, Manish Shrivastava, Jerome D. Fast, Wenxuan Cheng, Xiuwen Guo, Ming Chu, Nan Ma, Juan Hong, Qiaoqiao Wang, Xiaohong Yao, and Huiwang Gao
Atmos. Chem. Phys., 23, 10713–10730, https://doi.org/10.5194/acp-23-10713-2023, https://doi.org/10.5194/acp-23-10713-2023, 2023
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New particle formation is an important source of atmospheric particles, exerting critical influences on global climate. Numerical models are vital tools to understanding atmospheric particle evolution, which, however, suffer from large biases in simulating particle numbers. Here we improve the model chemical processes governing particle sizes and compositions. The improved model reveals substantial contributions of newly formed particles to climate through effects on cloud condensation nuclei.
Xiaodong Xie, Jianlin Hu, Momei Qin, Song Guo, Min Hu, Dongsheng Ji, Hongli Wang, Shengrong Lou, Cheng Huang, Chong Liu, Hongliang Zhang, Qi Ying, Hong Liao, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 10563–10578, https://doi.org/10.5194/acp-23-10563-2023, https://doi.org/10.5194/acp-23-10563-2023, 2023
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The atmospheric age of particles reflects how long particles have been formed and suspended in the atmosphere, which is closely associated with the evolution processes of particles. An analysis of the atmospheric age of PM2.5 provides a unique perspective on the evolution processes of different PM2.5 components. The results also shed lights on how to design effective emission control actions under unfavorable meteorological conditions.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Sara Jutterström, Jana Moldanova, Elisa Majamäki, and Jukka-Pekka Jalkanen
Atmos. Chem. Phys., 23, 10163–10189, https://doi.org/10.5194/acp-23-10163-2023, https://doi.org/10.5194/acp-23-10163-2023, 2023
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The Mediterranean Sea is a heavily trafficked shipping area, and air quality monitoring stations in numerous cities along the Mediterranean coast have detected high levels of air pollutants originating from shipping emissions. The current study investigates how existing restrictions on shipping-related emissions to the atmosphere ensure compliance with legislation. Focus was laid on fine particles and particle species, which were simulated with five different chemical transport models.
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
EGUsphere, https://doi.org/10.5194/egusphere-2023-1919, https://doi.org/10.5194/egusphere-2023-1919, 2023
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The presented study deals with the attribution of particulate matter (PM) concentrations to anthropogenic emissions over Central Europe using regional scale models. It calculates the present-day contributions of different emissions sectors to urban concentrations of PM and their secondary components. Moreover, the study investigates the effect of chemical non-linearities by using multiple methods of source attribution and calculation of secondary organic aerosol.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
EGUsphere, https://doi.org/10.5194/egusphere-2023-540, https://doi.org/10.5194/egusphere-2023-540, 2023
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We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
Noah A. Stanton and Neil F. Tandon
Atmos. Chem. Phys., 23, 9191–9216, https://doi.org/10.5194/acp-23-9191-2023, https://doi.org/10.5194/acp-23-9191-2023, 2023
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Chemistry in Earth’s atmosphere has a potentially strong but very uncertain impact on climate. Past attempts to fully model chemistry in Earth’s troposphere (the lowest layer of the atmosphere) typically simplified the representation of Earth’s surface, which in turn limited the ability to simulate changes in climate. The cutting-edge model that we use in this study does not require such simplification, and we use it to examine the climate effects of chemical interactions in the troposphere.
Yiqi Zheng, Larry W. Horowitz, Raymond Menzel, David J. Paynter, Vaishali Naik, Jingyi Li, and Jingqiu Mao
Atmos. Chem. Phys., 23, 8993–9007, https://doi.org/10.5194/acp-23-8993-2023, https://doi.org/10.5194/acp-23-8993-2023, 2023
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Biogenic secondary organic aerosols (SOAs) account for a large fraction of fine aerosol at the global scale. Using long-term measurements and a climate model, we investigate anthropogenic impacts on biogenic SOA at both decadal and centennial timescales. Results show that despite reductions in biogenic precursor emissions, SOA has been strongly amplified by anthropogenic emissions since the preindustrial era and exerts a cooling radiative forcing.
Yuyang Li, Jiewen Shen, Bin Zhao, Runlong Cai, Shuxiao Wang, Yang Gao, Manish Shrivastava, Da Gao, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 23, 8789–8804, https://doi.org/10.5194/acp-23-8789-2023, https://doi.org/10.5194/acp-23-8789-2023, 2023
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We set up a new parameterization for 1.4 nm particle formation rates from sulfuric acid–dimethylamine (SA–DMA) nucleation, fully including the effects of coagulation scavenging and cluster stability. Incorporating the new parameterization into 3-D chemical transport models, we achieved better consistencies between simulation results and observation data. This new parameterization provides new insights into atmospheric nucleation simulations and its effects on atmospheric pollution or health.
María Gonçalves Ageitos, Vincenzo Obiso, Ron L. Miller, Oriol Jorba, Martina Klose, Matt Dawson, Yves Balkanski, Jan Perlwitz, Sara Basart, Enza Di Tomaso, Jerónimo Escribano, Francesca Macchia, Gilbert Montané, Natalie M. Mahowald, Robert O. Green, David R. Thompson, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 8623–8657, https://doi.org/10.5194/acp-23-8623-2023, https://doi.org/10.5194/acp-23-8623-2023, 2023
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Dust aerosols affect our climate differently depending on their mineral composition. We include dust mineralogy in an atmospheric model considering two existing soil maps, which still have large associated uncertainties. The soil data and the distribution of the minerals in different aerosol sizes are key to our model performance. We find significant regional variations in climate-relevant variables, which supports including mineralogy in our current models and the need for improved soil maps.
Jianyan Lu, Sunling Gong, Jian Zhang, Jianmin Chen, Lei Zhang, and Chunhong Zhou
Atmos. Chem. Phys., 23, 8021–8037, https://doi.org/10.5194/acp-23-8021-2023, https://doi.org/10.5194/acp-23-8021-2023, 2023
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WRF/CUACE was used to assess the cloud chemistry contribution in China. Firstly, the CUACE cloud chemistry scheme was found to reproduce well the cloud processing and consumption of H2O2, O3, and SO2, as well as the increase of sulfate. Secondly, during cloud availability in December under a heavy pollution episode, sulfate production increased 60–95 % and SO2 was reduced by over 80 %. This study provides a way to analyze the phenomenon of overestimation of SO2 in many chemical transport models.
Laurent Menut, Arineh Cholakian, Guillaume Siour, Rémy Lapere, Romain Pennel, Sylvain Mailler, and Bertrand Bessagnet
Atmos. Chem. Phys., 23, 7281–7296, https://doi.org/10.5194/acp-23-7281-2023, https://doi.org/10.5194/acp-23-7281-2023, 2023
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This study is about the wildfires occurring in France during the summer 2022. We study the forest fires that took place in the Landes during the summer of 2022. We show the direct impact of these fires on the air quality, especially downstream of the smoke plume towards the Paris region. We quantify the impact of these fires on the pollutants peak concentrations and the possible exceedance of thresholds.
Hannah J. Rubin, Joshua S. Fu, Frank Dentener, Rui Li, Kan Huang, and Hongbo Fu
Atmos. Chem. Phys., 23, 7091–7102, https://doi.org/10.5194/acp-23-7091-2023, https://doi.org/10.5194/acp-23-7091-2023, 2023
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We update the 2010 global deposition budget for nitrogen (N) and sulfur (S) with new regional wet deposition measurements, improving the ensemble results of 11 global chemistry transport models from HTAP II. Our study demonstrates that a global measurement–model fusion approach can substantially improve N and S deposition model estimates at a regional scale and represents a step forward toward the WMO goal of global fusion products for accurately mapping harmful air pollution.
Chenxi Li, Yuyang Li, Xiaoxiao Li, Runlong Cai, Yaxin Fan, Xiaohui Qiao, Rujing Yin, Chao Yan, Yishuo Guo, Yongchun Liu, Jun Zheng, Veli-Matti Kerminen, Markku Kulmala, Huayun Xiao, and Jingkun Jiang
Atmos. Chem. Phys., 23, 6879–6896, https://doi.org/10.5194/acp-23-6879-2023, https://doi.org/10.5194/acp-23-6879-2023, 2023
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New particle formation and growth in polluted environments are not fully understood despite intensive research. We applied a cluster dynamics–multicomponent sectional model to simulate the new particle formation events observed in Beijing, China. The simulation approximately captures how the events evolve. Further diagnosis shows that the oxygenated organic molecules may have been under-detected, and modulating their abundance leads to significantly improved simulation–observation agreement.
Marianne Tronstad Lund, Gunnar Myhre, Ragnhild Bieltvedt Skeie, Bjørn Hallvard Samset, and Zbigniew Klimont
Atmos. Chem. Phys., 23, 6647–6662, https://doi.org/10.5194/acp-23-6647-2023, https://doi.org/10.5194/acp-23-6647-2023, 2023
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Here we show that differences, in magnitude and trend, between recent global anthropogenic emission inventories have a notable influence on simulated regional abundances of anthropogenic aerosol over the 1990–2019 period. This, in turn, affects estimates of radiative forcing. Our findings form a basis for comparing existing and upcoming studies on anthropogenic aerosols using different emission inventories.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Yele Sun, Pingqing Fu, Meng Gao, Huangjian Wu, Miaomiao Lu, Qian Wu, Shuyuan Huang, Wenxuan Sui, Jie Li, Xiaole Pan, Lin Wu, Hajime Akimoto, and Gregory R. Carmichael
Atmos. Chem. Phys., 23, 6217–6240, https://doi.org/10.5194/acp-23-6217-2023, https://doi.org/10.5194/acp-23-6217-2023, 2023
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A multi-air-pollutant inversion system has been developed in this study to estimate emission changes in China during COVID-19 lockdown. The results demonstrate that the lockdown is largely a nationwide road traffic control measure with NOx emissions decreasing by ~40 %. Emissions of other species only decreased by ~10 % due to smaller effects of lockdown on other sectors. Assessment results further indicate that the lockdown only had limited effects on the control of PM2.5 and O3 in China.
Ernesto Reyes-Villegas, Douglas Lowe, Jill S. Johnson, Kenneth S. Carslaw, Eoghan Darbyshire, Michael Flynn, James D. Allan, Hugh Coe, Ying Chen, Oliver Wild, Scott Archer-Nicholls, Alex Archibald, Siddhartha Singh, Manish Shrivastava, Rahul A. Zaveri, Vikas Singh, Gufran Beig, Ranjeet Sokhi, and Gordon McFiggans
Atmos. Chem. Phys., 23, 5763–5782, https://doi.org/10.5194/acp-23-5763-2023, https://doi.org/10.5194/acp-23-5763-2023, 2023
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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.
Eleftherios Ioannidis, Kathy S. Law, Jean-Christophe Raut, Louis Marelle, Tatsuo Onishi, Rachel M. Kirpes, Lucia M. Upchurch, Thomas Tuch, Alfred Wiedensohler, Andreas Massling, Henrik Skov, Patricia K. Quinn, and Kerri A. Pratt
Atmos. Chem. Phys., 23, 5641–5678, https://doi.org/10.5194/acp-23-5641-2023, https://doi.org/10.5194/acp-23-5641-2023, 2023
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Remote and local anthropogenic emissions contribute to wintertime Arctic haze, with enhanced aerosol concentrations, but natural sources, which also contribute, are less well studied. Here, modelled wintertime sea-spray aerosols are improved in WRF-Chem over the wider Arctic by including updated wind speed and temperature-dependent treatments. As a result, anthropogenic nitrate aerosols are also improved. Open leads are confirmed to be the main source of sea-spray aerosols over northern Alaska.
Wenfu Tang, Simone Tilmes, David M. Lawrence, Fang Li, Cenlin He, Louisa K. Emmons, Rebecca R. Buchholz, and Lili Xia
Atmos. Chem. Phys., 23, 5467–5486, https://doi.org/10.5194/acp-23-5467-2023, https://doi.org/10.5194/acp-23-5467-2023, 2023
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Globally, total wildfire burned area is projected to increase over the 21st century under scenarios without geoengineering and decrease under the two geoengineering scenarios. Geoengineering reduces fire by decreasing surface temperature and wind speed and increasing relative humidity and soil water. However, geoengineering also yields reductions in precipitation, which offset some of the fire reduction.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
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Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
Xuemei Wang, Hamish Gordon, Daniel P. Grosvenor, Meinrat O. Andreae, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 4431–4461, https://doi.org/10.5194/acp-23-4431-2023, https://doi.org/10.5194/acp-23-4431-2023, 2023
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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.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
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Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Jun-Wei Xu, Jintai Lin, Gan Luo, Jamiu Adeniran, and Hao Kong
Atmos. Chem. Phys., 23, 4149–4163, https://doi.org/10.5194/acp-23-4149-2023, https://doi.org/10.5194/acp-23-4149-2023, 2023
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Research on the sources of Chinese PM2.5 pollution has focused on the contributions of China’s domestic emissions. However, the impact of foreign anthropogenic emissions has typically been simplified or neglected. Here we find that foreign anthropogenic emissions play an important role in Chinese PM2.5 pollution through chemical interactions between foreign-transported pollutants and China’s local emissions. Thus, foreign emission reductions are essential for improving Chinese air quality.
Kun Wang, Xiaoyan Ma, Rong Tian, and Fangqun Yu
Atmos. Chem. Phys., 23, 4091–4104, https://doi.org/10.5194/acp-23-4091-2023, https://doi.org/10.5194/acp-23-4091-2023, 2023
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From 12 March to 6 April 2016 in Beijing, there were 11 typical new particle formation days, 13 non-event days, and 2 undefined days. We first analyzed the favorable background of new particle formation in Beijing and then conducted the simulations using four nucleation schemes based on a global chemistry transport model (GEOS-Chem) to understand the nucleation mechanism.
Arineh Cholakian, Matthias Beekmann, Guillaume Siour, Isabelle Coll, Manuela Cirtog, Elena Ormeño, Pierre-Marie Flaud, Emilie Perraudin, and Eric Villenave
Atmos. Chem. Phys., 23, 3679–3706, https://doi.org/10.5194/acp-23-3679-2023, https://doi.org/10.5194/acp-23-3679-2023, 2023
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This article revolves around the simulation of biogenic secondary organic aerosols in the Landes forest (southwestern France). Several sensitivity cases involving biogenic emission factors, land cover data, anthropogenic emissions, and physical or meteorological parameters were performed and each compared to measurements both in the forest canopy and around the forest. The chemistry behind the formation of these aerosols and their production and transport in the forest canopy is discussed.
Marina Liaskoni, Peter Huszar, Lukáš Bartík, Alvaro Patricio Prieto Perez, Jan Karlický, and Ondřej Vlček
Atmos. Chem. Phys., 23, 3629–3654, https://doi.org/10.5194/acp-23-3629-2023, https://doi.org/10.5194/acp-23-3629-2023, 2023
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Wind-blown dust (WBD) emissions emitted from European soils are estimated for the 2007–2016 period, and their impact on the total particulate matter (PM) concentration is calculated. We found a considerable increase in PM concentrations due to such emissions, especially on selected days (rather than on a seasonal average). We also found that WBD emissions are strongest over western Europe, and the highest impacts on PM are calculated for this region.
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Short summary
A novel inverse modelling framework is developed for analysing the sensitivity of cloud condensation nuclei (CCN) concentrations to simultaneous perturbations in multiple model parameters at atmospherically relevant humidities. Many parameter interactions are identified and CCN concentrations are found to be relatively insensitive to bulk–surface partitioning, while aerosol concentration, surface tension, composition and solution ideality exhibit a higher degree of sensitivity.
A novel inverse modelling framework is developed for analysing the sensitivity of cloud...
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