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ACP | Articles | Volume 20, issue 4
Atmos. Chem. Phys., 20, 2489–2512, 2020
https://doi.org/10.5194/acp-20-2489-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-2489-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 20, 2489–2512, 2020
https://doi.org/10.5194/acp-20-2489-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-2489-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
Research article 02 Mar 2020
Research article | 02 Mar 2020
A robust clustering algorithm for analysis of composition-dependent organic aerosol thermal desorption measurements
Ziyue Li et al.
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Yao Wang, Yue Zhao, Yuchen Wang, Jian-Zhen Yu, Jingyuan Shao, Ping Liu, Wenfei Zhu, Zhen Cheng, Ziyue Li, Naiqiang Yan, and Huayun Xiao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-784, https://doi.org/10.5194/acp-2020-784, 2020
Preprint under review for ACP
Short summary
Short summary
Organosulfates (OS) are important constituents and tracers of secondary organic aerosols (SOA) in the atmosphere. We comprehensively characterized the OS species in ambient aerosols in Shanghai, China. We find that the contribution of OS and SOA to OA has increased in recent years and that OS production was largely controlled by the oxidant level (Ox), in particular in summer. We infer that the mitigation of Ox pollution can effectively reduce the production of OS and SOA in eastern China.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
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Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Ziyue Li, Katherine A. Smith, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 14585–14608, https://doi.org/10.5194/acp-18-14585-2018, https://doi.org/10.5194/acp-18-14585-2018, 2018
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We investigated the influence of relative humidity (RH) on the heterogeneous oxidation of secondary organic aerosol (SOA) particles by OH radicals. We observed significantly faster volume loss and compositional change of SOA at high RH, showing that viscosity differences determine compositional changes, but variability in either the uptake coefficient or the fragmentation probability are required to explain the difference in volume loss between low and high RH.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Yao Wang, Yue Zhao, Yuchen Wang, Jian-Zhen Yu, Jingyuan Shao, Ping Liu, Wenfei Zhu, Zhen Cheng, Ziyue Li, Naiqiang Yan, and Huayun Xiao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-784, https://doi.org/10.5194/acp-2020-784, 2020
Preprint under review for ACP
Short summary
Short summary
Organosulfates (OS) are important constituents and tracers of secondary organic aerosols (SOA) in the atmosphere. We comprehensively characterized the OS species in ambient aerosols in Shanghai, China. We find that the contribution of OS and SOA to OA has increased in recent years and that OS production was largely controlled by the oxidant level (Ox), in particular in summer. We infer that the mitigation of Ox pollution can effectively reduce the production of OS and SOA in eastern China.
Olli-Pekka Tikkanen, Angela Buchholz, Arttu Ylisirniö, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 20, 10441–10458, https://doi.org/10.5194/acp-20-10441-2020, https://doi.org/10.5194/acp-20-10441-2020, 2020
Short summary
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We compared the volatility distributions of secondary organic aerosol (SOA) constituents estimated from isothermal evaporation experiments from either particle size change data, by process modelling and global optimization, or from mass spectrometer data with positive matrix factorization analysis. Our results show that, despite the two very different estimation methods, the volatility distributions are comparable if uncertainties are taken into account.
Samantha J. Kramer, Claudia Alvarez, Anne E. Barkley, Peter R. Colarco, Lillian Custals, Rodrigo Delgadillo, Cassandra J. Gaston, Ravi Govindaraju, and Paquita Zuidema
Atmos. Chem. Phys., 20, 10047–10062, https://doi.org/10.5194/acp-20-10047-2020, https://doi.org/10.5194/acp-20-10047-2020, 2020
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Comparisons of sea salt and size-resolved dust mass concentration measurements over southeast Florida to those from the MERRA-2/GEOS-5 FP aerosol reanalysis show the reanalysis depicts excessive sea salt and puts too much dust in larger intermediate sizes than do the measurements. The vertical distribution of the dust mass is approximately correct. The incorrect reanalysis aerosol speciation and dust sizes have implications for the modeling of their transport, deposition, and radiative impact.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
Arttu Ylisirniö, Luis Barreira, Iida Pullinen, Angela Buchholz, John Jayne, Jordan E. Krechmer, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-254, https://doi.org/10.5194/amt-2020-254, 2020
Preprint under review for AMT
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FIGAERO-ToF-CIMS enables online volatility measurements of chemical compounds in ambient aerosols. Previously published volatility calibration results however differ from each other significantly. In this study we investigate the reason for this discrepancy. We found a major source of error in the widely used syringe deposition method and propose a new method for volatility calibration by using atomized calibration compounds.
Christopher D. Cappa, Christopher Y. Lim, David H. Hagan, Matthew Coggon, Abigail Koss, Kanako Sekimoto, Joost de Gouw, Timothy B. Onasch, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 8511–8532, https://doi.org/10.5194/acp-20-8511-2020, https://doi.org/10.5194/acp-20-8511-2020, 2020
Short summary
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Smoke from combustion of a wide range of biomass fuels (e.g., leaves, twigs, logs, peat, and dung) was photochemically aged in a small chamber for up to 8 d of equivalent atmospheric aging. Upon aging, the particle chemical composition and ability to absorb sunlight changed owing to reactions in both the gas and particulate phases. We developed a model to explain the observations and used this to derive insights into the aging of smoke in the atmosphere.
Ryan Schmedding, Quazi Z. Rasool, Yue Zhang, Havala O. T. Pye, Haofei Zhang, Yuzhi Chen, Jason D. Surratt, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Allen H. Goldstein, and William Vizuete
Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, https://doi.org/10.5194/acp-20-8201-2020, 2020
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Accurate model prediction of aerosol concentrations is a known challenge. It is assumed in many modeling systems that aerosols are in a homogeneously mixed phase state. It has been observed that aerosols do phase separate and can form a highly viscous organic shell with an aqueous core impacting the formation processes of aerosols. This work is a model implementation to determine an aerosol's phase state using glass transition temperature and aerosol composition.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-543, https://doi.org/10.5194/acp-2020-543, 2020
Preprint under review for ACP
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX-SOA concentration changes. The explicit chemistry predicted substantial changes of IEPOX-SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physico-chemical dependencies in future SOA prediction.
Angela Buchholz, Arttu Ylisirniö, Wei Huang, Claudia Mohr, Manjula Canagaratna, Douglas R. Worsnop, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 20, 7693–7716, https://doi.org/10.5194/acp-20-7693-2020, https://doi.org/10.5194/acp-20-7693-2020, 2020
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To understand the role of aerosol particles in the atmosphere, it is necessary to know their detailed chemical composition and physical properties, especially volatility. The thermal desorption data from FIGAERO–CIMS provides both but are difficult to analyse. With positive matrix factorisation, we can separate instrument background from the real signal. Compounds can be classified by their apparent volatility, and the contribution of thermal decomposition in the instrument can be identified.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Sini Isokääntä, Eetu Kari, Angela Buchholz, Liqing Hao, Siegfried Schobesberger, Annele Virtanen, and Santtu Mikkonen
Atmos. Meas. Tech., 13, 2995–3022, https://doi.org/10.5194/amt-13-2995-2020, https://doi.org/10.5194/amt-13-2995-2020, 2020
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Online mass spectrometry produces large amounts of data. These data can be interpreted with statistical methods, enabling scientists to more easily understand the underlying processes. We compared these techniques on car exhaust measurements. We show differences and similarities between the methods and give recommendations on applicability of the methods on certain types of data. We show that applying multiple methods leads to more robust results, thus increasing reliability of the findings.
Camille Mouchel-Vallon, Julia Lee-Taylor, Alma Hodzic, Paulo Artaxo, Bernard Aumont, Marie Camredon, David Gurarie, Jose-Luis Jimenez, Donald H. Lenschow, Scot T. Martin, Janaina Nascimento, John J. Orlando, Brett B. Palm, John E. Shilling, Manish Shrivastava, and Sasha Madronich
Atmos. Chem. Phys., 20, 5995–6014, https://doi.org/10.5194/acp-20-5995-2020, https://doi.org/10.5194/acp-20-5995-2020, 2020
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The GoAmazon 2014/5 field campaign took place near the city of Manaus, Brazil, isolated in the Amazon rainforest, to study the impacts of urban pollution on natural air masses. We simulated this campaign with an extremely detailed organic chemistry model to understand how the city would affect the growth and composition of natural aerosol particles. Discrepancies between the model and the measurements indicate that the chemistry of naturally emitted organic compounds is still poorly understood.
Arttu Ylisirniö, Angela Buchholz, Claudia Mohr, Zijun Li, Luis Barreira, Andrew Lambe, Celia Faiola, Eetu Kari, Taina Yli-Juuti, Sergey A. Nizkorodov, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Chem. Phys., 20, 5629–5644, https://doi.org/10.5194/acp-20-5629-2020, https://doi.org/10.5194/acp-20-5629-2020, 2020
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We studied the chemical composition and volatility of secondary organic aerosol (SOA) particles formed from emissions of Scots pines and compared those results to SOA formed from α-pinene and from a sesquiterpene mixture. We found that SOA formed from single precursors cannot capture the properties of SOA formed from real plant emissions.
Lawrence I. Kleinman, Arthur J. Sedlacek III, Kouji Adachi, Peter R. Buseck, Sonya Collier, Manvendra K. Dubey, Anna L. Hodshire, Ernie Lewis, Timothy B. Onasch, Jeffery R. Pierce, John Shilling, Stephen R. Springston, Jian Wang, Qi Zhang, Shan Zhou, and Robert J. Yokelson
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-239, https://doi.org/10.5194/acp-2020-239, 2020
Revised manuscript accepted for ACP
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Aerosols from wildfires effect the Earth's temperature by absorbing light or reflecting it back into space. This study investigates time-dependent chemical, microphysical, and optical properties of aerosols generated by wildfires in the Pacific Northwest, USA. Wildfire smoke plumes were traversed by an instrumented aircraft at locations near the fire and up to 3.5-hour travel time downwind. Although there was no net aerosol production, aerosol particles grew and became more efficient scatters.
Sidhant J. Pai, Colette L. Heald, Jeffrey R. Pierce, Salvatore C. Farina, Eloise A. Marais, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Ann M. Middlebrook, Hugh Coe, John E. Shilling, Roya Bahreini, Justin H. Dingle, and Kennedy Vu
Atmos. Chem. Phys., 20, 2637–2665, https://doi.org/10.5194/acp-20-2637-2020, https://doi.org/10.5194/acp-20-2637-2020, 2020
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Aerosols in the atmosphere have significant health and climate impacts. Organic aerosol (OA) accounts for a large fraction of the total aerosol burden, but models have historically struggled to accurately simulate it. This study compares two very different OA model schemes and evaluates them against a suite of globally distributed airborne measurements with the goal of providing insight into the strengths and weaknesses of each approach across different environments.
Fan Mei, Jian Wang, Jennifer M. Comstock, Ralf Weigel, Martina Krämer, Christoph Mahnke, John E. Shilling, Johannes Schneider, Christiane Schulz, Charles N. Long, Manfred Wendisch, Luiz A. T. Machado, Beat Schmid, Trismono Krisna, Mikhail Pekour, John Hubbe, Andreas Giez, Bernadett Weinzierl, Martin Zoeger, Mira L. Pöhlker, Hans Schlager, Micael A. Cecchini, Meinrat O. Andreae, Scot T. Martin, Suzane S. de Sá, Jiwen Fan, Jason Tomlinson, Stephen Springston, Ulrich Pöschl, Paulo Artaxo, Christopher Pöhlker, Thomas Klimach, Andreas Minikin, Armin Afchine, and Stephan Borrmann
Atmos. Meas. Tech., 13, 661–684, https://doi.org/10.5194/amt-13-661-2020, https://doi.org/10.5194/amt-13-661-2020, 2020
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In 2014, the US DOE G1 aircraft and the German HALO aircraft overflew the Amazon basin to study how aerosols influence cloud cycles under a clean condition and around a tropical megacity. This paper describes how to meaningfully compare similar measurements from two research aircraft and identify the potential measurement issue. We also discuss the uncertainty range for each measurement for further usage in model evaluation and satellite data validation.
Crystal D. McClure, Christopher Y. Lim, David H. Hagan, Jesse H. Kroll, and Christopher D. Cappa
Atmos. Chem. Phys., 20, 1531–1547, https://doi.org/10.5194/acp-20-1531-2020, https://doi.org/10.5194/acp-20-1531-2020, 2020
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We characterized various optical, chemical, and physical properties of particles produced from combustion of a variety of different biomass fuels, many representative of those found in the western US. We find that many properties scale with the ratio between bulk average organic aerosol and black carbon mass concentrations, although there are some properties that do not.
Eetu Kari, Liqing Hao, Arttu Ylisirniö, Angela Buchholz, Ari Leskinen, Pasi Yli-Pirilä, Ilpo Nuutinen, Kari Kuuspalo, Jorma Jokiniemi, Celia L. Faiola, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 15651–15671, https://doi.org/10.5194/acp-19-15651-2019, https://doi.org/10.5194/acp-19-15651-2019, 2019
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We present, for the first time, the dual effect of GDI-vehicle exhaust on α-pinene SOA mass yield suppression. The first effect is a well-known NOx effect, but the second effect is more complex. Our results imply that this second effect is related to change of reaction pathways of α-pinene in the presence of GDI exhaust. The presence of vehicle exhaust caused more than 50 % suppression in α-pinene SOA mass yield compared to the α-pinene SOA mass yield measured in the absence of GDI emissions.
Giulia Stefenelli, Veronika Pospisilova, Felipe D. Lopez-Hilfiker, Kaspar R. Daellenbach, Christoph Hüglin, Yandong Tong, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 19, 14825–14848, https://doi.org/10.5194/acp-19-14825-2019, https://doi.org/10.5194/acp-19-14825-2019, 2019
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, https://doi.org/10.5194/acp-19-14875-2019, 2019
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Wildfire emissions significantly contribute to adverse air quality; however, the chemical processes that lead to hazardous pollutants, such as ozone, are not fully understood. In this study, we describe laboratory experiments where we simulate the atmospheric chemistry of smoke emitted from a range of biomass fuels. We show that certain understudied compounds, such as furans and phenolic compounds, are significant contributors to pollutants formed as a result of typical atmospheric oxidation.
Rupert Holzinger, W. Joe F. Acton, William J. Bloss, Martin Breitenlechner, Leigh R. Crilley, Sébastien Dusanter, Marc Gonin, Valerie Gros, Frank N. Keutsch, Astrid Kiendler-Scharr, Louisa J. Kramer, Jordan E. Krechmer, Baptiste Languille, Nadine Locoge, Felipe Lopez-Hilfiker, Dušan Materić, Sergi Moreno, Eiko Nemitz, Lauriane L. J. Quéléver, Roland Sarda Esteve, Stéphane Sauvage, Simon Schallhart, Roberto Sommariva, Ralf Tillmann, Sergej Wedel, David R. Worton, Kangming Xu, and Alexander Zaytsev
Atmos. Meas. Tech., 12, 6193–6208, https://doi.org/10.5194/amt-12-6193-2019, https://doi.org/10.5194/amt-12-6193-2019, 2019
Christopher Y. Lim, David H. Hagan, Matthew M. Coggon, Abigail R. Koss, Kanako Sekimoto, Joost de Gouw, Carsten Warneke, Christopher D. Cappa, and Jesse H. Kroll
Atmos. Chem. Phys., 19, 12797–12809, https://doi.org/10.5194/acp-19-12797-2019, https://doi.org/10.5194/acp-19-12797-2019, 2019
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Wildfires are a large source of gases and particles to the atmosphere, both of which impact human health and climate. The amount and composition of particles from wildfires can change with time in the atmosphere; however, the impact of aging is not well understood. In a series of controlled laboratory experiments, we show that the particles are oxidized and a significant fraction of the gas-phase carbon (24 %–56 %) is converted to particle mass over the course of several days in the atmosphere.
Markus Leiminger, Stefan Feil, Paul Mutschlechner, Arttu Ylisirniö, Daniel Gunsch, Lukas Fischer, Alfons Jordan, Siegfried Schobesberger, Armin Hansel, and Gerhard Steiner
Atmos. Meas. Tech., 12, 5231–5246, https://doi.org/10.5194/amt-12-5231-2019, https://doi.org/10.5194/amt-12-5231-2019, 2019
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We introduce an alternative type of atmospheric pressure interface time-of-flight mass spectrometer (APi-TOF) with the main difference of using hexapole instead of quadrupole ion guides. The transfer of cluster ions through the hexapoles was characterised with focus on transmission efficiency, mass range and fragmentation of cluster ions. At the CERN CLOUD experiment we compared the performance of the ioniAPi-TOF with a standard quadrupole APi-TOF under controlled conditions.
Felipe D. Lopez-Hilfiker, Veronika Pospisilova, Wei Huang, Markus Kalberer, Claudia Mohr, Giulia Stefenelli, Joel A. Thornton, Urs Baltensperger, Andre S. H. Prevot, and Jay G. Slowik
Atmos. Meas. Tech., 12, 4867–4886, https://doi.org/10.5194/amt-12-4867-2019, https://doi.org/10.5194/amt-12-4867-2019, 2019
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We present a novel, field-deployable extractive electrospray time-of-flight mass spectrometer (EESI-TOF), which provides real-time, near-molecular measurements of organic aerosol at atmospherically relevant concentrations, addressing a critical gap in existing measurement capabilities. Successful deployments of the EESI-TOF for laboratory measurements, ground-based ambient sampling, and aboard a research aircraft highlight the versatility and potential of the EESI-TOF system.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
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Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Ingeborg E. Nielsen, Henrik Skov, Andreas Massling, Axel C. Eriksson, Manuel Dall'Osto, Heikki Junninen, Nina Sarnela, Robert Lange, Sonya Collier, Qi Zhang, Christopher D. Cappa, and Jacob K. Nøjgaard
Atmos. Chem. Phys., 19, 10239–10256, https://doi.org/10.5194/acp-19-10239-2019, https://doi.org/10.5194/acp-19-10239-2019, 2019
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Measurements of the chemical composition of sub-micrometer aerosols were carried out in northern Greenland during the Arctic haze (February–May) where concentrations are high due to favorable conditions for long-range transport. Sulfate was the dominant aerosol (66 %), followed by organic matter (24 %). The highest black carbon concentrations where observed in February. Source apportionment yielded three factors: a primary factor (12 %), an Arctic haze factor (64 %) and a marine factor (22 %).
Erin E. McDuffie, Caroline C. Womack, Dorothy L. Fibiger, William P. Dube, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Joel A. Thornton, Alexander Moravek, Jennifer G. Murphy, Munkhbayar Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 19, 9287–9308, https://doi.org/10.5194/acp-19-9287-2019, https://doi.org/10.5194/acp-19-9287-2019, 2019
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Populated mountain basins, including the Salt Lake Valley (SLV) in Utah, suffer from wintertime stagnation events that trap emissions near the surface and cause fine particulate matter (PM2.5) concentrations to reach unhealthy levels. Previously limited by a lack of nighttime measurements, this study uses 2017 UWFPS aircraft campaign data, in combination with a box model, to show that nitrogen chemistry above the surface at night is a major source of PM2.5 during a wintertime event in the SLV.
Xiaoxi Liu, Benjamin Deming, Demetrios Pagonis, Douglas A. Day, Brett B. Palm, Ranajit Talukdar, James M. Roberts, Patrick R. Veres, Jordan E. Krechmer, Joel A. Thornton, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 12, 3137–3149, https://doi.org/10.5194/amt-12-3137-2019, https://doi.org/10.5194/amt-12-3137-2019, 2019
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Delays or losses of gases in sampling tubing and instrumental surfaces due to surface interactions can lead to inaccurate quantification. By sampling with several chemical ionization mass spectrometers and six tubing materials, we quantify delays of semivolatile organic compounds and small polar gases. Delay times generally increase with decreasing volatility or increasing polarity and also depend on materials. The method and results will inform inlet material selection and instrumental design.
Ali Akherati, Christopher D. Cappa, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, Stephen M. Griffith, Sebastien Dusanter, Philip S. Stevens, and Shantanu H. Jathar
Atmos. Chem. Phys., 19, 4561–4594, https://doi.org/10.5194/acp-19-4561-2019, https://doi.org/10.5194/acp-19-4561-2019, 2019
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Unburned and partially burned organic compounds emitted from fossil fuel and biomass combustion can react in the atmosphere in the presence of sunlight to form particles. In this work, we use an air pollution model to examine the influence of these organic compounds released by motor vehicles and fires on fine particle pollution in southern California.
Angela Buchholz, Andrew T. Lambe, Arttu Ylisirniö, Zijun Li, Olli-Pekka Tikkanen, Celia Faiola, Eetu Kari, Liqing Hao, Olli Luoma, Wei Huang, Claudia Mohr, Douglas R. Worsnop, Sergey A. Nizkorodov, Taina Yli-Juuti, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 4061–4073, https://doi.org/10.5194/acp-19-4061-2019, https://doi.org/10.5194/acp-19-4061-2019, 2019
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We studied the evaporation of α-pinene secondary organic aerosol particles in clean air to derive their volatility from the observed size changes. We found that the particles became more resilient to evaporation with increased oxidative age, possibly increasing their lifetime in the atmosphere. Also, increased relative humidity increased the particle evaporation. Mass spectrometry measurements of the particles at different stages of evaporation revealed some water-induced composition changes.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Jian Wang, John E. Shilling, Jiumeng Liu, Alla Zelenyuk, David M. Bell, Markus D. Petters, Ryan Thalman, Fan Mei, Rahul A. Zaveri, and Guangjie Zheng
Atmos. Chem. Phys., 19, 941–954, https://doi.org/10.5194/acp-19-941-2019, https://doi.org/10.5194/acp-19-941-2019, 2019
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Earlier studies showed organic hygroscopicity increases with oxidation level. Such increases have been attributed to higher water solubility for more oxidized organics. By systematically varying the water content of activating droplets, we show that for secondary organic aerosols, essentially all organics are dissolved at the point of droplet activation. Therefore, the organic hygroscopicity is not limited by solubility but is dictated mainly by the molecular weight of organic species.
Theo Kurtén, Noora Hyttinen, Emma Louise D'Ambro, Joel Thornton, and Nønne Lyng Prisle
Atmos. Chem. Phys., 18, 17589–17600, https://doi.org/10.5194/acp-18-17589-2018, https://doi.org/10.5194/acp-18-17589-2018, 2018
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We use COSMO-RS to compute saturation vapor pressures for two products of isoprene photo-oxidation and compare the results to measurements. COSMO-RS is an attractive option for calculating properties of molecules, as it is based on quantum mechanics and requires few fitting parameters. However, we show that the default implementation of this method suffers from errors related to both conformational sampling and intramolecular hydrogen bonding. We propose solutions to these problems.
Alessandro Franchin, Dorothy L. Fibiger, Lexie Goldberger, Erin E. McDuffie, Alexander Moravek, Caroline C. Womack, Erik T. Crosman, Kenneth S. Docherty, William P. Dube, Sebastian W. Hoch, Ben H. Lee, Russell Long, Jennifer G. Murphy, Joel A. Thornton, Steven S. Brown, Munkhbayar Baasandorj, and Ann M. Middlebrook
Atmos. Chem. Phys., 18, 17259–17276, https://doi.org/10.5194/acp-18-17259-2018, https://doi.org/10.5194/acp-18-17259-2018, 2018
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We present the results of aerosol and trace gas measurements from airborne and ground-based platforms. The measurements took place in January–February 2017 in northern Utah as part of the Utah Winter Fine Particulate Study (UWFPS). We characterized the chemical composition of PM1 on a regional scale, also probing the vertical dimension. We used a thermodynamic model to study the effectiveness of limiting total ammonium or total nitrate as a strategy to control aerosol concentrations.
Siegfried Schobesberger, Emma L. D'Ambro, Felipe D. Lopez-Hilfiker, Claudia Mohr, and Joel A. Thornton
Atmos. Chem. Phys., 18, 14757–14785, https://doi.org/10.5194/acp-18-14757-2018, https://doi.org/10.5194/acp-18-14757-2018, 2018
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Current mass spectrometers allow us to measure the composition of individual organic molecules in aerosol particles, as well as how they evaporate from the particles when those are slowly heated up to 200 °C. We have developed a detailed computer model to simulate the physical and chemical processes that underlie that evaporation and thus help us understand important aerosol properties. Among other factors, we discuss the roles of vapor pressures, and accretion and decomposition reactions.
Ziyue Li, Katherine A. Smith, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 14585–14608, https://doi.org/10.5194/acp-18-14585-2018, https://doi.org/10.5194/acp-18-14585-2018, 2018
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We investigated the influence of relative humidity (RH) on the heterogeneous oxidation of secondary organic aerosol (SOA) particles by OH radicals. We observed significantly faster volume loss and compositional change of SOA at high RH, showing that viscosity differences determine compositional changes, but variability in either the uptake coefficient or the fragmentation probability are required to explain the difference in volume loss between low and high RH.
Sailaja Eluri, Christopher D. Cappa, Beth Friedman, Delphine K. Farmer, and Shantanu H. Jathar
Atmos. Chem. Phys., 18, 13813–13838, https://doi.org/10.5194/acp-18-13813-2018, https://doi.org/10.5194/acp-18-13813-2018, 2018
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As oxidation flow reactors (OFRs) are increasingly used to study aerosol formation and evolution in laboratory and field environments, there is a need to develop models that can be used to interpret OFR data. In this work, we evaluate two coupled chemistry and thermodynamic models to simulate secondary organic aerosol formation (SOA) from diluted diesel exhaust and explore the sources, pathways, and processes important to SOA formation.
Chao Yan, Lubna Dada, Clémence Rose, Tuija Jokinen, Wei Nie, Siegfried Schobesberger, Heikki Junninen, Katrianne Lehtipalo, Nina Sarnela, Ulla Makkonen, Olga Garmash, Yonghong Wang, Qiaozhi Zha, Pauli Paasonen, Federico Bianchi, Mikko Sipilä, Mikael Ehn, Tuukka Petäjä, Veli-Matti Kerminen, Douglas R. Worsnop, and Markku Kulmala
Atmos. Chem. Phys., 18, 13231–13243, https://doi.org/10.5194/acp-18-13231-2018, https://doi.org/10.5194/acp-18-13231-2018, 2018
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Ions can play an important role in atmospheric new particle formation by stabilizing the embryonic clusters. Such a process is called ion-induced nucleation (IIN). We found two distinct IIN mechanisms – driven by H2SO4-NH3 clusters and by organic vapors, respectively. The concentration ratio of organic vapors to H2SO4 regulates via which pathway the IIN occur. As the organic vapor concentration is influenced by temperature, a seasonal variation in the main IIN mechanism can be expected.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Joel Brito, Samara Carbone, Igor O. Ribeiro, Glauber G. Cirino, Yingjun Liu, Ryan Thalman, Arthur Sedlacek, Aaron Funk, Courtney Schumacher, John E. Shilling, Johannes Schneider, Paulo Artaxo, Allen H. Goldstein, Rodrigo A. F. Souza, Jian Wang, Karena A. McKinney, Henrique Barbosa, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 18, 12185–12206, https://doi.org/10.5194/acp-18-12185-2018, https://doi.org/10.5194/acp-18-12185-2018, 2018
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This study aimed at understanding and quantifying the changes in mass concentration and composition of submicron airborne particulate matter (PM) in Amazonia due to urban pollution. Downwind of Manaus, PM concentrations increased by up to 200 % under polluted compared with background conditions. The observed changes included contributions from both primary and secondary processes. The differences in organic PM composition suggested a shift in the pathways of secondary production with pollution.
Sara D. Forestieri, Taylor M. Helgestad, Andrew T. Lambe, Lindsay Renbaum-Wolff, Daniel A. Lack, Paola Massoli, Eben S. Cross, Manvendra K. Dubey, Claudio Mazzoleni, Jason S. Olfert, Arthur J. Sedlacek III, Andrew Freedman, Paul Davidovits, Timothy B. Onasch, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 12141–12159, https://doi.org/10.5194/acp-18-12141-2018, https://doi.org/10.5194/acp-18-12141-2018, 2018
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We characterized optical properties of flame-derived black carbon particles and interpret our observations through the use of Mie theory and Rayleigh–Debye–Gans theory. We determined that the mass absorption coefficient is independent of particle collapse and use this to derive theory- and wavelength-specific refractive indices for black carbon (BC). We demonstrate the inadequacy of Mie theory and suggest an alternative approach for atmospheric models to better represent light absorption by BC.
Ben H. Lee, Felipe D. Lopez-Hilfiker, Emma L. D'Ambro, Putian Zhou, Michael Boy, Tuukka Petäjä, Liqing Hao, Annele Virtanen, and Joel A. Thornton
Atmos. Chem. Phys., 18, 11547–11562, https://doi.org/10.5194/acp-18-11547-2018, https://doi.org/10.5194/acp-18-11547-2018, 2018
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Molecular identities and abundances of organic compounds residing in the gas and particle phases above a Finnish boreal forest are presented. We determined that in each phase, the organic components are categorized into three subgroups based on their behavior in time. Some are more enhanced at night, others during midday, and another around sunrise. Identifying such collective behavior can potentially connect the chemical processes that evolve in time to specific distributions of products.
Sara D. Forestieri, Sean M. Staudt, Thomas M. Kuborn, Katharine Faber, Christopher R. Ruehl, Timothy H. Bertram, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 10985–11005, https://doi.org/10.5194/acp-18-10985-2018, https://doi.org/10.5194/acp-18-10985-2018, 2018
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Our work establishes how surface tension reduction influences droplet growth and activation of simple sea spray mimics (NaCl coated with fatty acids). Fatty acids can substantially reduce droplet surface tension near activation but have limited impact on activation. Coating of NaCl by palmitic acid (a wax) impedes water uptake, but this impedance is removed if oleic acid (a liquid) is mixed in. The properties that surface-active compounds need to impact activation are theoretically examined.
John E. Shilling, Mikhail S. Pekour, Edward C. Fortner, Paulo Artaxo, Suzane de Sá, John M. Hubbe, Karla M. Longo, Luiz A. T. Machado, Scot T. Martin, Stephen R. Springston, Jason Tomlinson, and Jian Wang
Atmos. Chem. Phys., 18, 10773–10797, https://doi.org/10.5194/acp-18-10773-2018, https://doi.org/10.5194/acp-18-10773-2018, 2018
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We report aircraft observations of the evolution of organic aerosol in the Manaus urban plume as it ages. We observe dynamic changes in the organic aerosol. The mean carbon oxidation state of the OA increases from −0.6 to −0.45. Hydrocarbon-like organic aerosol (HOA) mass is lost and is balanced out by formation of oxygenated organic aerosol (OOA). Because HOA loss is balanced by OOA formation, we observe little change in the net Δorg / ΔCO values with aging.
Dean B. Atkinson, Mikhail Pekour, Duli Chand, James G. Radney, Katheryn R. Kolesar, Qi Zhang, Ari Setyan, Norman T. O'Neill, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 5499–5514, https://doi.org/10.5194/acp-18-5499-2018, https://doi.org/10.5194/acp-18-5499-2018, 2018
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We use in situ measurements of particle light extinction to assess the performance of a typical aerosol remote retrieval method. The retrieved fine-mode fraction of extinction, a property commonly used to characterize the anthropogenic influence on the aerosol optical depth, compares well with the in situ measurements as does the retrieved effective fine-mode radius, which characterizes the average size of the particles that contribute most to scattering.
Nina Sarnela, Tuija Jokinen, Jonathan Duplissy, Chao Yan, Tuomo Nieminen, Mikael Ehn, Siegfried Schobesberger, Martin Heinritzi, Sebastian Ehrhart, Katrianne Lehtipalo, Jasmin Tröstl, Mario Simon, Andreas Kürten, Markus Leiminger, Michael J. Lawler, Matti P. Rissanen, Federico Bianchi, Arnaud P. Praplan, Jani Hakala, Antonio Amorim, Marc Gonin, Armin Hansel, Jasper Kirkby, Josef Dommen, Joachim Curtius, James N. Smith, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Neil M. Donahue, and Mikko Sipilä
Atmos. Chem. Phys., 18, 2363–2380, https://doi.org/10.5194/acp-18-2363-2018, https://doi.org/10.5194/acp-18-2363-2018, 2018
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Atmospheric trace gases can form small molecular clusters, which can grow to larger sizes through the condensation of vapours. This process is called new particle formation. In this paper we studied the formation of sulfuric acid and highly oxygenated molecules, the key compounds in atmospheric new particle formation, in chamber experiments and introduced a way to simulate these ozonolysis products of α-pinene in a simple manner.
Jingyi Li, Jingqiu Mao, Arlene M. Fiore, Ronald C. Cohen, John D. Crounse, Alex P. Teng, Paul O. Wennberg, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Jeff Peischl, Ilana B. Pollack, Thomas B. Ryerson, Patrick Veres, James M. Roberts, J. Andrew Neuman, John B. Nowak, Glenn M. Wolfe, Thomas F. Hanisco, Alan Fried, Hanwant B. Singh, Jack Dibb, Fabien Paulot, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2341–2361, https://doi.org/10.5194/acp-18-2341-2018, https://doi.org/10.5194/acp-18-2341-2018, 2018
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We present the first comprehensive model evaluation of summertime reactive oxidized nitrogen using a high-resolution chemistry–climate model with up-to-date isoprene oxidation chemistry, along with a series of observations from aircraft campaigns and ground measurement networks from 2004 to 2013 over the Southeast US. We investigate the impact of NOx emission reductions on changes in reactive nitrogen speciation and export efficiency as well as ozone in the past and future decade.
Alex K. Y. Lee, Chia-Li Chen, Jun Liu, Derek J. Price, Raghu Betha, Lynn M. Russell, Xiaolu Zhang, and Christopher D. Cappa
Atmos. Chem. Phys., 17, 15055–15067, https://doi.org/10.5194/acp-17-15055-2017, https://doi.org/10.5194/acp-17-15055-2017, 2017
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Understanding the mixing state of ambient black carbon (BC) and the chemical characteristics of its associated coatings is important to evaluate BC fate and environmental impacts. This study reports fresh secondary organic aerosol (SOA) formation near traffic emissions during daytime. Our observations suggest that BC was unlikely the major condensation sink of SOA, and a portion of SOA condensed on BC surface was chemically different from other SOA particles that were externally mixed with BC.
Gouri Prabhakar, Caroline L. Parworth, Xiaolu Zhang, Hwajin Kim, Dominique E. Young, Andreas J. Beyersdorf, Luke D. Ziemba, John B. Nowak, Timothy H. Bertram, Ian C. Faloona, Qi Zhang, and Christopher D. Cappa
Atmos. Chem. Phys., 17, 14747–14770, https://doi.org/10.5194/acp-17-14747-2017, https://doi.org/10.5194/acp-17-14747-2017, 2017
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This work assesses the processes that control the ambient concentrations of particulate nitrate in the the wintertime San Joaquin Valley of California through a combination of aircraft and surface measurements made during the DISCOVER-AQ study. We provide an observational demonstration of how nocturnal production and advection in aloft layers combines with daytime production and loss from entrainment and deposition to give rise to a distinct diurnal profile in surface nitrate concentrations.
Yue Zhao, Jeremy K. Chan, Felipe D. Lopez-Hilfiker, Megan A. McKeown, Emma L. D'Ambro, Jay G. Slowik, Jeffrey A. Riffell, and Joel A. Thornton
Atmos. Meas. Tech., 10, 3609–3625, https://doi.org/10.5194/amt-10-3609-2017, https://doi.org/10.5194/amt-10-3609-2017, 2017
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We present a novel atmospheric pressure electrospray chemical ionization (ESCI) source that can generate intense and stable currents of several specific reagent ions using a range of salt solutions prepared in methanol. We couple the ESCI source to a high-resolution time-of-flight mass spectrometer (HRToF-MS) and assess instrument performance through calibrations using different gas standards and measurements of organic mixtures formed by ozonolysis of α-pinene.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Matthew K. Newburn, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Ryan Thalman, Joel Brito, Samara Carbone, Paulo Artaxo, Allen H. Goldstein, Antonio O. Manzi, Rodrigo A. F. Souza, Fan Mei, John E. Shilling, Stephen R. Springston, Jian Wang, Jason D. Surratt, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 17, 6611–6629, https://doi.org/10.5194/acp-17-6611-2017, https://doi.org/10.5194/acp-17-6611-2017, 2017
Jianlin Hu, Shantanu Jathar, Hongliang Zhang, Qi Ying, Shu-Hua Chen, Christopher D. Cappa, and Michael J. Kleeman
Atmos. Chem. Phys., 17, 5379–5391, https://doi.org/10.5194/acp-17-5379-2017, https://doi.org/10.5194/acp-17-5379-2017, 2017
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Organic aerosol is a major constituent of ultrafine particulate matter (PM0.1). In this study, a source-oriented air quality model was used to simulate the concentrations and sources of primary and secondary organic aerosols in PM0.1 in California for a 9-year modeling period to provide useful information for epidemiological studies to further investigate the associations with health outcomes.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Emma L. D'Ambro, Ben H. Lee, Jiumeng Liu, John E. Shilling, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Siegfried Schobesberger, Rahul A. Zaveri, Claudia Mohr, Anna Lutz, Zhenfa Zhang, Avram Gold, Jason D. Surratt, Jean C. Rivera-Rios, Frank N. Keutsch, and Joel A. Thornton
Atmos. Chem. Phys., 17, 159–174, https://doi.org/10.5194/acp-17-159-2017, https://doi.org/10.5194/acp-17-159-2017, 2017
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We studied the formation and properties of secondary organic aerosol produced from isoprene. We find that a significant fraction (~50 %) of the mass is composed of low-volatility, highly oxidized compounds such as C5H12O6. A significant fraction of the remainder appears to be in the form of oligomeric material. Adding NOx maintained or decreased SOA yields while increasing the fraction of low-volatility material, possibly due to oligomers.
Neha Sareen, Annmarie G. Carlton, Jason D. Surratt, Avram Gold, Ben Lee, Felipe D. Lopez-Hilfiker, Claudia Mohr, Joel A. Thornton, Zhenfa Zhang, Yong B. Lim, and Barbara J. Turpin
Atmos. Chem. Phys., 16, 14409–14420, https://doi.org/10.5194/acp-16-14409-2016, https://doi.org/10.5194/acp-16-14409-2016, 2016
Michael J. Lawler, Paul M. Winkler, Jaeseok Kim, Lars Ahlm, Jasmin Tröstl, Arnaud P. Praplan, Siegfried Schobesberger, Andreas Kürten, Jasper Kirkby, Federico Bianchi, Jonathan Duplissy, Armin Hansel, Tuija Jokinen, Helmi Keskinen, Katrianne Lehtipalo, Markus Leiminger, Tuukka Petäjä, Matti Rissanen, Linda Rondo, Mario Simon, Mikko Sipilä, Christina Williamson, Daniela Wimmer, Ilona Riipinen, Annele Virtanen, and James N. Smith
Atmos. Chem. Phys., 16, 13601–13618, https://doi.org/10.5194/acp-16-13601-2016, https://doi.org/10.5194/acp-16-13601-2016, 2016
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We present chemical observations of newly formed particles as small as ~ 10 nm from new particle formation experiments using sulfuric acid, dimethylamine, ammonia, and water vapor as gas phase reactants. The nanoparticles were more acidic than expected based on thermodynamic expectations, particularly at the smallest measured sizes. The results suggest rapid surface conversion of SO2 to sulfate and show a marked composition change between 10 and 15 nm, possibly indicating a phase change.
Jiumeng Liu, Peng Lin, Alexander Laskin, Julia Laskin, Shawn M. Kathmann, Matthew Wise, Ryan Caylor, Felisha Imholt, Vanessa Selimovic, and John E. Shilling
Atmos. Chem. Phys., 16, 12815–12827, https://doi.org/10.5194/acp-16-12815-2016, https://doi.org/10.5194/acp-16-12815-2016, 2016
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Light absorbing organic aerosols (BrC) absorb sunlight thereby influencing climate; however, understanding of the link between their optical properties and environmental variables remains limited. Our chamber experiment results suggest that variables including NOx concentration, RH level, and photolysis time have considerable influence on secondary BrC optical properties. The results contribute to a more accurate characterization of the impacts of aerosols on climate, especially in urban areas.
Chao Yan, Wei Nie, Mikko Äijälä, Matti P. Rissanen, Manjula R. Canagaratna, Paola Massoli, Heikki Junninen, Tuija Jokinen, Nina Sarnela, Silja A. K. Häme, Siegfried Schobesberger, Francesco Canonaco, Lei Yao, André S. H. Prévôt, Tuukka Petäjä, Markku Kulmala, Mikko Sipilä, Douglas R. Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 16, 12715–12731, https://doi.org/10.5194/acp-16-12715-2016, https://doi.org/10.5194/acp-16-12715-2016, 2016
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Highly oxidized multifunctional compounds (HOMs) are known to have a significant contribution to secondary aerosol formation, yet their dominating formation pathways remain unclear in the atmosphere. We apply positive matrix factorization (PMF) on HOM data, and successfully retrieve factors representing different formation pathways. The results improve our understanding of HOM formation, and provide new perspectives on using PMF to study the variation of short-lived specie.
M. Dale Stokes, Grant Deane, Douglas B. Collins, Christopher Cappa, Timothy Bertram, Abigail Dommer, Steven Schill, Sara Forestieri, and Mathew Survilo
Atmos. Meas. Tech., 9, 4257–4267, https://doi.org/10.5194/amt-9-4257-2016, https://doi.org/10.5194/amt-9-4257-2016, 2016
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A small breaking wave and foam simulator has been fabricated that allows the continuous analysis of the produced marine aerosols. Based on the original Marine Aerosol Reference Tank (MART) the miniature version allows the culturing of delicate planktonic organisms because it operates without a large, sheer-inducing pump. This allows the study of marine aerosol production and the effects of biologically controlled seawater chemistry under controlled and repeatable experimental conditions.
Sara D. Forestieri, Gavin C. Cornwell, Taylor M. Helgestad, Kathryn A. Moore, Christopher Lee, Gordon A. Novak, Camille M. Sultana, Xiaofei Wang, Timothy H. Bertram, Kimberly A. Prather, and Christopher D. Cappa
Atmos. Chem. Phys., 16, 9003–9018, https://doi.org/10.5194/acp-16-9003-2016, https://doi.org/10.5194/acp-16-9003-2016, 2016
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Hygroscopic growth factors at 85 % relative humidity (GF(85 %)) were quantified along with particle composition for primary sea spray aerosol (SSA) particles generated in marine aerosol reference tanks (MARTs) from seawater in which two independent phytoplankton blooms were induced. The observed 5 to 15 % depression in the GF(85 %) values (relative to pure sea salt) is consistent with the large observed volume fractions of non-refractory organic matter (NR-OM) comprising the SSA.
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
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In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Alma Hodzic, Prasad S. Kasibhatla, Duseong S. Jo, Christopher D. Cappa, Jose L. Jimenez, Sasha Madronich, and Rokjin J. Park
Atmos. Chem. Phys., 16, 7917–7941, https://doi.org/10.5194/acp-16-7917-2016, https://doi.org/10.5194/acp-16-7917-2016, 2016
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The global budget and spatial distribution of secondary organic aerosol (SOA) are highly uncertain in chemistry-climate models, which reflects our inability to characterize all phases of the OA lifecycle. We have performed global model simulations with the newly proposed formation and removal processes (photolysis and heterogeneous chemistry) and shown that SOA is a far more dynamic system, with 4 times stronger production rates and more efficient removal mechanisms, than assumed in models.
Christopher D. Cappa, Katheryn R. Kolesar, Xiaolu Zhang, Dean B. Atkinson, Mikhail S. Pekour, Rahul A. Zaveri, Alla Zelenyuk, and Qi Zhang
Atmos. Chem. Phys., 16, 6511–6535, https://doi.org/10.5194/acp-16-6511-2016, https://doi.org/10.5194/acp-16-6511-2016, 2016
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Measurements of size-dependent aerosol optical properties at visible wavelengths made during the 2010 CARES study are reported on, with a special focus on the characterization of supermicron particles. The relationships with and dependence upon particle composition, particle size, photochemical aging, water uptake and heating are discussed, along with broader implications of these in situ measurements for the interpretation of remote sensing products.
Chun Zhao, Maoyi Huang, Jerome D. Fast, Larry K. Berg, Yun Qian, Alex Guenther, Dasa Gu, Manish Shrivastava, Ying Liu, Stacy Walters, Gabriele Pfister, Jiming Jin, John E. Shilling, and Carsten Warneke
Geosci. Model Dev., 9, 1959–1976, https://doi.org/10.5194/gmd-9-1959-2016, https://doi.org/10.5194/gmd-9-1959-2016, 2016
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In this study, the latest version of MEGAN is coupled within CLM4 in WRF-Chem. In this implementation, MEGAN shares a consistent vegetation map with CLM4. This improved modeling framework is used to investigate the impact of two land surface schemes on BVOCs and examine the sensitivity of BVOCs to vegetation distributions in California. This study indicates that more effort is needed to obtain the most appropriate and accurate land cover data sets for climate and air quality models.
Dominique E. Young, Hwajin Kim, Caroline Parworth, Shan Zhou, Xiaolu Zhang, Christopher D. Cappa, Roger Seco, Saewung Kim, and Qi Zhang
Atmos. Chem. Phys., 16, 5427–5451, https://doi.org/10.5194/acp-16-5427-2016, https://doi.org/10.5194/acp-16-5427-2016, 2016
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Aerosol chemistry and the sources and processes driving the observed temporal and diurnal variations of PM were studied in a polluted urban environment during winter 2013. These results were compared to a similar campaign from winter 2010. Meteorology strongly influenced PM composition, both directly and indirectly. Nighttime reactions played a more important role in 2013 and the influence from a nighttime formed residual layer that mixed down in the morning was also much more intense in 2013.
Felipe D. Lopez-Hilfiker, Siddarth Iyer, Claudia Mohr, Ben H. Lee, Emma L. D'Ambro, Theo Kurtén, and Joel A. Thornton
Atmos. Meas. Tech., 9, 1505–1512, https://doi.org/10.5194/amt-9-1505-2016, https://doi.org/10.5194/amt-9-1505-2016, 2016
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We present the maximum sensitivity of a TOF-CIMS using the collision limit and iodide adducts. We also present an ion adduct declustering scanning procedure which determines the effective binding energies of the detected ion adducts and therefore their approximate sensitivity. The combination of declustering scanning and the collision limit provides an approximate calibration for many compounds in the mass spectrum which would otherwise be impossible to obtain by traditional methods.
Christopher D. Cappa, Shantanu H. Jathar, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, John H. Seinfeld, and Anthony S. Wexler
Atmos. Chem. Phys., 16, 3041–3059, https://doi.org/10.5194/acp-16-3041-2016, https://doi.org/10.5194/acp-16-3041-2016, 2016
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Losses of vapors to walls of chambers can negatively bias SOA formation measurements, consequently leading to low predicted SOA concentrations in air quality models. Here, we show that accounting for such vapor losses leads to substantial increases in the predicted amount of SOA formed from VOCs and to notable increases in the O : C atomic ratio in two US regions. Comparison with a variety of observational data suggests generally improved model performance when vapor wall losses are accounted for.
G. M. Wolfe, J. Kaiser, T. F. Hanisco, F. N. Keutsch, J. A. de Gouw, J. B. Gilman, M. Graus, C. D. Hatch, J. Holloway, L. W. Horowitz, B. H. Lee, B. M. Lerner, F. Lopez-Hilifiker, J. Mao, M. R. Marvin, J. Peischl, I. B. Pollack, J. M. Roberts, T. B. Ryerson, J. A. Thornton, P. R. Veres, and C. Warneke
Atmos. Chem. Phys., 16, 2597–2610, https://doi.org/10.5194/acp-16-2597-2016, https://doi.org/10.5194/acp-16-2597-2016, 2016
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This study uses airborne trace gas observations acquired over the southeast US to examine how both natural (isoprene) and anthropogenic (NOx) emissions influence the production of formaldehyde (HCHO). We find a 3-fold increase in HCHO yield between rural and polluted environments. State-of-the-science chemical mechanisms are generally able to reproduce this behavior. These results add confidence to global hydrocarbon emission inventories constrained by spaceborne HCHO observations.
S. H. Jathar, C. D. Cappa, A. S. Wexler, J. H. Seinfeld, and M. J. Kleeman
Atmos. Chem. Phys., 16, 2309–2322, https://doi.org/10.5194/acp-16-2309-2016, https://doi.org/10.5194/acp-16-2309-2016, 2016
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Multi-generational chemistry schemes applied in regional models do not increase secondary organic aerosol (SOA) mass production relative to traditional "two-product" schemes when both models are fitted to the same chamber data. The multi-generational chemistry schemes do change the predicted composition of SOA and the source attribution of SOA.
L. Kleinman, C. Kuang, A. Sedlacek, G. Senum, S. Springston, J. Wang, Q. Zhang, J. Jayne, J. Fast, J. Hubbe, J. Shilling, and R. Zaveri
Atmos. Chem. Phys., 16, 1729–1746, https://doi.org/10.5194/acp-16-1729-2016, https://doi.org/10.5194/acp-16-1729-2016, 2016
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Atmospheric measurements of total organic aerosol (OA) and tracers of anthropogenic and biogenic emissions are used to quantify synergistic effects (A–B interactions) between two classes of precursors in the formation of OA. Regressions are consistent with the Sacramento plume composed mainly of modern carbon, and OA correlating best with an anthropogenic tracer. It is found that meteorological conditions during a pollution episode can mimic effects of A–B interactions.
T. P. Riedel, Y.-H. Lin, Z. Zhang, K. Chu, J. A. Thornton, W. Vizuete, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 16, 1245–1254, https://doi.org/10.5194/acp-16-1245-2016, https://doi.org/10.5194/acp-16-1245-2016, 2016
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IEPOX, a photooxidation product of isoprene, contributes to ambient secondary organic aerosol concentrations. Controlled atmospheric chamber experiments and modeling are used to extract formation rate information of chemical species that contribute to IEPOX-derived secondary organic aerosol.
R. J. Wild, P. M. Edwards, T. S. Bates, R. C. Cohen, J. A. de Gouw, W. P. Dubé, J. B. Gilman, J. Holloway, J. Kercher, A. R. Koss, L. Lee, B. M. Lerner, R. McLaren, P. K. Quinn, J. M. Roberts, J. Stutz, J. A. Thornton, P. R. Veres, C. Warneke, E. Williams, C. J. Young, B. Yuan, K. J. Zarzana, and S. S. Brown
Atmos. Chem. Phys., 16, 573–583, https://doi.org/10.5194/acp-16-573-2016, https://doi.org/10.5194/acp-16-573-2016, 2016
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High wintertime ozone levels have been observed in the Uintah Basin, Utah, a sparsely populated rural region with intensive oil and gas operations. The reactive nitrogen budget plays an important role in tropospheric ozone formation, and we find that nighttime chemistry has a large effect on its partitioning. Much of the oxidation of reactive nitrogen during a high-ozone year occurred via heterogeneous uptake onto aerosol at night, keeping NOx at concentrations comparable to a low-ozone year.
J. Kim, L. Ahlm, T. Yli-Juuti, M. Lawler, H. Keskinen, J. Tröstl, S. Schobesberger, J. Duplissy, A. Amorim, F. Bianchi, N. M. Donahue, R. C. Flagan, J. Hakala, M. Heinritzi, T. Jokinen, A. Kürten, A. Laaksonen, K. Lehtipalo, P. Miettinen, T. Petäjä, M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tomé, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, and A. Virtanen
Atmos. Chem. Phys., 16, 293–304, https://doi.org/10.5194/acp-16-293-2016, https://doi.org/10.5194/acp-16-293-2016, 2016
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The hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation during CLOUD7 at CERN in 2012. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles.
A. Kürten, S. Münch, L. Rondo, F. Bianchi, J. Duplissy, T. Jokinen, H. Junninen, N. Sarnela, S. Schobesberger, M. Simon, M. Sipilä, J. Almeida, A. Amorim, J. Dommen, N. M. Donahue, E. M. Dunne, R. C. Flagan, A. Franchin, J. Kirkby, A. Kupc, V. Makhmutov, T. Petäjä, A. P. Praplan, F. Riccobono, G. Steiner, A. Tomé, G. Tsagkogeorgas, P. E. Wagner, D. Wimmer, U. Baltensperger, M. Kulmala, D. R. Worsnop, and J. Curtius
Atmos. Chem. Phys., 15, 10701–10721, https://doi.org/10.5194/acp-15-10701-2015, https://doi.org/10.5194/acp-15-10701-2015, 2015
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New particle formation (NPF) is an important atmospheric process. At cold temperatures in the upper troposphere the binary (H2SO4-H2O) and ternary (H2SO4-H2O-NH3) system are thought to be important for NPF. Sulfuric acid monomer (H2SO4) and sulfuric acid dimer ((H2SO4)2) concentrations were measured between 208 and 248K for these systems and dimer evaporation rates were derived. These data will help to better understand and predict binary and ternary nucleation at low temperatures.
K. R. Kolesar, C. Chen, D. Johnson, and C. D. Cappa
Atmos. Chem. Phys., 15, 9327–9343, https://doi.org/10.5194/acp-15-9327-2015, https://doi.org/10.5194/acp-15-9327-2015, 2015
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Secondary organic aerosol from the dark ozonolysis of α‑pinene was formed at a range of mass loadings from 1 to 800μg m-3. The amount of mass loss during evaporation in a thermodenuder was found to be independent of mass loading. A kinetic model of evaporation was fit to the observations and good agreement was obtained when the particle was either composed of dimers that decompose into semi-volatile monomers or when it was composed of low-volatility compounds that evaporate directly.
S. H. Jathar, C. D. Cappa, A. S. Wexler, J. H. Seinfeld, and M. J. Kleeman
Geosci. Model Dev., 8, 2553–2567, https://doi.org/10.5194/gmd-8-2553-2015, https://doi.org/10.5194/gmd-8-2553-2015, 2015
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Multi-generational oxidation of organic vapors can significantly alter the mass, chemical composition and properties of secondary organic aerosol (SOA). Here, we implement a semi-explicit, constrained multi-generational oxidation model of Cappa and Wilson (2012) in a 3-D air quality model. When compared with results from a current-generation SOA model, we predict similar mass concentrations of SOA but a different chemical composition. O:C ratios of SOA are in line with those measured globally.
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. J. Carrasquillo, K. E. Daumit, J. F. Hunter, J. H. Kroll, D. R. Worsnop, and J. A. Thornton
Atmos. Chem. Phys., 15, 7765–7776, https://doi.org/10.5194/acp-15-7765-2015, https://doi.org/10.5194/acp-15-7765-2015, 2015
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We measured a large suite organic compounds using a recently developed Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a (HR-ToF-CIMS). The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We find that approximately 50% of the detected particle phase mass is associated with compounds having effective vapor pressures 4, or more, orders of magnitude lower than commonly measured products.
A. Franchin, S. Ehrhart, J. Leppä, T. Nieminen, S. Gagné, S. Schobesberger, D. Wimmer, J. Duplissy, F. Riccobono, E. M. Dunne, L. Rondo, A. Downard, F. Bianchi, A. Kupc, G. Tsagkogeorgas, K. Lehtipalo, H. E. Manninen, J. Almeida, A. Amorim, P. E. Wagner, A. Hansel, J. Kirkby, A. Kürten, N. M. Donahue, V. Makhmutov, S. Mathot, A. Metzger, T. Petäjä, R. Schnitzhofer, M. Sipilä, Y. Stozhkov, A. Tomé, V.-M. Kerminen, K. Carslaw, J. Curtius, U. Baltensperger, and M. Kulmala
Atmos. Chem. Phys., 15, 7203–7216, https://doi.org/10.5194/acp-15-7203-2015, https://doi.org/10.5194/acp-15-7203-2015, 2015
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The ion-ion recombination coefficient was measured at different temperatures, relative humidities and concentrations of ozone and sulfur dioxide. The experiments were carried out using the CLOUD chamber at CERN.
We observed a strong dependency on temperature and on relative humidity, which has not been reported previously. No dependency of the ion-ion recombination coefficient on ozone concentration was observed and a weak variation with sulfur dioxide concentration was also observed.
D. B. Millet, M. Baasandorj, D. K. Farmer, J. A. Thornton, K. Baumann, P. Brophy, S. Chaliyakunnel, J. A. de Gouw, M. Graus, L. Hu, A. Koss, B. H. Lee, F. D. Lopez-Hilfiker, J. A. Neuman, F. Paulot, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, B. J. Williams, and J. Xu
Atmos. Chem. Phys., 15, 6283–6304, https://doi.org/10.5194/acp-15-6283-2015, https://doi.org/10.5194/acp-15-6283-2015, 2015
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Formic acid (HCOOH) is an abundant atmospheric acid that affects precipitation chemistry and acidity. HCOOH measurements over the USA are 2-3× larger than can be explained by known sources and sinks, revealing a key gap in current understanding. Observations indicate a large biogenic source plus chemical production across a range of precursors. Model simulations cannot capture the HCOOH diurnal amplitude or nocturnal profile, implying a deposition bias and possibly even larger missing source.
A. P. Praplan, S. Schobesberger, F. Bianchi, M. P. Rissanen, M. Ehn, T. Jokinen, H. Junninen, A. Adamov, A. Amorim, J. Dommen, J. Duplissy, J. Hakala, A. Hansel, M. Heinritzi, J. Kangasluoma, J. Kirkby, M. Krapf, A. Kürten, K. Lehtipalo, F. Riccobono, L. Rondo, N. Sarnela, M. Simon, A. Tomé, J. Tröstl, P. M. Winkler, C. Williamson, P. Ye, J. Curtius, U. Baltensperger, N. M. Donahue, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 4145–4159, https://doi.org/10.5194/acp-15-4145-2015, https://doi.org/10.5194/acp-15-4145-2015, 2015
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Our study shows, based on data from three atmospheric pressure interface time-of-flight mass spectrometers measuring in parallel charged and neutral molecules and molecular clusters, how oxidised organic compounds bind to inorganic ions (e.g. bisulfate, nitrate, ammonium). This ionisation is selective for compounds with lower molar mass due to their limited amount and variety of functional groups. We also found that extremely low volatile organic compounds (ELVOCs) can be formed immediately.
D. B. Atkinson, J. G. Radney, J. Lum, K. R. Kolesar, D. J. Cziczo, M. S. Pekour, Q. Zhang, A. Setyan, A. Zelenyuk, and C. D. Cappa
Atmos. Chem. Phys., 15, 4045–4061, https://doi.org/10.5194/acp-15-4045-2015, https://doi.org/10.5194/acp-15-4045-2015, 2015
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This work describes an analysis of measurements of the influence of water uptake on the light-scattering properties of sub- and supermicron-sized particles as observed in the Sacramento, CA, USA region during the 2010 CARES field campaign. The observations are used to derive campaign-average effective hygroscopicity parameters for submicron oxygenated organic aerosol and for supermicron particles, and the influence of chloride displacement reactions on particle hygroscopicity is examined.
S. Schobesberger, A. Franchin, F. Bianchi, L. Rondo, J. Duplissy, A. Kürten, I. K. Ortega, A. Metzger, R. Schnitzhofer, J. Almeida, A. Amorim, J. Dommen, E. M. Dunne, M. Ehn, S. Gagné, L. Ickes, H. Junninen, A. Hansel, V.-M. Kerminen, J. Kirkby, A. Kupc, A. Laaksonen, K. Lehtipalo, S. Mathot, A. Onnela, T. Petäjä, F. Riccobono, F. D. Santos, M. Sipilä, A. Tomé, G. Tsagkogeorgas, Y. Viisanen, P. E. Wagner, D. Wimmer, J. Curtius, N. M. Donahue, U. Baltensperger, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 55–78, https://doi.org/10.5194/acp-15-55-2015, https://doi.org/10.5194/acp-15-55-2015, 2015
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We used an ion mass spectrometer at CERN's CLOUD chamber to investigate the detailed composition of ammonia--sulfuric acid ion clusters (of both polarities) as they initially form and then grow into aerosol particles, at atmospherically relevant conditions. We found that these clusters’ composition is mainly determined by the ratio of the precursor vapors and ranges from ammonia-free clusters to clusters containing > 1 ammonia per sulfuric acid. Acid--base bindings are a key formation mechanism.
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
L. Rondo, A. Kürten, S. Ehrhart, S. Schobesberger, A. Franchin, H. Junninen, T. Petäjä, M. Sipilä, D. R. Worsnop, and J. Curtius
Atmos. Meas. Tech., 7, 3849–3859, https://doi.org/10.5194/amt-7-3849-2014, https://doi.org/10.5194/amt-7-3849-2014, 2014
J. Kukkonen, J. Nikmo, M. Sofiev, K. Riikonen, T. Petäjä, A. Virkkula, J. Levula, S. Schobesberger, and D. M. Webber
Geosci. Model Dev., 7, 2663–2681, https://doi.org/10.5194/gmd-7-2663-2014, https://doi.org/10.5194/gmd-7-2663-2014, 2014
E. Kassianov, J. Barnard, M. Pekour, L. K. Berg, J. Shilling, C. Flynn, F. Mei, and A. Jefferson
Atmos. Meas. Tech., 7, 3247–3261, https://doi.org/10.5194/amt-7-3247-2014, https://doi.org/10.5194/amt-7-3247-2014, 2014
J. D. Fast, J. Allan, R. Bahreini, J. Craven, L. Emmons, R. Ferrare, P. L. Hayes, A. Hodzic, J. Holloway, C. Hostetler, J. L. Jimenez, H. Jonsson, S. Liu, Y. Liu, A. Metcalf, A. Middlebrook, J. Nowak, M. Pekour, A. Perring, L. Russell, A. Sedlacek, J. Seinfeld, A. Setyan, J. Shilling, M. Shrivastava, S. Springston, C. Song, R. Subramanian, J. W. Taylor, V. Vinoj, Q. Yang, R. A. Zaveri, and Q. Zhang
Atmos. Chem. Phys., 14, 10013–10060, https://doi.org/10.5194/acp-14-10013-2014, https://doi.org/10.5194/acp-14-10013-2014, 2014
A. Setyan, C. Song, M. Merkel, W. B. Knighton, T. B. Onasch, M. R. Canagaratna, D. R. Worsnop, A. Wiedensohler, J. E. Shilling, and Q. Zhang
Atmos. Chem. Phys., 14, 6477–6494, https://doi.org/10.5194/acp-14-6477-2014, https://doi.org/10.5194/acp-14-6477-2014, 2014
C. J. Gaston, J. A. Thornton, and N. L. Ng
Atmos. Chem. Phys., 14, 5693–5707, https://doi.org/10.5194/acp-14-5693-2014, https://doi.org/10.5194/acp-14-5693-2014, 2014
R. A. Zaveri, R. C. Easter, J. E. Shilling, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 5153–5181, https://doi.org/10.5194/acp-14-5153-2014, https://doi.org/10.5194/acp-14-5153-2014, 2014
A. Virkkula, J. Levula, T. Pohja, P. P. Aalto, P. Keronen, S. Schobesberger, C. B. Clements, L. Pirjola, A.-J. Kieloaho, L. Kulmala, H. Aaltonen, J. Patokoski, J. Pumpanen, J. Rinne, T. Ruuskanen, M. Pihlatie, H. E. Manninen, V. Aaltonen, H. Junninen, T. Petäjä, J. Backman, M. Dal Maso, T. Nieminen, T. Olsson, T. Grönholm, J. Aalto, T. H. Virtanen, M. Kajos, V.-M. Kerminen, D. M. Schultz, J. Kukkonen, M. Sofiev, G. De Leeuw, J. Bäck, P. Hari, and M. Kulmala
Atmos. Chem. Phys., 14, 4473–4502, https://doi.org/10.5194/acp-14-4473-2014, https://doi.org/10.5194/acp-14-4473-2014, 2014
S. Bleicher, J. C. Buxmann, R. Sander, T. P. Riedel, J. A. Thornton, U. Platt, and C. Zetzsch
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-10135-2014, https://doi.org/10.5194/acpd-14-10135-2014, 2014
Revised manuscript has not been submitted
T. P. Riedel, G. M. Wolfe, K. T. Danas, J. B. Gilman, W. C. Kuster, D. M. Bon, A. Vlasenko, S.-M. Li, E. J. Williams, B. M. Lerner, P. R. Veres, J. M. Roberts, J. S. Holloway, B. Lefer, S. S. Brown, and J. A. Thornton
Atmos. Chem. Phys., 14, 3789–3800, https://doi.org/10.5194/acp-14-3789-2014, https://doi.org/10.5194/acp-14-3789-2014, 2014
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. Lutz, M. Hallquist, D. Worsnop, and J. A. Thornton
Atmos. Meas. Tech., 7, 983–1001, https://doi.org/10.5194/amt-7-983-2014, https://doi.org/10.5194/amt-7-983-2014, 2014
S. E. Pusede, D. R. Gentner, P. J. Wooldridge, E. C. Browne, A. W. Rollins, K.-E. Min, A. R. Russell, J. Thomas, L. Zhang, W. H. Brune, S. B. Henry, J. P. DiGangi, F. N. Keutsch, S. A. Harrold, J. A. Thornton, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, J. Sanders, X. Ren, T. C. VandenBoer, M. Z. Markovic, A. Guha, R. Weber, A. H. Goldstein, and R. C. Cohen
Atmos. Chem. Phys., 14, 3373–3395, https://doi.org/10.5194/acp-14-3373-2014, https://doi.org/10.5194/acp-14-3373-2014, 2014
G. M. Buffaloe, D. A. Lack, E. J. Williams, D. Coffman, K. L. Hayden, B. M. Lerner, S.-M. Li, I. Nuaaman, P. Massoli, T. B. Onasch, P. K. Quinn, and C. D. Cappa
Atmos. Chem. Phys., 14, 1881–1896, https://doi.org/10.5194/acp-14-1881-2014, https://doi.org/10.5194/acp-14-1881-2014, 2014
R. L. N. Yatavelli, H. Stark, S. L. Thompson, J. R. Kimmel, M. J. Cubison, D. A. Day, P. Campuzano-Jost, B. B. Palm, A. Hodzic, J. A. Thornton, J. T. Jayne, D. R. Worsnop, and J. L. Jimenez
Atmos. Chem. Phys., 14, 1527–1546, https://doi.org/10.5194/acp-14-1527-2014, https://doi.org/10.5194/acp-14-1527-2014, 2014
C. D. Cappa, E. J. Williams, D. A. Lack, G. M. Buffaloe, D. Coffman, K. L. Hayden, S. C. Herndon, B. M. Lerner, S.-M. Li, P. Massoli, R. McLaren, I. Nuaaman, T. B. Onasch, and P. K. Quinn
Atmos. Chem. Phys., 14, 1337–1352, https://doi.org/10.5194/acp-14-1337-2014, https://doi.org/10.5194/acp-14-1337-2014, 2014
B. Friedman, A. Zelenyuk, J. Beranek, G. Kulkarni, M. Pekour, A. Gannet Hallar, I. B. McCubbin, J. A. Thornton, and D. J Cziczo
Atmos. Chem. Phys., 13, 11839–11851, https://doi.org/10.5194/acp-13-11839-2013, https://doi.org/10.5194/acp-13-11839-2013, 2013
P. M. Edwards, C. J. Young, K. Aikin, J. deGouw, W. P. Dubé, F. Geiger, J. Gilman, D. Helmig, J. S. Holloway, J. Kercher, B. Lerner, R. Martin, R. McLaren, D. D. Parrish, J. Peischl, J. M. Roberts, T. B. Ryerson, J. Thornton, C. Warneke, E. J. Williams, and S. S. Brown
Atmos. Chem. Phys., 13, 8955–8971, https://doi.org/10.5194/acp-13-8955-2013, https://doi.org/10.5194/acp-13-8955-2013, 2013
H. Keskinen, A. Virtanen, J. Joutsensaari, G. Tsagkogeorgas, J. Duplissy, S. Schobesberger, M. Gysel, F. Riccobono, J. G. Slowik, F. Bianchi, T. Yli-Juuti, K. Lehtipalo, L. Rondo, M. Breitenlechner, A. Kupc, J. Almeida, A. Amorim, E. M. Dunne, A. J. Downard, S. Ehrhart, A. Franchin, M.K. Kajos, J. Kirkby, A. Kürten, T. Nieminen, V. Makhmutov, S. Mathot, P. Miettinen, A. Onnela, T. Petäjä, A. Praplan, F. D. Santos, S. Schallhart, M. Sipilä, Y. Stozhkov, A. Tomé, P. Vaattovaara, D. Wimmer, A. Prevot, J. Dommen, N. M. Donahue, R.C. Flagan, E. Weingartner, Y. Viisanen, I. Riipinen, A. Hansel, J. Curtius, M. Kulmala, D. R. Worsnop, U. Baltensperger, H. Wex, F. Stratmann, and A. Laaksonen
Atmos. Chem. Phys., 13, 5587–5600, https://doi.org/10.5194/acp-13-5587-2013, https://doi.org/10.5194/acp-13-5587-2013, 2013
J. E. Shilling, R. A. Zaveri, J. D. Fast, L. Kleinman, M. L. Alexander, M. R. Canagaratna, E. Fortner, J. M. Hubbe, J. T. Jayne, A. Sedlacek, A. Setyan, S. Springston, D. R. Worsnop, and Q. Zhang
Atmos. Chem. Phys., 13, 2091–2113, https://doi.org/10.5194/acp-13-2091-2013, https://doi.org/10.5194/acp-13-2091-2013, 2013
C. D. Cappa, X. Zhang, C. L. Loza, J. S. Craven, L. D. Yee, and J. H. Seinfeld
Atmos. Chem. Phys., 13, 1591–1606, https://doi.org/10.5194/acp-13-1591-2013, https://doi.org/10.5194/acp-13-1591-2013, 2013
J. S. Craven, L. D. Yee, N. L. Ng, M. R. Canagaratna, C. L. Loza, K. A. Schilling, R. L. N. Yatavelli, J. A. Thornton, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 12, 11795–11817, https://doi.org/10.5194/acp-12-11795-2012, https://doi.org/10.5194/acp-12-11795-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Molecular understanding of the suppression of new-particle formation by isoprene
Complex plant-derived organic aerosol as ice-nucleating particles – more than the sums of their parts?
Liquid–liquid phase separation and morphologies in organic particles consisting of α-pinene and β-caryophyllene ozonolysis products and mixtures with commercially available organic compounds
Oligomer and highly oxygenated organic molecule formation from oxidation of oxygenated monoterpenes emitted by California sage plants
Laboratory studies of fresh and aged biomass burning aerosol emitted from east African biomass fuels – Part 2: Chemical properties and characterization
Impact of NOx on secondary organic aerosol (SOA) formation from α-pinene and β-pinene photooxidation: the role of highly oxygenated organic nitrates
Evaluation of the chemical composition of gas- and particle-phase products of aromatic oxidation
Glyoxal's impact on dry ammonium salts: fast and reversible surface aerosol browning
Oxygenated products formed from OH-initiated reactions of trimethylbenzene: autoxidation and accretion
Chemical composition and light absorption of carbonaceous aerosols emitted from crop residue burning: Influence of combustion efficiency
Biomass-burning-derived particles from a wide variety of fuels – Part 2: Effects of photochemical aging on particle optical and chemical properties
Measured solid state and subcooled liquid vapour pressures of nitroaromatics using Knudsen effusion mass spectrometry
Polar semivolatile organic compounds in biomass-burning emissions and their chemical transformations during aging in an oxidation flow reactor
Temperature effects on optical properties and chemical composition of secondary organic aerosol derived from n-dodecane
An investigation on hygroscopic properties of 15 black carbon (BC)-containing particles from different carbon sources: roles of organic and inorganic components
Deconvolution of FIGAERO–CIMS thermal desorption profiles using positive matrix factorisation to identify chemical and physical processes during particle evaporation
Mineralogy and geochemistry of Asian dust: dependence on migration path, fractionation, and reactions with polluted air
Chemical composition, structures, and light absorption of N-containing aromatic compounds emitted from burning wood and charcoal in household cookstoves
Secondary Organic Aerosol Yields from the Oxidation of Benzyl Alcohol
Photochemical transformation of residential wood combustion emissions: dependence of organic aerosol composition on OH exposure
Hygroscopic behavior of aerosols generated from solutions of 3-methyl-1,2,3-butanetricarboxylic acid, its sodium salts, and its mixtures with NaCl
Seawater analysis by ambient mass-spectrometry-based seaomics
Distinct chemical and mineralogical composition of Icelandic dust compared to North African and Asian dust
Molecular composition and photochemical evolution of water-soluble organic carbon (WSOC) extracted from field biomass burning aerosols using high-resolution mass spectrometry
Heterogeneous oxidation of amorphous organic aerosol surrogates by O3, NO3, and OH at typical tropospheric temperatures
On mineral dust aerosol hygroscopicity
Direct contribution of ammonia to CCN-size alpha-pinene secondary organic aerosol formation
High levels of primary biogenic organic aerosols are driven by only a few plant-associated microbial taxa
Formation of highly oxygenated organic molecules from chlorine-atom-initiated oxidation of alpha-pinene
The evolutionary behavior of chromophoric brown carbon during ozone aging of fine particles from biomass burning
Technical note: Preparation and purification of atmospherically relevant α-hydroxynitrate esters of monoterpenes
Effect of inorganic-to-organic mass ratio on the heterogeneous OH reaction rates of erythritol: implications for atmospheric chemical stability of 2-methyltetrols
Ambient air quality in the Kathmandu Valley, Nepal, during the pre-monsoon: concentrations and sources of particulate matter and trace gases
Morphology and size of the particles emitted from a gasoline-direct-injection-engine vehicle and their ageing in an environmental chamber
The Aarhus Chamber Campaign on Highly Oxidized Multifunctional Organic Molecules and Aerosols (ACCHA): Particle Formation and Detailed Chemical Composition at Different Temperatures
Biomass-burning-derived particles from a wide variety of fuels – Part 1: Properties of primary particles
Molecular composition and photochemical lifetimes of brown carbon chromophores in biomass burning organic aerosol
Cloud history can change water–ice–surface interactions of oxide mineral aerosols: a case study on silica
Relationship between the molecular composition, visible light absorption, and health-related properties of smoldering woodsmoke aerosols
Impact of isolated atmospheric aging processes on the cloud condensation nuclei activation of soot particles
Secondary organic aerosol formation from OH-initiated oxidation of m-xylene: effects of relative humidity on yield and chemical composition
A study of volatility by composition, heating, and dilution measurements of secondary organic aerosol from 1,3,5-trimethylbenzene
Effects of NO2 and C3H6 on the heterogeneous oxidation of SO2 on TiO2 in the presence or absence of UV–Vis irradiation
Single-particle experiments measuring humidity and inorganic salt effects on gas-particle partitioning of butenedial
Gaseous, PM2.5 mass, and speciated emission factors from laboratory chamber peat combustion
Molecular characterization of polar organic aerosol constituents in off-road engine emissions using Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS): implications for source apportionment
Secondary organic aerosol formation from the laboratory oxidation of biomass burning emissions
Chemical composition and hydrolysis of organic nitrate aerosol formed from hydroxyl and nitrate radical oxidation of α-pinene and β-pinene
A review of experimental techniques for aerosol hygroscopicity studies
Enhanced heterogeneous uptake of sulfur dioxide on mineral particles through modification of iron speciation during simulated cloud processing
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Isabelle Steinke, Naruki Hiranuma, Roger Funk, Kristina Höhler, Nadine Tüllmann, Nsikanabasi Silas Umo, Peter G. Weidler, Ottmar Möhler, and Thomas Leisner
Atmos. Chem. Phys., 20, 11387–11397, https://doi.org/10.5194/acp-20-11387-2020, https://doi.org/10.5194/acp-20-11387-2020, 2020
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In this study, we highlight the potential impact of particles from certain terrestrial sources on the formation of ice crystals in clouds. In particular, we focus on biogenic particles consisting of various organic compounds, which makes it very difficult to predict the ice nucleation properties of complex ambient particles. We find that these ambient particles are often more ice active than individual components.
Young-Chul Song, Ariana G. Bé, Scot T. Martin, Franz M. Geiger, Allan K. Bertram, Regan J. Thomson, and Mijung Song
Atmos. Chem. Phys., 20, 11263–11273, https://doi.org/10.5194/acp-20-11263-2020, https://doi.org/10.5194/acp-20-11263-2020, 2020
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We report the liquid–liquid phase separation (LLPS) of organic aerosol consisting of α-pinene- and β-caryophyllene-derived ozonolysis products and commercial organic compounds. As compositional complexity increased from one to two organic species, LLPS occurred over a wider range of average O : C values (increasing from 0.44 to 0.67). These results provide further evidence that LLPS is likely frequent in organic aerosol particles in the troposphere, even in the absence of inorganic salt.
Archit Mehra, Jordan E. Krechmer, Andrew Lambe, Chinmoy Sarkar, Leah Williams, Farzaneh Khalaj, Alex Guenther, John Jayne, Hugh Coe, Douglas Worsnop, Celia Faiola, and Manjula Canagaratna
Atmos. Chem. Phys., 20, 10953–10965, https://doi.org/10.5194/acp-20-10953-2020, https://doi.org/10.5194/acp-20-10953-2020, 2020
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Emissions of volatile organic compounds (VOCs) from plants are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Real plant emissions are much more diverse than the few proxies widely used for studies of plant SOA. Here we present the first study of SOA from Californian sage plants and the oxygenated monoterpenes representing their major emissions. We identify SOA products and show the importance of the formation of highly oxygenated organic molecules and oligomers.
Damon M. Smith, Tianqu Cui, Marc N. Fiddler, Rudra P. Pokhrel, Jason D. Surratt, and Solomon Bililign
Atmos. Chem. Phys., 20, 10169–10191, https://doi.org/10.5194/acp-20-10169-2020, https://doi.org/10.5194/acp-20-10169-2020, 2020
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Biomass fuels used for domestic purposes in east Africa produce a significant atmospheric burden of aerosols and volatile organic compounds. The chemical properties and composition of these aerosols have not been investigated in the laboratory. In this work methanol extracts from filter samples of aerosol collected from an indoor smog chamber were analyzed to determine the chemical composition and identify the light absorption properties of organic aerosol constituents.
Iida Pullinen, Sebastian Schmitt, Sungah Kang, Mehrnaz Sarrafzadeh, Patrick Schlag, Stefanie Andres, Einhard Kleist, Thomas F. Mentel, Franz Rohrer, Monika Springer, Ralf Tillmann, Jürgen Wildt, Cheng Wu, Defeng Zhao, Andreas Wahner, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 20, 10125–10147, https://doi.org/10.5194/acp-20-10125-2020, https://doi.org/10.5194/acp-20-10125-2020, 2020
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Biogenic and anthropogenic air masses mix in the atmosphere, bringing plant-emitted monoterpenes and traffic-related nitrogen oxides together. There is debate whether the presence of nitrogen oxides reduces or increases secondary aerosol formation. This is important as secondary aerosols have cooling effects in the climate system but also constitute a health risk in populated areas. We show that the presence of NOx alone should not much affect the mass yields of secondary organic aerosols.
Archit Mehra, Yuwei Wang, Jordan E. Krechmer, Andrew Lambe, Francesca Majluf, Melissa A. Morris, Michael Priestley, Thomas J. Bannan, Daniel J. Bryant, Kelly L. Pereira, Jacqueline F. Hamilton, Andrew R. Rickard, Mike J. Newland, Harald Stark, Philip Croteau, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, Lin Wang, and Hugh Coe
Atmos. Chem. Phys., 20, 9783–9803, https://doi.org/10.5194/acp-20-9783-2020, https://doi.org/10.5194/acp-20-9783-2020, 2020
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Aromatic volatile organic compounds (VOCs) emitted from anthropogenic activity are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Here we present a detailed chemical characterisation of SOA from four C9-aromatic isomers and a polycyclic aromatic hydrocarbon (PAH). We identify and compare their oxidation products in the gas and particle phases, showing the different relative importance of oxidation pathways and proportions of highly oxygenated organic molecules.
David O. De Haan, Lelia N. Hawkins, Kevin Jansen, Hannah G. Welsh, Raunak Pednekar, Alexia de Loera, Natalie G. Jimenez, Margaret A. Tolbert, Mathieu Cazaunau, Aline Gratien, Antonin Bergé, Edouard Pangui, Paola Formenti, and Jean-François Doussin
Atmos. Chem. Phys., 20, 9581–9590, https://doi.org/10.5194/acp-20-9581-2020, https://doi.org/10.5194/acp-20-9581-2020, 2020
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When exposed to glyoxal in chamber experiments, dry ammonium or methylammonium sulfate particles turn brown immediately and reversibly without increasing in size. Much less browning was observed on wet aerosol particles, and no browning was observed with sodium sulfate aerosol. While estimated dry aerosol light absorption caused by background glyoxal (70 ppt) is insignificant compared to that of secondary brown carbon overall, in polluted regions this process could be a source of brown carbon.
Yuwei Wang, Archit Mehra, Jordan E. Krechmer, Gan Yang, Xiaoyu Hu, Yiqun Lu, Andrew Lambe, Manjula Canagaratna, Jianmin Chen, Douglas Worsnop, Hugh Coe, and Lin Wang
Atmos. Chem. Phys., 20, 9563–9579, https://doi.org/10.5194/acp-20-9563-2020, https://doi.org/10.5194/acp-20-9563-2020, 2020
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A series of OH-initiated oxidation experiments of trimethylbenzene were investigated in the absence and presence of NOx. Many C9 products with 1–11 oxygen atoms and C18 products presumably formed from dimerization of C9 peroxy radicals were observed, hinting at the extensive existence of autoxidation and accretion reaction pathways. The presence of NOx would suppress the formation of highly oxygenated C18 molecules and enhance the formation of organonitrates and even dinitrate compounds.
Yujue Wang, Min Hu, Nan Xu, Yanhong Qin, Zhijun Wu, Liwu Zeng, Xiaofeng Huang, and Lingyan He
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-676, https://doi.org/10.5194/acp-2020-676, 2020
Revised manuscript accepted for ACP
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Field straw residue burning is a widespread type of biomass burning in Asia, while its emissions are poorly understood. In this study, we designed lab-controlled experiments to comprehensively investigate the emission factors, chemical compositions and light absorption properties of both water-soluble and water-insoluble carbonaceous aerosols emitted from straw burning. The results clearly highlight the significant influences of burning conditions and combustion efficiency on the emissions.
Christopher D. Cappa, Christopher Y. Lim, David H. Hagan, Matthew Coggon, Abigail Koss, Kanako Sekimoto, Joost de Gouw, Timothy B. Onasch, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 8511–8532, https://doi.org/10.5194/acp-20-8511-2020, https://doi.org/10.5194/acp-20-8511-2020, 2020
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Smoke from combustion of a wide range of biomass fuels (e.g., leaves, twigs, logs, peat, and dung) was photochemically aged in a small chamber for up to 8 d of equivalent atmospheric aging. Upon aging, the particle chemical composition and ability to absorb sunlight changed owing to reactions in both the gas and particulate phases. We developed a model to explain the observations and used this to derive insights into the aging of smoke in the atmosphere.
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.
Deep Sengupta, Vera Samburova, Chiranjivi Bhattarai, Adam C. Watts, Hans Moosmüller, and Andrey Y. Khlystov
Atmos. Chem. Phys., 20, 8227–8250, https://doi.org/10.5194/acp-20-8227-2020, https://doi.org/10.5194/acp-20-8227-2020, 2020
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This paper presents important results on the atmospheric chemistry of combustion emissions. Organic compounds from these emissions can contribute significantly to chemical and physical properties of atmospheric aerosols. In this paper, a detailed chemical analysis of gas- and particle-phase polar organic compounds from the laboratory combustion of globally important fuels is presented. The aging experiments were performed to understand the fate of biomass-burning organics in the atmosphere.
Junling Li, Weigang Wang, Kun Li, Wenyu Zhang, Chao Peng, Li Zhou, Bo Shi, Yan Chen, Mingyuan Liu, Hong Li, and Maofa Ge
Atmos. Chem. Phys., 20, 8123–8137, https://doi.org/10.5194/acp-20-8123-2020, https://doi.org/10.5194/acp-20-8123-2020, 2020
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Long-chain alkanes (a large fraction of diesel fuel and its exhaust) are important potential contributors of SOA. Through the analysis of the components of formed SOA, we found that low-temperature conditions promote the oligomerization of n-dodecane, and the degree of oligomerization can reach tetramerization. The presence of the oligomers enhances the light extinction of the particles. UV-scattering particles in the boundary layer can accelerate photochemical reactions and haze production.
Minli Wang, Yiqun Chen, Heyun Fu, Xiaolei Qu, Bengang Li, Shu Tao, and Dongqiang Zhu
Atmos. Chem. Phys., 20, 7941–7954, https://doi.org/10.5194/acp-20-7941-2020, https://doi.org/10.5194/acp-20-7941-2020, 2020
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The mechanism and factors controlling the hygroscopicity of black-carbon-containing particles (BCPs) from different carbon sources are not well understood. We thoroughly characterized the chemical and compositional properties of 15 samples of BCPs from different sources (wood, herb, and soot) and further investigated their hygroscopicity. Depending on the carbon source, organic carbon and dissolved mineral contents were key determinants of the equilibrium and kinetics of water uptake by BCPs.
Angela Buchholz, Arttu Ylisirniö, Wei Huang, Claudia Mohr, Manjula Canagaratna, Douglas R. Worsnop, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 20, 7693–7716, https://doi.org/10.5194/acp-20-7693-2020, https://doi.org/10.5194/acp-20-7693-2020, 2020
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To understand the role of aerosol particles in the atmosphere, it is necessary to know their detailed chemical composition and physical properties, especially volatility. The thermal desorption data from FIGAERO–CIMS provides both but are difficult to analyse. With positive matrix factorisation, we can separate instrument background from the real signal. Compounds can be classified by their apparent volatility, and the contribution of thermal decomposition in the instrument can be identified.
Gi Young Jeong
Atmos. Chem. Phys., 20, 7411–7428, https://doi.org/10.5194/acp-20-7411-2020, https://doi.org/10.5194/acp-20-7411-2020, 2020
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During long-range transport, mineral dust interacts with the atmosphere, biosphere, cryosphere, and pedosphere, influencing ecosystems, the atmospheric energy balance, and air quality. This study analyzed the mineral and chemical compositions of Asian dust samples collected during 14 years in Korea. The result showed mineralogical and geochemical variation depending on the dust migration path, fractionation, and atmospheric reactions as well as average properties.
Mingjie Xie, Zhenzhen Zhao, Amara L. Holder, Michael D. Hays, Xie Chen, Guofeng Shen, James J. Jetter, and Qin'geng Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-594, https://doi.org/10.5194/acp-2020-594, 2020
Revised manuscript accepted for ACP
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This study investigated the composition, structures, and light absorption of N-containing aromatic compounds (NACs) in PM2.5 emitted from burning red oak and charcoal in a variety of cookstoves. The results suggest that the identified NACs might have substantial fractions remaining in the gas-phase. In comparison to other sources, cookstove emissions from red oak or charcoal fuels did not exhibit unique NAC structural features, but had distinct NACs composition.
Sophia M. Charan, Reina S. Buenconsejo, and John H. Seinfeld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-492, https://doi.org/10.5194/acp-2020-492, 2020
Revised manuscript accepted for ACP
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In urban areas, the emissions from volatile chemical products may be responsible for the formation of as much particulate matter as motor vehicles. Since exposure to particulate matter is a public health crisis, understanding its formation is critical. In this work we investigate the secondary organic aerosol formation potential of benzyl alcohol, an important compound that is representative of some of these new emission sources, and find that more particulate matter forms than is expected.
Anni Hartikainen, Petri Tiitta, Mika Ihalainen, Pasi Yli-Pirilä, Jürgen Orasche, Hendryk Czech, Miika Kortelainen, Heikki Lamberg, Heikki Suhonen, Hanna Koponen, Liqing Hao, Ralf Zimmermann, Jorma Jokiniemi, Jarkko Tissari, and Olli Sippula
Atmos. Chem. Phys., 20, 6357–6378, https://doi.org/10.5194/acp-20-6357-2020, https://doi.org/10.5194/acp-20-6357-2020, 2020
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Residential wood combustion emits large amounts of organic compounds, which are transformed in the atmosphere via photochemical ageing reactions. We assessed this organic emission at various stages of exposure with an oxidation flow reactor. Ageing led to major changes in both gaseous and particulate phases including increased acidic compounds and transformation of the polycyclic aromatic compounds. Such changes have serious implications for the health- and climate-related effects of combustion.
Li Wu, Clara Becote, Sophie Sobanska, Pierre-Marie Flaud, Emilie Perraudin, Eric Villenave, Young-Chul Song, and Chul-Un Ro
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-428, https://doi.org/10.5194/acp-2020-428, 2020
Revised manuscript accepted for ACP
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3-methyl-1,2,3-butanetricarboxylic acid (MBTCA), a second-generation product of monoterpenes, is one of the most relevant tracer compounds for biogenic SOAs. Laboratory-generated, micrometer-sized, pure MBTCA, mono-/di-/tri-sodium MBTCA salts, and MBTCA-NaCl mixture aerosol particles were examined systematically to observe their hygroscopic behavior and it was also observed that the monosodium MBTCA salt aerosols were formed through a reaction between MBTCA and NaCl.
Nicolás Zabalegui, Malena Manzi, Antoine Depoorter, Nathalie Hayeck, Marie Roveretto, Chunlin Li, Manuela van Pinxteren, Hartmut Herrmann, Christian George, and María Eugenia Monge
Atmos. Chem. Phys., 20, 6243–6257, https://doi.org/10.5194/acp-20-6243-2020, https://doi.org/10.5194/acp-20-6243-2020, 2020
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A new approach to bridging different fields of science by studying the air–sea interface is described. An untargeted ambient mass-spectrometry-based metabolomics method enables the study of enriched organic compounds found on the sea surface for air–water transfer processes. Results from the metabolomics experiments and a lab-to-field approach provide new opportunities for characterizing the seawater organic-matter content and discovering compounds involved in aerosol-formation processes.
Clarissa Baldo, Paola Formenti, Sophie Nowak, Servanne Chevaillier, Mathieu Cazaunau, Edouard Pangui, Claudia Di Biagio, Jean-Francois Doussin, Konstantin Ignatyev, Pavla Dagsson Waldhauserova, Olafur Arnalds, A. Robert MacKenzie, and Zongbo Shi
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-437, https://doi.org/10.5194/acp-2020-437, 2020
Revised manuscript accepted for ACP
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We showed that Icelandic dust has a fundamentally different chemical and mineralogical composition from low latitude dust. In particular, magnetite is as high as 1–2 % of the total dust mass. Our results suggest that Icelandic dust may have an important impact on the radiation balance in the sub-polar and polar regions.
Jing Cai, Xiangying Zeng, Guorui Zhi, Sasho Gligorovski, Guoying Sheng, Zhiqiang Yu, Xinming Wang, and Ping'an Peng
Atmos. Chem. Phys., 20, 6115–6128, https://doi.org/10.5194/acp-20-6115-2020, https://doi.org/10.5194/acp-20-6115-2020, 2020
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The composition and light-induced evolution of a water-soluble organic carbon mixture from fresh biomass burning aerosols was investigated with direct infusion electrospray ionisation high-resolution mass spectrometry (HRMS) and liquid chromatography coupled with HRMS. Our findings indicate that the water-soluble organic fraction of combustion-derived aerosols has the potential to form more oxidised organic matter, contributing to the highly oxygenated nature of atmospheric organic aerosols.
Jienan Li, Seanna M. Forrester, and Daniel A. Knopf
Atmos. Chem. Phys., 20, 6055–6080, https://doi.org/10.5194/acp-20-6055-2020, https://doi.org/10.5194/acp-20-6055-2020, 2020
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Organic aerosol is ubiquitous in the atmosphere and can change its phase state from liquid to solid in response to temperature. Our laboratory measurements demonstrate that the chemical reactivity of typical organic aerosol species with atmospheric oxidants is modulated by the species’ phase state. We find that under temperatures typical of the middle and upper troposphere the chemical lifetime of organic aerosol can be significantly extended due to the reduced reactive uptake of gas oxidants.
Lanxiadi Chen, Chao Peng, Athanasios Nenes, Wenjun Gu, Hanjing Fu, Xing Jian, Huanhuan Zhang, Guohua Zhang, Jianxi Zhu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-442, https://doi.org/10.5194/acp-2020-442, 2020
Revised manuscript accepted for ACP
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We investigated hygroscopic properties of a number of mineral dust particles in a quantitative manner, via measuring the sample mass at different relative humidities. The robust and comprehensive data obtained would significantly improve our knowledge of hygroscopicity of mineral dust and its impacts on atmospheric chemistry and climate.
Liqing Hao, Eetu Kari, Ari Leskinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-457, https://doi.org/10.5194/acp-2020-457, 2020
Revised manuscript accepted for ACP
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Our work presents secondary organic aerosol (SOA) formation results in the presence of gaseous ammonia. The particle phase ammonium was continuously produced even after SOA formation has ceased. The gas phase organic acids were experimentally observed to contribute to the formed particle phase ammonium salts. This study suggests that the presence of ammonia may change the mass and chemical composition of large-size SOA particles and can potentially alter the aerosol impact on climate change.
Abdoulaye Samaké, Aurélie Bonin, Jean-Luc Jaffrezo, Pierre Taberlet, Samuël Weber, Gaëlle Uzu, Véronique Jacob, Sébastien Conil, and Jean M. F. Martins
Atmos. Chem. Phys., 20, 5609–5628, https://doi.org/10.5194/acp-20-5609-2020, https://doi.org/10.5194/acp-20-5609-2020, 2020
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Despite being a major source of coarse organic matter, primary biogenic organic aerosols (PBOAs) remain poorly implemented in source-resolved chemical transport models. This study, based on an intensive field sampling of aerosols, combined physicochemical characterizations of PM10 with DNA high-throughput sequencing to provide a comprehensive understanding of the microbial fingerprints associated with primary sugar compounds (tracers of PBOAs) and their main surrounding environmental sources.
Yonghong Wang, Matthieu Riva, Hongbin Xie, Liine Heikkinen, Simon Schallhart, Qiaozhi Zha, Chao Yan, Xu-Cheng He, Otso Peräkylä, and Mikael Ehn
Atmos. Chem. Phys., 20, 5145–5155, https://doi.org/10.5194/acp-20-5145-2020, https://doi.org/10.5194/acp-20-5145-2020, 2020
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Chamber experiments were conducted with alpha-pinene and chlorine under low- and high-nitrogen-oxide (NOX) conditions. We estimated the HOM yields from chlorine-initiated oxidation of alpha-pinene under low-NOX conditions to be around 1.8 %, though with a uncertainty range (0.8 %–4 %) due to lack of suitable calibration methods. Our study clearly demonstrates that the chlorine-atom-initiated oxidation of alpha-pinene can produce low-volatility organic compounds.
Xingjun Fan, Tao Cao, Xufang Yu, Yan Wang, Xin Xiao, Feiyue Li, Yue Xie, Wenchao Ji, Jianzhong Song, and Ping'an Peng
Atmos. Chem. Phys., 20, 4593–4605, https://doi.org/10.5194/acp-20-4593-2020, https://doi.org/10.5194/acp-20-4593-2020, 2020
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A particle-phase O3 oxidation of biomass burning (BB) smoke particles was conducted to investigate the evolution of brown carbon (BrC) therein. The O3 aging induced the decomposition of chromophores and fluorophores. EEM–PARAFAC showed a predominant decomposition of protein-like substances and a gradual increase proportion of humic-like substances for BB BrC during O3 aging. The dynamic spectral behavior of chromophores and functional groups within BrC was further explored by 2D-COS.
Elena Ali McKnight, Nicole P. Kretekos, Demi Owusu, and Rebecca Lyn LaLonde
Atmos. Chem. Phys., 20, 4241–4254, https://doi.org/10.5194/acp-20-4241-2020, https://doi.org/10.5194/acp-20-4241-2020, 2020
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This report describes a simple, safe and effective method to prepare nitrate esters of terpenes (carene, limonene, perillic alcohol, beta-pinene and alpha-pinene) which are key oxidation products in the atmosphere. These compounds are implicated in the formation of secondary organic aerosols. A compilation of the relevant spectroscopic data has been presented. The availability of these compounds and their characterization data will enable further study of the structure–reactivity relationships.
Rongshuang Xu, Hoi Ki Lam, Kevin R. Wilson, James F. Davies, Mijung Song, Wentao Li, Ying-Lung Steve Tse, and Man Nin Chan
Atmos. Chem. Phys., 20, 3879–3893, https://doi.org/10.5194/acp-20-3879-2020, https://doi.org/10.5194/acp-20-3879-2020, 2020
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Atmospheric particles, a complex mixture of inorganic salts, organic compounds and water, can continually undergo heterogeneous oxidation initiated by gas-phase oxidants at the particle surface. We found that ammonium sulfate can decelerate the rate of heterogeneous OH reaction with 2-methyltetrols when the inorganic-to-organic mass ratio increases. These results would suggest 2-methyltetrols are likely chemically stable against heterogeneous OH oxidation in the atmosphere.
Md. Robiul Islam, Thilina Jayarathne, Isobel J. Simpson, Benjamin Werden, John Maben, Ashley Gilbert, Puppala S. Praveen, Sagar Adhikari, Arnico K. Panday, Maheswar Rupakheti, Donald R. Blake, Robert J. Yokelson, Peter F. DeCarlo, William C. Keene, and Elizabeth A. Stone
Atmos. Chem. Phys., 20, 2927–2951, https://doi.org/10.5194/acp-20-2927-2020, https://doi.org/10.5194/acp-20-2927-2020, 2020
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The Kathmandu Valley experiences high levels of air pollution. In this study, atmospheric gases and particulate matter were characterized by online and off-line measurements, with an emphasis on understanding their sources. The major sources of particulate matter and trace gases were identified as garbage burning, biomass burning, and vehicles. The majority of secondary organic aerosol was attributed to anthropogenic precursors, while a minority was attributed to biogenic gases.
Jiaoping Xing, Longyi Shao, Wenbin Zhang, Jianfei Peng, Wenhua Wang, Shijin Shuai, Min Hu, and Daizhou Zhang
Atmos. Chem. Phys., 20, 2781–2794, https://doi.org/10.5194/acp-20-2781-2020, https://doi.org/10.5194/acp-20-2781-2020, 2020
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Our results highlight the contribution of gasoline-direct-injection (GDI) vehicles to aerosols, both primary and secondary. The major particles from GDI vehicles are organic and soot particles; they actively participate in chemical conversions in the atmosphere, leading to morphology and composition changes in hours. Rapid ageing could be attributable to the acid-catalysed mechanism and high concentrations of gaseous pollutants. These results would be beneficial for control of PM2.5 pollution.
Kasper Kristensen, Louise N. Jensen, Lauriane L. J. Quéléver, Sigurd Christiansen, Bernadette Rosati, Jonas Elm, Ricky Teiwes, Henrik B. Pedersen, Marianne Glasius, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-99, https://doi.org/10.5194/acp-2020-99, 2020
Revised manuscript accepted for ACP
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Atmospheric particles are important in relation to human health and the global climate. As the global temperature changes, so may the atmospheric chemistry controlling the formation of particles formed from the reactions of natural emitted volatile organic compounds (VOCs). In the current work, we show how temperatures influence the formation and chemical composition of atmospheric particles from α-pinene; a biogenic VOC largely emitted in high-latitude environments such as the boreal forests.
Crystal D. McClure, Christopher Y. Lim, David H. Hagan, Jesse H. Kroll, and Christopher D. Cappa
Atmos. Chem. Phys., 20, 1531–1547, https://doi.org/10.5194/acp-20-1531-2020, https://doi.org/10.5194/acp-20-1531-2020, 2020
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We characterized various optical, chemical, and physical properties of particles produced from combustion of a variety of different biomass fuels, many representative of those found in the western US. We find that many properties scale with the ratio between bulk average organic aerosol and black carbon mass concentrations, although there are some properties that do not.
Lauren T. Fleming, Peng Lin, James M. Roberts, Vanessa Selimovic, Robert Yokelson, Julia Laskin, Alexander Laskin, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 20, 1105–1129, https://doi.org/10.5194/acp-20-1105-2020, https://doi.org/10.5194/acp-20-1105-2020, 2020
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We have explored the nature and stability of molecules that give biomass burning smoke its faint brown color. Different types of biomass fuels were burned and the resulting smoke was collected for a detailed chemical analysis. We found that brown molecules in smoke become less colored when they are irradiated by sunlight, but this photobleaching process is very slow. This means that biomass burning smoke will remain brown-colored for a long time and efficiently warm up the atmosphere.
Ahmed Abdelmonem, Sanduni Ratnayake, Jonathan D. Toner, and Johannes Lützenkirchen
Atmos. Chem. Phys., 20, 1075–1087, https://doi.org/10.5194/acp-20-1075-2020, https://doi.org/10.5194/acp-20-1075-2020, 2020
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We address, on the molecular level, the potential for, and consequences of, surface property variations in aerosol particles in the atmosphere. Aerosol surface aging changes the interfacial chemistry, giving rise to marked variations in the ice nucleation ability of the surface. This study provides new insights into atmospheric processes, particularly cloud formation and aerosol aging in the atmosphere, with potential implications for the pharmaceutical and food industries.
Lam Kam Chan, Khanh Q. Nguyen, Noreen Karim, Yatian Yang, Robert H. Rice, Guochun He, Michael S. Denison, and Tran B. Nguyen
Atmos. Chem. Phys., 20, 539–559, https://doi.org/10.5194/acp-20-539-2020, https://doi.org/10.5194/acp-20-539-2020, 2020
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Aerosols from the low-intensity smoldering combustion of nine types of wood were generated in a controlled laboratory environment and subjected to chemical, physical, and biological and toxicological analysis. These smoldering woodsmoke aerosols have significant biological activity that is comparable to other combustion-derived sources. We describe the molecular composition of the woodsmoke aerosols and find links between specific compounds and aerosol optical–biological properties.
Franz Friebel, Prem Lobo, David Neubauer, Ulrike Lohmann, Saskia Drossaart van Dusseldorp, Evelyn Mühlhofer, and Amewu A. Mensah
Atmos. Chem. Phys., 19, 15545–15567, https://doi.org/10.5194/acp-19-15545-2019, https://doi.org/10.5194/acp-19-15545-2019, 2019
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We investigated the change in cloud droplet activity of size-selected soot particles after being exposed to atmospheric levels of ozone over the course of 12 h. For this, we operated a 3 m3 aerosol chamber in continuous-flow mode. The results were fed into a climate model (ECHAM-HAM). We found that the oxidation of soot particles with ozone is a significant source of cloud condensation nuclei in the atmosphere.
Qun Zhang, Yongfu Xu, and Long Jia
Atmos. Chem. Phys., 19, 15007–15021, https://doi.org/10.5194/acp-19-15007-2019, https://doi.org/10.5194/acp-19-15007-2019, 2019
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The negative effects of relative humidity (RH) on secondary organic aerosol (SOA) formation from m-xylene under low NOx conditions were observed. The mechanisms of the RH effects of SOA yields have been sufficiently discussed. The decrease of SOA formation at high RH may be mainly attributed to the suppression of oligomers and the further particle-phase reaction of highly oxygenated organic molecules. The faster wall loss of SOA precursors at higher RH may also influence the SOA yield.
Kei Sato, Yuji Fujitani, Satoshi Inomata, Yu Morino, Kiyoshi Tanabe, Toshihide Hikida, Akio Shimono, Akinori Takami, Akihiro Fushimi, Yoshinori Kondo, Takashi Imamura, Hiroshi Tanimoto, and Seiji Sugata
Atmos. Chem. Phys., 19, 14901–14915, https://doi.org/10.5194/acp-19-14901-2019, https://doi.org/10.5194/acp-19-14901-2019, 2019
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The volatility distributions of secondary organic aerosol (SOA) formed from the photooxidation of 1,3,5-trimethylbenzene were investigated by composition, heating, and dilution measurements. Fresh SOA, formed from 1,3,5-trimethylbenzene, included low-volatility compounds with < 1 μg m–3 saturation concentrations, which are not assumed to exist in fresh SOA particles in the standard volatility basis-set approach. Improvements in the organic aerosol model will be necessary.
Biwu Chu, Yali Wang, Weiwei Yang, Jinzhu Ma, Qingxin Ma, Peng Zhang, Yongchun Liu, and Hong He
Atmos. Chem. Phys., 19, 14777–14790, https://doi.org/10.5194/acp-19-14777-2019, https://doi.org/10.5194/acp-19-14777-2019, 2019
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This study found that the coexisting NO2 and/or C2H2 had significant influences on heterogeneous oxidation of SO2 due to the ubiquitous interactions between organic and inorganic species, and their effects were different under dark conditions or with UV irradiation. The experimental results of this study highlighted the requirement to consider the influence of coexisting organics and other inorganic gases in the heterogeneous oxidation kinetics of SO2.
Adam W. Birdsall, Jack C. Hensley, Paige S. Kotowitz, Andrew J. Huisman, and Frank N. Keutsch
Atmos. Chem. Phys., 19, 14195–14209, https://doi.org/10.5194/acp-19-14195-2019, https://doi.org/10.5194/acp-19-14195-2019, 2019
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We have measured the evaporation rates of butenedial, a four-carbon dialdehyde produced in the atmosphere, from individual levitated particles. Effective vapor pressures and Henry's law constants, which characterize the compound's gas-particle partitioning behavior, were determined. The important role of hydration reactions was observed under both dry and humid conditions, as well as a salting-out effect in the presence of sodium chloride or sodium sulfate.
John G. Watson, Junji Cao, L.-W. Antony Chen, Qiyuan Wang, Jie Tian, Xiaoliang Wang, Steven Gronstal, Steven Sai Hang Ho, Adam C. Watts, and Judith C. Chow
Atmos. Chem. Phys., 19, 14173–14193, https://doi.org/10.5194/acp-19-14173-2019, https://doi.org/10.5194/acp-19-14173-2019, 2019
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Although peat burning is a common global emission source, region-specific emission factors are lacking. This work fills that gap for six peat-bearing regions. It is also shown through simulated aging with an oxidation flow reactor that potential aerosol mass changes during transport.
Min Cui, Cheng Li, Yingjun Chen, Fan Zhang, Jun Li, Bin Jiang, Yangzhi Mo, Jia Li, Caiqing Yan, Mei Zheng, Zhiyong Xie, Gan Zhang, and Junyu Zheng
Atmos. Chem. Phys., 19, 13945–13956, https://doi.org/10.5194/acp-19-13945-2019, https://doi.org/10.5194/acp-19-13945-2019, 2019
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Refined source apportionment is urgently needed but hard to achieve due to a lack of specific biomarkers. Recently, Fourier transform ion cyclotron resonance mass spectrometry has been used to analyse the probable chemical structure of polar organic matter emitted from off-road engines. We found more condensed aromatic rings in S-containing compounds for HFO-fueled vessels, while more abundant aliphatic chains were observed in emissions from diesel equipment.
Christopher Y. Lim, David H. Hagan, Matthew M. Coggon, Abigail R. Koss, Kanako Sekimoto, Joost de Gouw, Carsten Warneke, Christopher D. Cappa, and Jesse H. Kroll
Atmos. Chem. Phys., 19, 12797–12809, https://doi.org/10.5194/acp-19-12797-2019, https://doi.org/10.5194/acp-19-12797-2019, 2019
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Wildfires are a large source of gases and particles to the atmosphere, both of which impact human health and climate. The amount and composition of particles from wildfires can change with time in the atmosphere; however, the impact of aging is not well understood. In a series of controlled laboratory experiments, we show that the particles are oxidized and a significant fraction of the gas-phase carbon (24 %–56 %) is converted to particle mass over the course of several days in the atmosphere.
Masayuki Takeuchi and Nga L. Ng
Atmos. Chem. Phys., 19, 12749–12766, https://doi.org/10.5194/acp-19-12749-2019, https://doi.org/10.5194/acp-19-12749-2019, 2019
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Organic nitrate is ubiquitous in the atmosphere and impacts the formation of aerosol and ozone, two leading air pollutants of concern worldwide. We conducted a comprehensive laboratory study to investigate the hydrolysis process of organic nitrate aerosol formed from monoterpenes, which are important reactive chemicals emitted by plants. Our results provide experimentally constrained parameters required to assess the role of organic nitrate in the formation of the air pollutants of our concern.
Mingjin Tang, Chak K. Chan, Yong Jie Li, Hang Su, Qingxin Ma, Zhijun Wu, Guohua Zhang, Zhe Wang, Maofa Ge, Min Hu, Hong He, and Xinming Wang
Atmos. Chem. Phys., 19, 12631–12686, https://doi.org/10.5194/acp-19-12631-2019, https://doi.org/10.5194/acp-19-12631-2019, 2019
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Hygroscopicity is one of the most important properties of aerosol particles, and a number of experimental techniques, which differ largely in principles, configurations and cost, have been developed to investigate hygroscopic properties of atmospherically relevant particles. Our paper provides a comprehensive and critical review of available techniques for aerosol hygroscopicity studies.
Zhenzhen Wang, Tao Wang, Hongbo Fu, Liwu Zhang, Mingjin Tang, Christian George, Vicki H. Grassian, and Jianmin Chen
Atmos. Chem. Phys., 19, 12569–12585, https://doi.org/10.5194/acp-19-12569-2019, https://doi.org/10.5194/acp-19-12569-2019, 2019
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This study confirmed that SO2 uptake on mineral particles could be greatly enhanced during cloud processing. The large pH fluctuations between the cloud-aerosol modes could significantly modify the microphysical properties of particles, and triggered the formation of reactive Fe particles to accelerate sulfate formation via a self-amplifying process. Results of this study could partly explain the missing source of sulfate and improve agreement between models and field observations.
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Short summary
We discuss the development and application of a robust clustering method for the interpretation of compound-specific organic aerosol thermal desorption profiles. We demonstrate the utility of clustering for analysis and interpretation of the composition and volatility of secondary organic aerosol. We show that the thermal desorption profiles are represented by only 9–13 distinct clusters, with the number of clusters obtained dependent on the precursor and formation conditions.
We discuss the development and application of a robust clustering method for the interpretation...
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