Articles | Volume 14, issue 11
https://doi.org/10.5194/acp-14-5639-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-14-5639-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
06 Jun 2014
Research article |
| 06 Jun 2014
An assessment of the performance of the Monitor for AeRosols and GAses in ambient air (MARGA): a semi-continuous method for soluble compounds
I. C. Rumsey
Office of Research and Development, US Environmental Protection Agency, Research Triangle Park, NC 27711, USA
K. A. Cowen
Battelle, Columbus, OH, 43201, USA
J. T. Walker
Office of Research and Development, US Environmental Protection Agency, Research Triangle Park, NC 27711, USA
T. J. Kelly
Battelle, Columbus, OH, 43201, USA
E. A. Hanft
Battelle, Columbus, OH, 43201, USA
K. Mishoe
AMEC, Jacksonville, FL, 32669, USA
C. Rogers
AMEC, Jacksonville, FL, 32669, USA
R. Proost
Metrohm Applikon B.V., Schiedam, the Netherlands
G. M. Beachley
Clean Air Markets Division, US Environmental Protection Agency, Washington, DC 20460, USA
G. Lear
Clean Air Markets Division, US Environmental Protection Agency, Washington, DC 20460, USA
T. Frelink
Metrohm Applikon B.V., Schiedam, the Netherlands
R. P. Otjes
Energy Research Centre of the Netherlands (ECN), Petten, the Netherlands
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Ian C. Rumsey and John T. Walker
Atmos. Meas. Tech., 9, 2581–2592, https://doi.org/10.5194/amt-9-2581-2016, https://doi.org/10.5194/amt-9-2581-2016, 2016
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The performance of the MARGA (Monitor of AeRosols and GAses in ambient air) instrument in measuring speciated nitrogen and sulfur fluxes is evaluated for the first time. The results demonstrate that the MARGA instrument can be used to make accurate measurements of speciated nitrogen and sulfur deposition. These measurements are urgently needed to evaluate chemical transport models and develop risk assessments and mitigation strategies to protect ecosystems from nutrient and acidic deposition.
Davide Putero, Paolo Cristofanelli, Kai-Lan Chang, Gaëlle Dufour, Gregory Beachley, Cédric Couret, Peter Effertz, Daniel A. Jaffe, Dagmar Kubistin, Jason Lynch, Irina Petropavlovskikh, Melissa Puchalski, Timothy Sharac, Barkley C. Sive, Martin Steinbacher, Carlos Torres, and Owen R. Cooper
Atmos. Chem. Phys., 23, 15693–15709, https://doi.org/10.5194/acp-23-15693-2023, https://doi.org/10.5194/acp-23-15693-2023, 2023
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We investigated the impact of societal restriction measures during the COVID-19 pandemic on surface ozone at 41 high-elevation sites worldwide. Negative ozone anomalies were observed for spring and summer 2020 for all of the regions considered. In 2021, negative anomalies continued for Europe and partially for the eastern US, while western US sites showed positive anomalies due to wildfires. IASI satellite data and the Carbon Monitor supported emission reductions as a cause of the anomalies.
John T. Walker, Xi Chen, Zhiyong Wu, Donna Schwede, Ryan Daly, Aleksandra Djurkovic, A. Christopher Oishi, Eric Edgerton, Jesse Bash, Jennifer Knoepp, Melissa Puchalski, John Iiames, and Chelcy F. Miniat
Biogeosciences, 20, 971–995, https://doi.org/10.5194/bg-20-971-2023, https://doi.org/10.5194/bg-20-971-2023, 2023
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Better estimates of atmospheric nitrogen (N) deposition are needed to accurately assess ecosystem risk and impacts from deposition of nutrients and acidity. Using measurements and modeling, we estimate total N deposition of 6.7 kg N ha−1 yr−1 at a forest site in the southern Appalachian Mountains, a region sensitive to atmospheric deposition. Reductions in deposition of reduced forms of N (ammonia and ammonium) will be needed to meet the lowest estimates of N critical loads for the region.
Sarah Waldo, Jake J. Beaulieu, William Barnett, D. Adam Balz, Michael J. Vanni, Tanner Williamson, and John T. Walker
Biogeosciences, 18, 5291–5311, https://doi.org/10.5194/bg-18-5291-2021, https://doi.org/10.5194/bg-18-5291-2021, 2021
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Human-made reservoirs impact the carbon cycle. In particular, the breakdown of organic matter in reservoir sediments can result in large emissions of greenhouse gases (especially methane) to the atmosphere. This study takes an intensive look at the patterns in greenhouse gas emissions from a single reservoir in Ohio (United States) and the role of water temperature, precipitation, and algal blooms in emissions. We saw a "spring burst" of elevated emissions that challenged our assumptions.
Zhiyong Wu, Leiming Zhang, John T. Walker, Paul A. Makar, Judith A. Perlinger, and Xuemei Wang
Geosci. Model Dev., 14, 5093–5105, https://doi.org/10.5194/gmd-14-5093-2021, https://doi.org/10.5194/gmd-14-5093-2021, 2021
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A community dry deposition algorithm for modeling the gaseous dry deposition process in chemistry transport models was extended to include an additional 12 oxidized volatile organic compounds and hydrogen cyanide based on their physicochemical properties and was then evaluated using field flux measurements over a mixed forest. This study provides a useful tool that is needed in chemistry transport models with increasing complexity for simulating an important atmospheric process.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Xi Chen, Mingjie Xie, Michael D. Hays, Eric Edgerton, Donna Schwede, and John T. Walker
Atmos. Chem. Phys., 18, 6829–6846, https://doi.org/10.5194/acp-18-6829-2018, https://doi.org/10.5194/acp-18-6829-2018, 2018
Xi Chen, John T. Walker, and Chris Geron
Atmos. Meas. Tech., 10, 3893–3908, https://doi.org/10.5194/amt-10-3893-2017, https://doi.org/10.5194/amt-10-3893-2017, 2017
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The MARGA instrument is a powerful research tool for investigating atmospheric chemistry and the exchange of gases and particles between the atmosphere and biosphere. Our study examines the operating characteristics of the instrument with a focus on the software used to calculate air concentrations. We show that more accurate measurements may be obtained by calibrating the instrument with a range of standards in addition to the single internal standard used in online concentration calculations.
Ian C. Rumsey and John T. Walker
Atmos. Meas. Tech., 9, 2581–2592, https://doi.org/10.5194/amt-9-2581-2016, https://doi.org/10.5194/amt-9-2581-2016, 2016
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The performance of the MARGA (Monitor of AeRosols and GAses in ambient air) instrument in measuring speciated nitrogen and sulfur fluxes is evaluated for the first time. The results demonstrate that the MARGA instrument can be used to make accurate measurements of speciated nitrogen and sulfur deposition. These measurements are urgently needed to evaluate chemical transport models and develop risk assessments and mitigation strategies to protect ecosystems from nutrient and acidic deposition.
F. Yu, G. Luo, S. C. Pryor, P. R. Pillai, S. H. Lee, J. Ortega, J. J. Schwab, A. G. Hallar, W. R. Leaitch, V. P. Aneja, J. N. Smith, J. T. Walker, O. Hogrefe, and K. L. Demerjian
Atmos. Chem. Phys., 15, 13993–14003, https://doi.org/10.5194/acp-15-13993-2015, https://doi.org/10.5194/acp-15-13993-2015, 2015
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The role of low-volatility organics in new particle formation (NPF) in the atmosphere is assessed. An empirical formulation in which formation rate is a function of the concentrations of sulfuric acid and low-volatility organics significantly overpredicts NPF in the summer.
Two different schemes predict quite different nucleation rates (including their spatial patterns), concentrations of cloud condensation nuclei, and aerosol first indirect radiative forcing in North America.
M. M. Twigg, C. F. Di Marco, S. Leeson, N. van Dijk, M. R. Jones, I. D. Leith, E. Morrison, M. Coyle, R. Proost, A. N. M. Peeters, E. Lemon, T. Frelink, C. F. Braban, E. Nemitz, and J. N. Cape
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Hourly inorganic composition of UK background particulate matter (PM10 and PM2.5) has been studied for a 6.5-year period at Auchencorth Moss, Scotland. Long-range transport of both anthropogenic secondary and natural primary PM is observed, driven primarily by meteorology. The importance of nitrate, sulfate and ammonium during pollution events in the UK is demonstrated.
B. B. Almand-Hunter, J. T. Walker, N. P. Masson, L. Hafford, and M. P. Hannigan
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Biogeosciences, 10, 1635–1645, https://doi.org/10.5194/bg-10-1635-2013, https://doi.org/10.5194/bg-10-1635-2013, 2013
J. T. Walker, M. R. Jones, J. O. Bash, L. Myles, T. Meyers, D. Schwede, J. Herrick, E. Nemitz, and W. Robarge
Biogeosciences, 10, 981–998, https://doi.org/10.5194/bg-10-981-2013, https://doi.org/10.5194/bg-10-981-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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Measurement report: Atmospheric ice nuclei in the Changbai Mountains (2623 m a.s.l.) in northeastern Asia
Morphological and optical properties of carbonaceous aerosol particles from ship emissions and biomass burning during a summer cruise measurement in the South China Sea
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Chemical composition, sources and formation mechanism of urban PM2.5 in Southwest China: a case study at the beginning of 2023
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Variation in chemical composition and volatility of oxygenated organic aerosol in different rural, urban, and mountain environments
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Roles of marine biota in the formation of atmospheric bioaerosols, cloud condensation nuclei, and ice-nucleating particles over the North Pacific Ocean, Bering Sea, and Arctic Ocean
Evolution of nucleophilic high molecular-weight organic compounds in ambient aerosols: a case study
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Source apportionment of PM2.5 in Montréal, Canada, and health risk assessment for potentially toxic elements
Physicochemical and temporal characteristics of individual atmospheric aerosol particles in urban Seoul during KORUS-AQ campaign: insights from single-particle analysis
Mass spectrometric analysis of unprecedented high levels of carbonaceous aerosol particles long-range transported from wildfires in the Siberian Arctic
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Marine carbohydrates in Arctic aerosol particles and fog – diversity of oceanic sources and atmospheric transformations
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Daytime and nighttime aerosol soluble iron formation in clean and slightly-polluted moisture air in a coastal city in eastern China
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Summertime response of ozone and fine particulate matter to mixing layer meteorology over the North China Plain
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Yi-Jia Ma, Yu Xu, Ting Yang, Hong-Wei Xiao, and Hua-Yun Xiao
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Maud Leriche, Pierre Tulet, Laurent Deguillaume, Frédéric Burnet, Aurélie Colomb, Agnès Borbon, Corinne Jambert, Valentin Duflot, Stéphan Houdier, Jean-Luc Jaffrezo, Mickaël Vaïtilingom, Pamela Dominutti, Manon Rocco, Camille Mouchel-Vallon, Samira El Gdachi, Maxence Brissy, Maroua Fathalli, Nicolas Maury, Bert Verreyken, Crist Amelynck, Niels Schoon, Valérie Gros, Jean-Marc Pichon, Mickael Ribeiro, Eric Pique, Emmanuel Leclerc, Thierry Bourrianne, Axel Roy, Eric Moulin, Joël Barrie, Jean-Marc Metzger, Guillaume Péris, Christian Guadagno, Chatrapatty Bhugwant, Jean-Mathieu Tibere, Arnaud Tournigand, Evelyn Freney, Karine Sellegri, Anne-Marie Delort, Pierre Amato, Muriel Joly, Jean-Luc Baray, Pascal Renard, Angelica Bianco, Anne Réchou, and Guillaume Payen
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Xinya Liu, Bas Henzing, Arjan Hensen, Jan Mulder, Peng Yao, Danielle van Dinther, Jerry van Bronckhorst, Rujin Huang, and Ulrike Dusek
Atmos. Chem. Phys., 24, 3405–3420, https://doi.org/10.5194/acp-24-3405-2024, https://doi.org/10.5194/acp-24-3405-2024, 2024
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Eva-Lou Edwards, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Claire E. Robinson, Michael A. Shook, Edward L. Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 24, 3349–3378, https://doi.org/10.5194/acp-24-3349-2024, https://doi.org/10.5194/acp-24-3349-2024, 2024
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We investigate Cl− depletion in sea salt particles over the northwest Atlantic from December 2021 to June 2022 using an airborne dataset. Losses of Cl− are greatest in May and least in December–February and March. Inorganic acidic species can account for all depletion observed for December–February, March, and June near Bermuda but none in May. Quantifying Cl− depletion as a percentage captures seasonal trends in depletion but fails to convey the effects it may have on atmospheric oxidation.
Yue Sun, Yujiao Zhu, Yanbin Qi, Lanxiadi Chen, Jiangshan Mu, Ye Shan, Yu Yang, Yanqiu Nie, Ping Liu, Can Cui, Ji Zhang, Mingxuan Liu, Lingli Zhang, Yufei Wang, Xinfeng Wang, Mingjin Tang, Wenxing Wang, and Likun Xue
Atmos. Chem. Phys., 24, 3241–3256, https://doi.org/10.5194/acp-24-3241-2024, https://doi.org/10.5194/acp-24-3241-2024, 2024
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Field observations were conducted at the summit of Changbai Mountain in northeast Asia. The cumulative number concentration of ice-nucleating particles (INPs) varied from 1.6 × 10−3 to 78.3 L−1 over the temperature range of −5.5 to −29.0 ℃. Biological INPs (bio-INPs) accounted for the majority of INPs, and the proportion exceeded 90% above −13.0 ℃. Planetary boundary layer height, valley breezes, and long-distance transport of air mass influence the abundance of bio-INPs.
Cuizhi Sun, Yongyun Zhang, Baoling Liang, Min Gao, Xi Sun, Fei Li, Xue Ni, Qibin Sun, Hengjia Ou, Dexian Chen, Shengzhen Zhou, and Jun Zhao
Atmos. Chem. Phys., 24, 3043–3063, https://doi.org/10.5194/acp-24-3043-2024, https://doi.org/10.5194/acp-24-3043-2024, 2024
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In a May–June 2021 expedition in the South China Sea, we analyzed black and brown carbon in marine aerosols, key to light absorption and climate impact. Using advanced in situ and microscope techniques, we observed particle size, structure, and tar balls mixed with various elements. Results showed biomass burning and fossil fuels majorly influence light absorption, especially during significant burning events. This research aids the understanding of carbonaceous aerosols' role in marine climate.
C. Isabel Moreno, Radovan Krejci, Jean-Luc Jaffrezo, Gaëlle Uzu, Andrés Alastuey, Marcos F. Andrade, Valeria Mardóñez, Alkuin Maximilian Koenig, Diego Aliaga, Claudia Mohr, Laura Ticona, Fernando Velarde, Luis Blacutt, Ricardo Forno, David N. Whiteman, Alfred Wiedensohler, Patrick Ginot, and Paolo Laj
Atmos. Chem. Phys., 24, 2837–2860, https://doi.org/10.5194/acp-24-2837-2024, https://doi.org/10.5194/acp-24-2837-2024, 2024
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Aerosol chemical composition (ions, sugars, carbonaceous matter) from 2011 to 2020 was studied at Mt. Chacaltaya (5380 m a.s.l., Bolivian Andes). Minimum concentrations occur in the rainy season with maxima in the dry and transition seasons. The origins of the aerosol are located in a radius of hundreds of kilometers: nearby urban and rural areas, natural biogenic emissions, vegetation burning from Amazonia and Chaco, Pacific Ocean emissions, soil dust, and Peruvian volcanism.
Junke Zhang, Yunfei Su, Chunying Chen, Wenkai Guo, Qinwen Tan, Miao Feng, Danlin Song, Tao Jiang, Qiang Chen, Yuan Li, Wei Li, Yizhi Wang, Xiaojuan Huang, Lin Han, Wanqing Wu, and Gehui Wang
Atmos. Chem. Phys., 24, 2803–2820, https://doi.org/10.5194/acp-24-2803-2024, https://doi.org/10.5194/acp-24-2803-2024, 2024
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Typical haze events in Chengdu at the beginning of 2023 were investigated with bulk-chemical and single-particle analyses along with numerical model simulations. By integrating the obtained chemical composition, source, mixing state and numerical simulation results, we infer that Haze-1 was mainly caused by pollutants related to fossil fuel combustion, especially local mobile sources, while Haze-2 was triggered by the secondary pollutants, which mainly came from regional transmission.
Elena Barbaro, Matteo Feltracco, Fabrizio De Blasi, Clara Turetta, Marta Radaelli, Warren Cairns, Giulio Cozzi, Giovanna Mazzi, Marco Casula, Jacopo Gabrieli, Carlo Barbante, and Andrea Gambaro
Atmos. Chem. Phys., 24, 2821–2835, https://doi.org/10.5194/acp-24-2821-2024, https://doi.org/10.5194/acp-24-2821-2024, 2024
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The study analyzed a year of atmospheric aerosol composition at Col Margherita in the Italian Alps. Over 100 chemical markers were identified, including major ions, organic compounds, and trace elements. It revealed sources of aerosol, highlighted impacts of Saharan dust events, and showed anthropogenic pollution's influence despite the site's remoteness. Enrichment factors emphasized non-natural sources of trace elements. Source apportionment identified four key factors affecting the area.
Karl Espen Yttri, Are Bäcklund, Franz Conen, Sabine Eckhardt, Nikolaos Evangeliou, Markus Fiebig, Anne Kasper-Giebl, Avram Gold, Hans Gundersen, Cathrine Lund Myhre, Stephen Matthew Platt, David Simpson, Jason D. Surratt, Sönke Szidat, Martin Rauber, Kjetil Tørseth, Martin Album Ytre-Eide, Zhenfa Zhang, and Wenche Aas
Atmos. Chem. Phys., 24, 2731–2758, https://doi.org/10.5194/acp-24-2731-2024, https://doi.org/10.5194/acp-24-2731-2024, 2024
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We discuss carbonaceous aerosol (CA) observed at the high Arctic Zeppelin Observatory (2017 to 2020). We find that organic aerosol is a significant fraction of the Arctic aerosol, though less than sea salt aerosol and mineral dust, as well as non-sea-salt sulfate, originating mainly from anthropogenic sources in winter and from natural sources in summer, emphasizing the importance of wildfires for biogenic secondary organic aerosol and primary biological aerosol particles observed in the Arctic.
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr
Atmos. Chem. Phys., 24, 2607–2624, https://doi.org/10.5194/acp-24-2607-2024, https://doi.org/10.5194/acp-24-2607-2024, 2024
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We present distinct molecular composition and volatility of oxygenated organic aerosol particles in different rural, urban, and mountain environments. We do a comprehensive investigation of the relationship between the chemical composition and volatility of oxygenated organic aerosol particles across different systems and environments. This study provides implications for volatility descriptions of oxygenated organic aerosol particles in different model frameworks.
Jing Cai, Juha Sulo, Yifang Gu, Sebastian Holm, Runlong Cai, Steven Thomas, Almuth Neuberger, Fredrik Mattsson, Marco Paglione, Stefano Decesari, Matteo Rinaldi, Rujing Yin, Diego Aliaga, Wei Huang, Yuanyuan Li, Yvette Gramlich, Giancarlo Ciarelli, Lauriane Quéléver, Nina Sarnela, Katrianne Lehtipalo, Nora Zannoni, Cheng Wu, Wei Nie, Juha Kangasluoma, Claudia Mohr, Markku Kulmala, Qiaozhi Zha, Dominik Stolzenburg, and Federico Bianchi
Atmos. Chem. Phys., 24, 2423–2441, https://doi.org/10.5194/acp-24-2423-2024, https://doi.org/10.5194/acp-24-2423-2024, 2024
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By combining field measurements, simulations and recent chamber experiments, we investigate new particle formation (NPF) and growth in the Po Valley, where both haze and frequent NPF occur. Our results show that sulfuric acid, ammonia and amines are the dominant NPF precursors there. A high NPF rate and a lower condensation sink lead to a greater survival probability for newly formed particles, highlighting the importance of gas-to-particle conversion for aerosol concentrations.
Kaori Kawana, Fumikazu Taketani, Kazuhiko Matsumoto, Yutaka Tobo, Yoko Iwamoto, Takuma Miyakawa, Akinori Ito, and Yugo Kanaya
Atmos. Chem. Phys., 24, 1777–1799, https://doi.org/10.5194/acp-24-1777-2024, https://doi.org/10.5194/acp-24-1777-2024, 2024
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Based on comprehensive shipborne observations, we found strong links between sea-surface biological materials and the formation of atmospheric fluorescent bioaerosols, cloud condensation nuclei, and ice-nucleating particles over the Arctic Ocean and Bering Sea during autumn 2019. Taking the wind-speed effect into account, we propose equations to approximate the links for this cruise, which can be used as a guide for modeling as well as for systematic comparisons with other observations.
Chen He, Hanxiong Che, Zier Bao, Yiliang Liu, Qing Li, Miao Hu, Jiawei Zhou, Shumin Zhang, Xiaojiang Yao, Quan Shi, Chunmao Chen, Yan Han, Lingshuo Meng, Xin Long, Fumo Yang, and Yang Chen
Atmos. Chem. Phys., 24, 1627–1639, https://doi.org/10.5194/acp-24-1627-2024, https://doi.org/10.5194/acp-24-1627-2024, 2024
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We examined the daily evolution of high molecular-weight organic compounds with a molecular weight of up to 1000 Da in order to comprehend their behaviors in the atmosphere under actual conditions. These compounds were proven to undergo multi-generation oxidation, carboxylation, and nitrification via both day- and nighttime chemistry.
Karine Desboeufs, Paola Formenti, Raquel Torres-Sánchez, Kerstin Schepanski, Jean-Pierre Chaboureau, Hendrik Andersen, Jan Cermak, Stefanie Feuerstein, Benoit Laurent, Danitza Klopper, Andreas Namwoonde, Mathieu Cazaunau, Servanne Chevaillier, Anaïs Feron, Cécile Mirande-Bret, Sylvain Triquet, and Stuart J. Piketh
Atmos. Chem. Phys., 24, 1525–1541, https://doi.org/10.5194/acp-24-1525-2024, https://doi.org/10.5194/acp-24-1525-2024, 2024
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This study investigates the fractional solubility of iron (Fe) in dust particles along the coast of Namibia, a critical region for the atmospheric Fe supply of the South Atlantic Ocean. Our results suggest a possible two-way interplay whereby marine biogenic emissions from the coastal marine ecosystems into the atmosphere would increase the solubility of Fe-bearing dust by photo-reduction processes. The subsequent deposition of soluble Fe could act to further enhance marine biogenic emissions.
Sunhye Kim, Jo Machesky, Drew R. Gentner, and Albert A. Presto
Atmos. Chem. Phys., 24, 1281–1298, https://doi.org/10.5194/acp-24-1281-2024, https://doi.org/10.5194/acp-24-1281-2024, 2024
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Cooking emissions are often an overlooked source of air pollution. We used a mobile lab to measure the characteristics of particles emitted from cooking sites in two cities. Our findings showed that cooking releases a substantial number of fine particles. While most emissions were similar, a bakery site showed distinctive chemical compositions with higher nitrogen compound levels. Thus, understanding the particle emissions from different cooking activities is crucial.
Nansi Fakhri, Robin Stevens, Arnold Downey, Konstantina Oikonomou, Jean Sciare, Charbel Afif, and Patrick L. Hayes
Atmos. Chem. Phys., 24, 1193–1212, https://doi.org/10.5194/acp-24-1193-2024, https://doi.org/10.5194/acp-24-1193-2024, 2024
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We investigated the chemical composition of atmospheric fine particles, their emission sources, and the potential human health risk associated with trace elements in particles for an urban site in Montréal over a 3-month period (August–November). This study represents the first time that such extensive composition measurements were included in an urban source apportionment study in Canada, and it provides greater resolution of fine-particle sources than has been previously achieved in Canada.
Hanjin Yoo, Li Wu, Hong Geng, and Chul-Un Ro
Atmos. Chem. Phys., 24, 853–867, https://doi.org/10.5194/acp-24-853-2024, https://doi.org/10.5194/acp-24-853-2024, 2024
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We conducted an investigation of atmospheric aerosols collected in Seoul, South Korea, during the KORUS-AQ campaign on a single-particle basis. We were able to identify their sources, the atmospheric fate, and the impacts of local emissions and long-range transport on aerosol composition. Additionally, we traced potential sources of non-exhaust heavy-metal particles. This comprehensive analysis provides valuable insights into the complex dynamics of urban aerosols.
Eric Schneider, Hendryk Czech, Olga Popovicheva, Marina Chichaeva, Vasily Kobelev, Nikolay Kasimov, Tatiana Minkina, Christopher Paul Rüger, and Ralf Zimmermann
Atmos. Chem. Phys., 24, 553–576, https://doi.org/10.5194/acp-24-553-2024, https://doi.org/10.5194/acp-24-553-2024, 2024
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This study provides insights into the complex chemical composition of long-range-transported wildfire plumes from Yakutia, which underwent different levels of atmospheric processing. With complementary mass spectrometric techniques, we improve our understanding of the chemical processes and atmospheric fate of wildfire plumes. Unprecedented high levels of carbonaceous aerosols crossed the polar circle with implications for the Arctic ecosystem and consequently climate.
Qiongqiong Wang, Shuhui Zhu, Shan Wang, Cheng Huang, Yusen Duan, and Jian Zhen Yu
Atmos. Chem. Phys., 24, 475–486, https://doi.org/10.5194/acp-24-475-2024, https://doi.org/10.5194/acp-24-475-2024, 2024
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We investigated short-term source apportionment of PM2.5 utilizing rolling positive matrix factorization (PMF) and online PM chemical speciation data, which included source-specific organic tracers collected over a period of 37 d during the winter of 2019–2020 in suburban Shanghai, China. The findings highlight that by imposing constraints on the primary source profiles, short-term PMF analysis successfully replicated both the individual primary sources and the total secondary sources.
Jiyuan Yang, Guoyang Lei, Jinfeng Zhu, Yutong Wu, Chang Liu, Kai Hu, Junsong Bao, Zitong Zhang, Weili Lin, and Jun Jin
Atmos. Chem. Phys., 24, 123–136, https://doi.org/10.5194/acp-24-123-2024, https://doi.org/10.5194/acp-24-123-2024, 2024
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The atmospheric pollution and formation mechanisms of particulate-bound alkyl nitrate in Beijing were studied. C9–C16 long-chain n-alkyl nitrates negatively correlated with O3 but positively correlated with PM2.5 and NO2, so they may not be produced during gas-phase homogeneous reactions in the photochemical process but form through reactions between alkanes and nitrates on PM surfaces. Particulate-bound n-alkyl nitrates strongly affect both haze pollution and atmospheric visibility.
Yanqin Ren, Zhenhai Wu, Yuanyuan Ji, Fang Bi, Junling Li, Haijie Zhang, Hao Zhang, Hong Li, and Gehui Wang
EGUsphere, https://doi.org/10.5194/egusphere-2023-2593, https://doi.org/10.5194/egusphere-2023-2593, 2024
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Nitrated aromatic compounds (NACs) and oxygenated derivatives of polycyclic aromatic hydrocarbons (OPAHs) in PM2.5 were examined from an urban area in Beijing during the autumn and winter. The OPAHs and NACs concentrations were much higher during heating than those before heating. They majorly originated from the combustion of biomass and automobile emissions, and the secondary generation was the major contributor throughout the whole sampling period.
Lisa Azzarello, Rebecca A. Washenfelder, Michael A. Robinson, Alessandro Franchin, Caroline C. Womack, Christopher D. Holmes, Steven S. Brown, Ann Middlebrook, Tim Newberger, Colm Sweeney, and Cora J. Young
Atmos. Chem. Phys., 23, 15643–15654, https://doi.org/10.5194/acp-23-15643-2023, https://doi.org/10.5194/acp-23-15643-2023, 2023
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We present a molecular size-resolved offline analysis of water-soluble brown carbon collected on an aircraft during FIREX-AQ. The smoke plumes were aged 0 to 5 h, where absorption was dominated by small molecular weight molecules, brown carbon absorption downwind did not consistently decrease, and the measurements differed from online absorption measurements of the same samples. We show how differences between online and offline absorption could be related to different measurement conditions.
Sebastian Zeppenfeld, Manuela van Pinxteren, Markus Hartmann, Moritz Zeising, Astrid Bracher, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 15561–15587, https://doi.org/10.5194/acp-23-15561-2023, https://doi.org/10.5194/acp-23-15561-2023, 2023
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Marine carbohydrates are produced in the surface of the ocean, enter the atmophere as part of sea spray aerosol particles, and potentially contribute to the formation of fog and clouds. Here, we present the results of a sea–air transfer study of marine carbohydrates conducted in the high Arctic. Besides a chemo-selective transfer, we observed a quick atmospheric aging of carbohydrates, possibly as a result of both biotic and abiotic processes.
Xing Wei, Yanjie Shen, Xiao-Ying Yu, Yang Gao, Huiwang Gao, Ming Chu, Yujiao Zhu, and Xiaohong Yao
Atmos. Chem. Phys., 23, 15325–15350, https://doi.org/10.5194/acp-23-15325-2023, https://doi.org/10.5194/acp-23-15325-2023, 2023
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We investigate the contribution of grown new particles to Nccn at a rural mountain site in the North China Plain. The total particle number concentrations (Ncn) observed on 8 new particle formation (NPF) days were higher compared to non-NPF days. The Nccn at 0.2 % supersaturation (SS) and 0.4 % SS on the NPF days was significantly lower than on non-NPF days. Only one of eight NPF events had detectable net contributions to Nccn at 0.4 % SS and 1.0 % SS with increased κ values.
Yuquan Gong, Ru-Jin Huang, Lu Yang, Ting Wang, Wei Yuan, Wei Xu, Wenjuan Cao, Yang Wang, and Yongjie Li
Atmos. Chem. Phys., 23, 15197–15207, https://doi.org/10.5194/acp-23-15197-2023, https://doi.org/10.5194/acp-23-15197-2023, 2023
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This study reveals the large day–night differences in brown carbon (BrC) chromophore composition, which was not known previously. The results provide insights into the effects of atmospheric processes and emissions on BrC composition.
Ryan N. Farley, Sonya Collier, Christopher D. Cappa, Leah R. Williams, Timothy B. Onasch, Lynn M. Russell, Hwajin Kim, and Qi Zhang
Atmos. Chem. Phys., 23, 15039–15056, https://doi.org/10.5194/acp-23-15039-2023, https://doi.org/10.5194/acp-23-15039-2023, 2023
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Soot particles, also known as black carbon (BC), have important implications for global climate and regional air quality. After the particles are emitted, BC can be coated with other material, impacting the aerosol properties. We selectively measured the composition of particles containing BC to explore their sources and chemical transformations in the atmosphere. We focus on a persistent, multiday fog event in order to study the effects of chemical reactions occurring within liquid droplets.
Wenshuai Li, Yuxuan Qi, Yingchen Liu, Guanru Wu, Yanjing Zhang, Jinhui Shi, Wenjun Qu, Lifang Sheng, Wencai Wang, Daizhou Zhang, and Yang Zhou
EGUsphere, https://doi.org/10.5194/egusphere-2023-2698, https://doi.org/10.5194/egusphere-2023-2698, 2023
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Aerosol particles from mainland can transport to oceans and deposit, providing soluble Fe and affecting phytoplankton growth. Thus, we studied the dissolution process of aerosol Fe and found that photochemistry played a key role in promoting Fe dissolution in clean conditions. RH-dependent reactions were more influential in slightly-polluted conditions. These results highlight the distinct roles of two weather-related parameters (radiation and RH) in influencing geochemical cycles related to Fe.
Fuzhen Shen, Michaela I. Hegglin, and Yue Yuan
EGUsphere, https://doi.org/10.5194/egusphere-2023-2425, https://doi.org/10.5194/egusphere-2023-2425, 2023
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We attempt to use a novel structural Self-Organising Map and Machine Learning models to identify a weather system and quantify the importance of each meteorological factor in driving the unexpected PM2.5 and O3 changes under the specific weather system during the COVID-19 lockdown in China. The result highlights temperature under the double-centre high-pressure system plays the most crucial role in abnormal events.
Xiaoxiao Li, Yijing Chen, Yuyang Li, Runlong Cai, Yiran Li, Chenjuan Deng, Jin Wu, Chao Yan, Hairong Cheng, Yongchun Liu, Markku Kulmala, Jiming Hao, James N. Smith, and Jingkun Jiang
Atmos. Chem. Phys., 23, 14801–14812, https://doi.org/10.5194/acp-23-14801-2023, https://doi.org/10.5194/acp-23-14801-2023, 2023
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Near-continuous measurements show the composition, sources, and seasonal variations of ultrafine particles (UFPs) in urban Beijing. Vehicle and cooking emissions and new particle formation are the main sources of UFPs, and aqueous/heterogeneous processes increase UFP mode diameters. UFPs are the highest in winter due to the highest primary particle emission rates and new particle formation rates, and CHO fractions are the highest in summer due to the strongest photooxidation.
Jiaqi Wang, Jian Gao, Fei Che, Xin Yang, Yuanqin Yang, Lei Liu, Yan Xiang, and Haisheng Li
Atmos. Chem. Phys., 23, 14715–14733, https://doi.org/10.5194/acp-23-14715-2023, https://doi.org/10.5194/acp-23-14715-2023, 2023
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Regional-scale observations of surface O3, PM2.5 and its major chemical species, mixing layer height (MLH), and other meteorological parameters were made in the North China Plain during summer. Unlike the cold season, synchronized increases in MDA8 O3 and PM2.5 under medium MLH conditions have been witnessed. The increasing trend of PM2.5 was associated with enhanced secondary chemical formation. The correlation between MLH and secondary air pollutants should be treated with care in hot seasons.
Takuma Miyakawa, Akinori Ito, Chunmao Zhu, Atsushi Shimizu, Erika Matsumoto, Yusuke Mizuno, and Yugo Kanaya
Atmos. Chem. Phys., 23, 14609–14626, https://doi.org/10.5194/acp-23-14609-2023, https://doi.org/10.5194/acp-23-14609-2023, 2023
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This study conducted semi-continuous measurements of PM2.5 aerosols and their elemental composition in western Japan, during spring 2018. It analyzed the emissions, transport, and wet removal of elements such as Pb, Cu, Fe, and Mn. It also assessed the accuracy of modeled concentrations and found overestimations of BC and underestimations of Cu and anthropogenic Fe in East Asia. Insights into emissions, removals, and source apportionment of trace metals in the East Asian outflow were provided.
Jingjing Meng, Yachen Wang, Yuanyuan Li, Tonglin Huang, Zhifei Wang, Yiqiu Wang, Min Chen, Zhanfang Hou, Houhua Zhou, Keding Lu, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 23, 14481–14503, https://doi.org/10.5194/acp-23-14481-2023, https://doi.org/10.5194/acp-23-14481-2023, 2023
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This study investigated the effect of COVID-19 lockdown (LCD) measures on the formation and evolutionary process of diacids and related compounds from field observations. Results demonstrate that more aged organic aerosols are observed during the LCD due to the enhanced photochemical oxidation. Our study also found that the reactivity of 13C was higher than that of 12C in the gaseous photochemical oxidation, leading to higher δ13C values of C2 during the LCD than before the LCD.
Christopher J. Hennigan, Michael McKee, Vikram Pratap, Bryanna Boegner, Jasper Reno, Lucia Garcia, Madison McLaren, and Sara M. Lance
Atmos. Chem. Phys., 23, 14437–14449, https://doi.org/10.5194/acp-23-14437-2023, https://doi.org/10.5194/acp-23-14437-2023, 2023
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This study characterized the optical properties of light-absorbing organic compounds, called brown carbon (BrC), in atmospheric cloud water samples. In all samples, light absorption by BrC increased linearly with increasing pH. There was variability in the sensitivity of the absorption–pH relationship, depending on the degree of influence from fire emissions. Overall, these results show that the climate forcing of BrC is quite strongly affected by its pH-dependent absorption.
Máté Vörösmarty, Gaëlle Uzu, Jean-Luc Jaffrezo, Pamela Dominutti, Zsófia Kertész, Enikő Papp, and Imre Salma
Atmos. Chem. Phys., 23, 14255–14269, https://doi.org/10.5194/acp-23-14255-2023, https://doi.org/10.5194/acp-23-14255-2023, 2023
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Poor air quality caused by high concentrations of particulate matter is one of the most severe public health concerns for humans worldwide. One of the most important biological mechanisms inducing adverse health effects is the oxidant–antioxidant imbalance. We showed that the oxidative stress changed substantially and in a complex manner with location and season. Biomass burning exhibited the dominant influence, while motor vehicles played an important role in the non-heating period.
Da Lu, Hao Li, Mengke Tian, Guochen Wang, Xiaofei Qin, Na Zhao, Juntao Huo, Fan Yang, Yanfen Lin, Jia Chen, Qingyan Fu, Yusen Duan, Xinyi Dong, Congrui Deng, Sabur F. Abdullaev, and Kan Huang
Atmos. Chem. Phys., 23, 13853–13868, https://doi.org/10.5194/acp-23-13853-2023, https://doi.org/10.5194/acp-23-13853-2023, 2023
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Environmental conditions during dust are usually not favorable for secondary aerosol formation. However in this study, an unusual dust event was captured in a Chinese mega-city and showed “anomalous” meteorology and a special dust backflow transport pathway. The underlying formation mechanisms of secondary aerosols are probed in the context of this special dust event. This study shows significant implications for the varying dust aerosol chemistry in the future changing climate.
Thomas Audoux, Benoit Laurent, Karine Desboeufs, Gael Noyalet, Franck Maisonneuve, Olivier Lauret, and Servanne Chevaillier
Atmos. Chem. Phys., 23, 13485–13503, https://doi.org/10.5194/acp-23-13485-2023, https://doi.org/10.5194/acp-23-13485-2023, 2023
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In the Paris region, a campaign was conducted to study wet deposition of aerosol particles during rainfall events. Simultaneous measurements of aerosol and wet deposition allowed us to discuss their transfer from the atmosphere to rain. Chemical evolution within events revealed meteorology, atmospheric conditions and local vs. long range sources as key factors. This study highlights the variability of wet deposition and the need to consider event-specific factors to understand its mechanisms.
Ting Yang, Yu Xu, Qing Ye, Yi-Jia Ma, Yu-Chen Wang, Jian-Zhen Yu, Yu-Sen Duan, Chen-Xi Li, Hong-Wei Xiao, Zi-Yue Li, Yue Zhao, and Hua-Yun Xiao
Atmos. Chem. Phys., 23, 13433–13450, https://doi.org/10.5194/acp-23-13433-2023, https://doi.org/10.5194/acp-23-13433-2023, 2023
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In this study, 130 OS species were quantified in ambient fine particulate matter (PM2.5) collected in urban and suburban Shanghai (East China) in the summer of 2021. The daytime OS formation was concretized based on the interactions among OSs, ultraviolet (UV), ozone (O3), and sulfate. Our finding provides field evidence for the influence of photochemical process and anthropogenic sulfate on OS formation and has important implications for the mitigation of organic particulate pollution.
Shan Wang, Kezheng Liao, Zijing Zhang, Yuk Ying Cheng, Qiongqiong Wang, Hanzhe Chen, and Jian Zhen Yu
EGUsphere, https://doi.org/10.5194/egusphere-2023-2286, https://doi.org/10.5194/egusphere-2023-2286, 2023
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In this work, hourly primary and secondary organic carbon were estimated by a novel Bayesian inference approach in suburban Hong Kong. Their multi-temporal scale variations and evolution characteristics during PM2.5 episodes were examined. The methodology could serve as a guide for other locations with similar monitoring capabilities. The observation-based results are helpful for understanding the evolving nature of secondary organic aerosols and refining the accuracy of model simulations.
Marco Paglione, David C. S. Beddows, Anna Jones, Thomas Lachlan-Cope, Matteo Rinaldi, Stefano Decesari, Francesco Manarini, Mara Russo, Karam Mansour, Roy M. Harrison, Andrea Mazzanti, Emilio Tagliavini, and Manuel Dall'Osto
EGUsphere, https://doi.org/10.5194/egusphere-2023-2275, https://doi.org/10.5194/egusphere-2023-2275, 2023
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Applying factor analysis techniques to H-NMR spectra, we present the Organic Aerosol (OA) source apportionment of PM1 samples collected in parallel at two peri-Antarctic stations, namely Signy and Halley, important to investigate aerosol-climate interactions in an unperturbed atmosphere. Our results show remarkable differences between pelagic (open ocean) and sympagic (sea-ice influenced) air masses and indicate that various sources and processes are controlling Antarctic aerosols.
Miao Zhong, Jianzhong Xu, Huiqin Wang, Li Gao, Haixia Zhu, Lixiang Zhai, Xinghua Zhang, and Wenhui Zhao
Atmos. Chem. Phys., 23, 12609–12630, https://doi.org/10.5194/acp-23-12609-2023, https://doi.org/10.5194/acp-23-12609-2023, 2023
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This study focus on coal-combustion-dominated aerosol in urban areas in northwestern China and combines the results of optical measurement and chemical analysis to deduce the evolution of these characteristics in the atmosphere, which has previously been unknown. The results provide insights into the effects of atmospheric processes and emissions on brown carbon properties.
Li Wu, Hyo-Jin Eom, Hanjin Yoo, Dhrubajyoti Gupta, Hye-Rin Cho, Pingqing Fu, and Chul-Un Ro
Atmos. Chem. Phys., 23, 12571–12588, https://doi.org/10.5194/acp-23-12571-2023, https://doi.org/10.5194/acp-23-12571-2023, 2023
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Hygroscopicity of ambient marine aerosols is of critical relevance to investigate their atmospheric impacts, which, however, remain uncertain due to their complex compositions and mixing states. Therefore, a study on the hygroscopic behavior of ambient marine aerosols for understanding the phase states when interacting with water vapor at different RH levels and their subsequent impacts on the heterogeneous chemical reactions, atmospheric environment, and human health is of vital importance.
Yutong Liang, Rebecca A. Wernis, Kasper Kristensen, Nathan M. Kreisberg, Philip L. Croteau, Scott C. Herndon, Arthur W. H. Chan, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 23, 12441–12454, https://doi.org/10.5194/acp-23-12441-2023, https://doi.org/10.5194/acp-23-12441-2023, 2023
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We measured the gas–particle partitioning behaviors of biomass burning markers and examined the effect of wildfire organic aerosol on the partitioning of semivolatile organic compounds. Most compounds measured are less volatile than model predictions. Wildfire aerosol enhanced the condensation of polar compounds and caused some nonpolar (e.g., polycyclic aromatic hydrocarbons) compounds to partition into the gas phase, thus affecting their lifetimes in the atmosphere and the mode of exposure.
Bojiang Su, Xinhui Bi, Zhou Zhang, Yue Liang, Congbo Song, Tao Wang, Yaohao Hu, Lei Li, Zhen Zhou, Jinpei Yan, Xinming Wang, and Guohua Zhang
Atmos. Chem. Phys., 23, 10697–10711, https://doi.org/10.5194/acp-23-10697-2023, https://doi.org/10.5194/acp-23-10697-2023, 2023
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During the R/V Xuelong cruise observation over the Ross Sea, Antarctica, the mass concentrations of water-soluble Ca2+ and the mass spectra of individual calcareous particles were measured. Our results indicated that lower temperature, lower wind speed, and the presence of sea ice may facilitate Ca2+ enrichment in sea spray aerosols and highlighted the potential contribution of organically complexed calcium to calcium enrichment, which is inaccurate based solely on water-soluble Ca2+ estimation.
Valeria Mardoñez, Marco Pandolfi, Lucille Joanna S. Borlaza, Jean-Luc Jaffrezo, Andrés Alastuey, Jean-Luc Besombes, Isabel Moreno R., Noemi Perez, Griša Močnik, Patrick Ginot, Radovan Krejci, Vladislav Chrastny, Alfred Wiedensohler, Paolo Laj, Marcos Andrade, and Gaëlle Uzu
Atmos. Chem. Phys., 23, 10325–10347, https://doi.org/10.5194/acp-23-10325-2023, https://doi.org/10.5194/acp-23-10325-2023, 2023
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La Paz and El Alto are two fast-growing, high-altitude Bolivian cities forming the second-largest metropolitan area in the country. The sources of particulate matter (PM) in this conurbation were not previously investigated. This study identified 11 main sources of PM, of which dust and vehicular emissions stand out as the main ones. The influence of regional biomass combustion and local waste combustion was also observed, with the latter being a major source of hazardous compounds.
Sayako Ueda, Yoko Iwamoto, Fumikazu Taketani, Mingxu Liu, and Hitoshi Matsui
Atmos. Chem. Phys., 23, 10117–10135, https://doi.org/10.5194/acp-23-10117-2023, https://doi.org/10.5194/acp-23-10117-2023, 2023
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We examine iron in atmospheric fine aerosol particles collected over the Indian Ocean during shipborne observations in November 2018. Transmission electron microscopy analysis with water dialysis shows that various types of iron (fly ash, iron oxide, and mineral dust) co-exist with ammonium sulfate and that their solubility differs depending on the iron type. Using PM2.5 bulk samples and global model simulations, we elucidate their origins, aging, and implications for present iron simulations.
Farhan R. Nursanto, Roy Meinen, Rupert Holzinger, Maarten C. Krol, Xinya Liu, Ulrike Dusek, Bas Henzing, and Juliane L. Fry
Atmos. Chem. Phys., 23, 10015–10034, https://doi.org/10.5194/acp-23-10015-2023, https://doi.org/10.5194/acp-23-10015-2023, 2023
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Particulate matter (PM) is a harmful air pollutant that depends on the complex mixture of natural and anthropogenic emissions into the atmosphere. Thus, in different regions and seasons, the way that PM is formed and grows can differ. In this study, we use a combined statistical analysis of the chemical composition and particle size distribution to determine what drives particle formation and growth across seasons, using varying wind directions to elucidate the role of different sources.
Kohei Sakata, Aya Sakaguchi, Yoshiaki Yamakawa, Chihiro Miyamoto, Minako Kurisu, and Yoshio Takahashi
Atmos. Chem. Phys., 23, 9815–9836, https://doi.org/10.5194/acp-23-9815-2023, https://doi.org/10.5194/acp-23-9815-2023, 2023
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Anthropogenic iron is the dominant source of dissolved Fe in aerosol particles, but its contribution to dissolved Fe in aerosol particles has not been quantitatively evaluated. We established the molar concentration ratio of dissolved Fe to dissolved Al as a new indicator to evaluate the contribution of anthropogenic iron. As a result, about 10 % of dissolved Fe in aerosol particles was derived from anthropogenic iron when aerosol particles were transported from East Asia to the Pacific Ocean.
Li Li, Qiyuan Wang, Jie Tian, Huikun Liu, Yong Zhang, Steven Sai Hang Ho, Weikang Ran, and Junji Cao
Atmos. Chem. Phys., 23, 9597–9612, https://doi.org/10.5194/acp-23-9597-2023, https://doi.org/10.5194/acp-23-9597-2023, 2023
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The Tibetan Plateau has a unique geographical location, but there is a lack of detailed research on the real-time characteristics of full aerosol composition. This study elaborates the changes in chemical characteristics between transport and local fine particles during the pre-monsoon, reveals the size distribution and the mixing states of different individual particles, and highlights the contributions of photooxidation and aqueous reaction to the formation of the secondary species.
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