Articles | Volume 18, issue 23
Atmos. Chem. Phys., 18, 17307–17323, 2018
https://doi.org/10.5194/acp-18-17307-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 18, 17307–17323, 2018
https://doi.org/10.5194/acp-18-17307-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article 06 Dec 2018
Research article | 06 Dec 2018
The underappreciated role of nonvolatile cations in aerosol ammonium-sulfate molar ratios
Hongyu Guo et al.
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Richard H. Moore, Elizabeth B. Wiggins, Adam T. Ahern, Stephen Zimmerman, Lauren Montgomery, Pedro Campuzano Jost, Claire E. Robinson, Luke D. Ziemba, Edward L. Winstead, Bruce E. Anderson, Charles A. Brock, Matthew D. Brown, Gao Chen, Ewan C. Crosbie, Hongyu Guo, Jose L. Jimenez, Carolyn E. Jordan, Ming Lyu, Benjamin A. Nault, Nicholas E. Rothfuss, Kevin J. Sanchez, Melinda Schueneman, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Nicholas L. Wagner, and Jian Wang
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-21, https://doi.org/10.5194/amt-2021-21, 2021
Preprint under review for AMT
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Atmospheric particles are everywhere and exist in a range of sizes from a few nanometers to hundreds of microns. Because particle size determines the behavior of chemical and physical processes, accurately measuring particle sizes is an important and integral part of atmospheric field measurements! Here, we discuss the performance of two, commonly-used particle sizers and how changes in particle composition and optical properties may result in sizing uncertainties, which we quantify.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Hongyu Guo, Duseong S. Jo, Anne V. Handschy, Demetrios Pagonis, Jason C. Schroder, Melinda K. Schueneman, Michael J. Cubison, Jack E. Dibb, Alma Hodzic, Weiwei Hu, Brett B. Palm, and Jose L. Jimenez
Atmos. Meas. Tech., 13, 6193–6213, https://doi.org/10.5194/amt-13-6193-2020, https://doi.org/10.5194/amt-13-6193-2020, 2020
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Collecting particulate matter, or aerosols, onto filters to be analyzed offline is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
Bingqing Zhang, Huizhong Shen, Pengfei Liu, Hongyu Guo, Yongtao Hu, Yilin Chen, Shaodong Xie, Ziyan Xi, and Armistead G. Russell
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-879, https://doi.org/10.5194/acp-2020-879, 2020
Revised manuscript accepted for ACP
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Large-scale ground-level measurements are coupled with model simulations to comprehensively compare the aerosol acidity in China and the United States. Aerosol in China is significantly less acidic than that in the United States, with pH values 1–2 units higher. The abundance of ammonia and ammonium in China is the leading cause of the pH difference, and the large difference indicates potential distinctions in aerosol formation, composition, and toxicity between these two countries.
Jian Xu, Jia Chen, Na Zhao, Guochen Wang, Guangyuan Yu, Hao Li, Juntao Huo, Yanfen Lin, Qingyan Fu, Hongyu Guo, Congrui Deng, Shan-Hu Lee, Jianmin Chen, and Kan Huang
Atmos. Chem. Phys., 20, 7259–7269, https://doi.org/10.5194/acp-20-7259-2020, https://doi.org/10.5194/acp-20-7259-2020, 2020
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This study provided evidence that gas-particle partitioning of ammonia, as opposed to ammonia concentration, plays a critical role in the haze formation. A reduction in ammonia emissions alone may not reduce air pollution effectively, at least at rural agricultural sites in China.
Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Douglas A. Day, Jason C. Schroder, Jack E. Dibb, Maximilian Dollner, Bernadett Weinzierl, and Jose L. Jimenez
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-224, https://doi.org/10.5194/amt-2020-224, 2020
Revised manuscript accepted for AMT
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We utilize a set of high-quality datasets collected during the NASA ATom aircraft mission to investigate the impact of differences in observable particle sizes across aerosol instruments, in aerosol measurement comparisons. Very good agreement was found between chemically and physically derived submicron aerosol volume. Results support a lack of significant unknown biases in the response of Aerodyne Aerosol Mass Spectrometer (AMS) when sampling remote aerosols across the globe.
Theodora Nah, Yi Ji, David J. Tanner, Hongyu Guo, Amy P. Sullivan, Nga Lee Ng, Rodney J. Weber, and L. Gregory Huey
Atmos. Meas. Tech., 11, 5087–5104, https://doi.org/10.5194/amt-11-5087-2018, https://doi.org/10.5194/amt-11-5087-2018, 2018
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The sources and atmospheric chemistry of gas-phase organic acids are currently poorly understood, due in part to the limited range of measurement techniques available. We evaluated the use of SF6− as a sensitive and selective chemical ionization reagent ion for real-time measurements of gas-phase organic acids at a rural site in Yorkville, Georgia. We found that ambient concentrations of organic acids ranged from a few ppt to several ppb, and are dependent on ambient temperature.
Hongyu Guo, Rene Otjes, Patrick Schlag, Astrid Kiendler-Scharr, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 12241–12256, https://doi.org/10.5194/acp-18-12241-2018, https://doi.org/10.5194/acp-18-12241-2018, 2018
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Reduction in ammonia has been proposed as a way to lower fine particle mass and improve air quality, but gas-phase ammonia is linked to agricultural productivity. We assess the feasibility of ammonia control at a variety of locations through an aerosol thermodynamic analysis. We show that aerosol response to ammonia control is highly nonlinear and only becomes effective when ambient particle pH drops below approximately 3. Particle pH is a relevant aerosol air quality parameter.
Theodora Nah, Hongyu Guo, Amy P. Sullivan, Yunle Chen, David J. Tanner, Athanasios Nenes, Armistead Russell, Nga Lee Ng, L. Gregory Huey, and Rodney J. Weber
Atmos. Chem. Phys., 18, 11471–11491, https://doi.org/10.5194/acp-18-11471-2018, https://doi.org/10.5194/acp-18-11471-2018, 2018
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We present measurements from a field study conducted in an agriculturally intensive region in the southeastern US during the fall of 2016 to investigate how NH3 affects particle acidity and SOA formation via gas–particle partitioning of semi-volatile organic acids. For this study, higher NH3 concentrations relative to what has been measured in the region in previous studies had minor effects on PM1 organic acids and their influence on the overall organic aerosol and PM1 mass concentrations.
Haiyan Li, Qiang Zhang, Bo Zheng, Chunrong Chen, Nana Wu, Hongyu Guo, Yuxuan Zhang, Yixuan Zheng, Xin Li, and Kebin He
Atmos. Chem. Phys., 18, 5293–5306, https://doi.org/10.5194/acp-18-5293-2018, https://doi.org/10.5194/acp-18-5293-2018, 2018
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This study revealed the driving role of nitrate in urban haze development in the North China Plain (NCP) during summertime. Several factors favoring the rapid nitrate formation were investigated in detail. The higher concentration and, in particular, the higher contribution of nitrate in PM1 suggest an urgent need to initiate ammonia emission control measures and further reduce NOx emissions over the NCP region.
Hongyu Guo, Jiumeng Liu, Karl D. Froyd, James M. Roberts, Patrick R. Veres, Patrick L. Hayes, Jose L. Jimenez, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 17, 5703–5719, https://doi.org/10.5194/acp-17-5703-2017, https://doi.org/10.5194/acp-17-5703-2017, 2017
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Fine particle pH is linked to many environmental impacts by affecting particle concentration and composition. Predicted Pasadena, CA (CalNex campaign), PM1 pH is 1.9 and PM2.5 pH 2.7, the latter higher due to sea salts. The model predicted gas–particle partitionings of HNO3–NO3−, NH3–NH4+, and HCl–Cl− are in good agreement, verifying the model predictions. A summary of contrasting locations in the US and eastern Mediterranean shows fine particles are generally highly acidic, with pH below 3.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
H. Guo, L. Xu, A. Bougiatioti, K. M. Cerully, S. L. Capps, J. R. Hite Jr., A. G. Carlton, S.-H. Lee, M. H. Bergin, N. L. Ng, A. Nenes, and R. J. Weber
Atmos. Chem. Phys., 15, 5211–5228, https://doi.org/10.5194/acp-15-5211-2015, https://doi.org/10.5194/acp-15-5211-2015, 2015
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Particle pH can affect many aerosol processes, including gas-particle partitioning, SOA formation, and mobilization of toxic redox metals. pH is challenging to directly measure and often improperly characterized by proxies like ion balances or molar ratios of measured aerosol ionic species. We present a detailed analysis predicting pH with a thermodynamic model, verify the prediction, and test pH sensitivity to model inputs based on data from the SOAS field campaign.
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
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Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
T. K. V. Nguyen, M. D. Petters, S. R. Suda, H. Guo, R. J. Weber, and A. G. Carlton
Atmos. Chem. Phys., 14, 10911–10930, https://doi.org/10.5194/acp-14-10911-2014, https://doi.org/10.5194/acp-14-10911-2014, 2014
J. Liu, M. Bergin, H. Guo, L. King, N. Kotra, E. Edgerton, and R. J. Weber
Atmos. Chem. Phys., 13, 12389–12404, https://doi.org/10.5194/acp-13-12389-2013, https://doi.org/10.5194/acp-13-12389-2013, 2013
Irini Tsiodra, Georgios Grivas, Kalliopi Tavernaraki, Aikaterini Bougiatioti, Maria Apostolaki, Despina Paraskevopoulou, Alexandra Gogou, Constantine Parinos, Konstantina Oikonomou, Maria Tsagkaraki, Pavlos Zarmpas, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-393, https://doi.org/10.5194/acp-2021-393, 2021
Preprint under review for ACP
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We analyze observations from year-long measurements at Athens, Greece. Nighttime wintertime PAH levels are four times higher than daytime, and wintertime values are 15 times higher than summertime. Biomass burning aerosol during wintertime pollution events is responsible for these significant wintertime enhancements, and accounts for 43 % of the population exposure to PAH carcinogenic risk. Biomass burning poses additional health risks beyond those associated with high PM levels that develop.
Spiro Jorga, Kalliopi Florou, Christos Kaltsonoudis, John Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros Pandis
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-284, https://doi.org/10.5194/acp-2021-284, 2021
Preprint under review for ACP
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We test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through oxidation of the emitted organic vapors by the nitrate radical produced during the reaction of ozone and nitrogen oxides. Our experiments using as a starting point the ambient air of an urban area with high biomass burning activity demonstrate that indeed even with sunlight there is 20–70 % additional organic aerosol formed in a few hours.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
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Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Yang Wang, Guangjie Zheng, Michael Jensen, Daniel Knopf, Alexander Laskin, Alyssa Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur Sedlacek, John Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria Zawadowicz, and Jian Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-300, https://doi.org/10.5194/acp-2021-300, 2021
Preprint under review for ACP
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This manuscript reports the vertical profiles of trace gas and aerosol properties over the Eastern North Atlantic, a region of persistent but diverse subtropical marine boundary layer (MBL) clouds. We examined the key processes that drive the cloud condensation nuclei (CCN) population and how it varies with season and synoptic conditions. This study helps improve the model representation of the aerosol processes in the remote MBL, reducing the simulated aerosol indirect effects.
Yuhan Yang, Dong Gao, and Rodney J. Weber
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-72, https://doi.org/10.5194/amt-2021-72, 2021
Preprint under review for AMT
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Iron and copper are commonly found in ambient aerosols and have been linked to adverse health effects. We describe a relatively simple bench-top instrument that can be used to quantify these metals in aqueous solutions and verify the method by comparison with inductively coupled plasma mass spectrometry. The approach is based on forming light absorbing metal-ligand complexes that can be measured with high sensitivity utilizing a long-path liquid waveguide capillary cell.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-173, https://doi.org/10.5194/acp-2021-173, 2021
Preprint under review for ACP
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere, and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
Richard H. Moore, Elizabeth B. Wiggins, Adam T. Ahern, Stephen Zimmerman, Lauren Montgomery, Pedro Campuzano Jost, Claire E. Robinson, Luke D. Ziemba, Edward L. Winstead, Bruce E. Anderson, Charles A. Brock, Matthew D. Brown, Gao Chen, Ewan C. Crosbie, Hongyu Guo, Jose L. Jimenez, Carolyn E. Jordan, Ming Lyu, Benjamin A. Nault, Nicholas E. Rothfuss, Kevin J. Sanchez, Melinda Schueneman, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Nicholas L. Wagner, and Jian Wang
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-21, https://doi.org/10.5194/amt-2021-21, 2021
Preprint under review for AMT
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Atmospheric particles are everywhere and exist in a range of sizes from a few nanometers to hundreds of microns. Because particle size determines the behavior of chemical and physical processes, accurately measuring particle sizes is an important and integral part of atmospheric field measurements! Here, we discuss the performance of two, commonly-used particle sizers and how changes in particle composition and optical properties may result in sizing uncertainties, which we quantify.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Yilin Chen, Huizhong Shen, Jennifer Kaiser, Yongtao Hu, Shannon L. Capps, Shunliu Zhao, Amir Hakami, Jhih-Shyang Shih, Gertrude K. Pavur, Matthew D. Turner, Daven K. Henze, Jaroslav Resler, Athanasios Nenes, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Tianfeng Chai, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, and Armistead G. Russell
Atmos. Chem. Phys., 21, 2067–2082, https://doi.org/10.5194/acp-21-2067-2021, https://doi.org/10.5194/acp-21-2067-2021, 2021
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Ammonia (NH3) emissions can exert adverse impacts on air quality and ecosystem well-being. NH3 emission inventories are viewed as highly uncertain. Here we optimize the NH3 emission estimates in the US using an air quality model and NH3 measurements from the IASI satellite instruments. The optimized NH3 emissions are much higher than the National Emissions Inventory estimates in April. The optimized NH3 emissions improved model performance when evaluated against independent observation.
Jens Redemann, Robert Wood, Paquita Zuidema, Sarah J. Doherty, Bernadette Luna, Samuel E. LeBlanc, Michael S. Diamond, Yohei Shinozuka, Ian Y. Chang, Rei Ueyama, Leonhard Pfister, Ju-Mee Ryoo, Amie N. Dobracki, Arlindo M. da Silva, Karla M. Longo, Meloë S. Kacenelenbogen, Connor J. Flynn, Kristina Pistone, Nichola M. Knox, Stuart J. Piketh, James M. Haywood, Paola Formenti, Marc Mallet, Philip Stier, Andrew S. Ackerman, Susanne E. Bauer, Ann M. Fridlind, Gregory R. Carmichael, Pablo E. Saide, Gonzalo A. Ferrada, Steven G. Howell, Steffen Freitag, Brian Cairns, Brent N. Holben, Kirk D. Knobelspiesse, Simone Tanelli, Tristan S. L'Ecuyer, Andrew M. Dzambo, Ousmane O. Sy, Greg M. McFarquhar, Michael R. Poellot, Siddhant Gupta, Joseph R. O'Brien, Athanasios Nenes, Mary Kacarab, Jenny P. S. Wong, Jennifer D. Small-Griswold, Kenneth L. Thornhill, David Noone, James R. Podolske, K. Sebastian Schmidt, Peter Pilewskie, Hong Chen, Sabrina P. Cochrane, Arthur J. Sedlacek, Timothy J. Lang, Eric Stith, Michal Segal-Rozenhaimer, Richard A. Ferrare, Sharon P. Burton, Chris A. Hostetler, David J. Diner, Felix C. Seidel, Steven E. Platnick, Jeffrey S. Myers, Kerry G. Meyer, Douglas A. Spangenberg, Hal Maring, and Lan Gao
Atmos. Chem. Phys., 21, 1507–1563, https://doi.org/10.5194/acp-21-1507-2021, https://doi.org/10.5194/acp-21-1507-2021, 2021
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Southern Africa produces significant biomass burning emissions whose impacts on regional and global climate are poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA investigation designed to study the key processes that determine these climate impacts. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project, the dataset it produced, and the most important initial findings.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-58, https://doi.org/10.5194/acp-2021-58, 2021
Preprint under review for ACP
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks involving both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlight needs for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Stylianos Kakavas, David Patoulias, Maria Zakoura, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 799–811, https://doi.org/10.5194/acp-21-799-2021, https://doi.org/10.5194/acp-21-799-2021, 2021
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The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles in northern and southern Europe. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 pH units decrease over 2.5 km). The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol.
Georgia Sotiropoulou, Étienne Vignon, Gillian Young, Hugh Morrison, Sebastian J. O'Shea, Thomas Lachlan-Cope, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 21, 755–771, https://doi.org/10.5194/acp-21-755-2021, https://doi.org/10.5194/acp-21-755-2021, 2021
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Summer clouds have a significant impact on the radiation budget of the Antarctic surface and thus on ice-shelf melting. However, these are poorly represented in climate models due to errors in their microphysical structure, including the number of ice crystals that they contain. We show that breakup from ice particle collisions can substantially magnify the ice crystal number concentration with significant implications for surface radiation. This process is currently missing in climate models.
Johannes Quaas, Antti Arola, Brian Cairns, Matthew Christensen, Hartwig Deneke, Annica M. L. Ekman, Graham Feingold, Ann Fridlind, Edward Gryspeerdt, Otto Hasekamp, Zhanqing Li, Antti Lipponen, Po-Lun Ma, Johannes Mülmenstädt, Athanasios Nenes, Joyce E. Penner, Daniel Rosenfeld, Roland Schrödner, Kenneth Sinclair, Odran Sourdeval, Philip Stier, Matthias Tesche, Bastiaan van Diedenhoven, and Manfred Wendisch
Atmos. Chem. Phys., 20, 15079–15099, https://doi.org/10.5194/acp-20-15079-2020, https://doi.org/10.5194/acp-20-15079-2020, 2020
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Anthropogenic pollution particles – aerosols – serve as cloud condensation nuclei and thus increase cloud droplet concentration and the clouds' reflection of sunlight (a cooling effect on climate). This Twomey effect is poorly constrained by models and requires satellite data for better quantification. The review summarizes the challenges in properly doing so and outlines avenues for progress towards a better use of aerosol retrievals and better retrievals of droplet concentrations.
Paraskevi Georgakaki, Aikaterini Bougiatioti, Jörg Wieder, Claudia Mignani, Fabiola Ramelli, Zamin A. Kanji, Jan Henneberger, Maxime Hervo, Alexis Berne, Ulrike Lohmann, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1036, https://doi.org/10.5194/acp-2020-1036, 2020
Revised manuscript under review for ACP
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Aerosol and cloud observations coupled with a droplet activation parameterization was used to investigate the aerosol-cloud droplet link in mixed-phase Alpine clouds. Predicted droplet number, Nd, agrees with observations, and never exceeds a characteristic
limiting droplet number, Ndlim, which depends solely on σw. Nd becomes velocity-limited when it is to within 50 % of Ndlim. Identifying when dynamical changes control Nd variability is central for understanding aerosol-cloud interactions.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Hongyu Guo, Duseong S. Jo, Anne V. Handschy, Demetrios Pagonis, Jason C. Schroder, Melinda K. Schueneman, Michael J. Cubison, Jack E. Dibb, Alma Hodzic, Weiwei Hu, Brett B. Palm, and Jose L. Jimenez
Atmos. Meas. Tech., 13, 6193–6213, https://doi.org/10.5194/amt-13-6193-2020, https://doi.org/10.5194/amt-13-6193-2020, 2020
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Collecting particulate matter, or aerosols, onto filters to be analyzed offline is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
Ari Laaksonen, Jussi Malila, and Athanasios Nenes
Atmos. Chem. Phys., 20, 13579–13589, https://doi.org/10.5194/acp-20-13579-2020, https://doi.org/10.5194/acp-20-13579-2020, 2020
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Aerosol particles containing black carbon are ubiquitous in the atmosphere and originate from combustion processes. We examine their capability to act as condensation centers for water vapor. We make use of published experimental data sets for different types of black carbon particles, ranging from very pure particles to particles that contain both black carbon and water soluble organic matter, and we show that a recently developed theory reproduces most of the experimental results.
Lanxiadi Chen, Chao Peng, Wenjun Gu, Hanjing Fu, Xing Jian, Huanhuan Zhang, Guohua Zhang, Jianxi Zhu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13611–13626, https://doi.org/10.5194/acp-20-13611-2020, https://doi.org/10.5194/acp-20-13611-2020, 2020
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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.
Aikaterini Bougiatioti, Athanasios Nenes, Jack J. Lin, Charles A. Brock, Joost A. de Gouw, Jin Liao, Ann M. Middlebrook, and André Welti
Atmos. Chem. Phys., 20, 12163–12176, https://doi.org/10.5194/acp-20-12163-2020, https://doi.org/10.5194/acp-20-12163-2020, 2020
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The number concentration of droplets in clouds in the summertime in the southeastern United States is influenced by aerosol variations but limited by the strong competition for supersaturated water vapor. Concurrent variations in vertical velocity magnify the response of cloud droplet number to aerosol increases by up to a factor of 5. Omitting the covariance of vertical velocity with aerosol number may therefore bias estimates of the cloud albedo effect from aerosols.
Georgia Sotiropoulou, Luisa Ickes, Athanasios Nenes, and Annica M. L. Ekman
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-786, https://doi.org/10.5194/acp-2020-786, 2020
Revised manuscript under review for ACP
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Mixed-phase clouds are a large source of uncertainty in projections of the Arctic climate. This is partly due to the poor representation of the cloud-ice formation processes. Implementing a parameterization for ice multiplication due to mechanical break-up upon collision of two ice particles in a high resolution model improves cloud-ice phase representation. However, the results are sensitive to poorly constrained microphysical parameters (e.g. ice habit, rimed fraction, autoconversion rate).
Bingqing Zhang, Huizhong Shen, Pengfei Liu, Hongyu Guo, Yongtao Hu, Yilin Chen, Shaodong Xie, Ziyan Xi, and Armistead G. Russell
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-879, https://doi.org/10.5194/acp-2020-879, 2020
Revised manuscript accepted for ACP
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Large-scale ground-level measurements are coupled with model simulations to comprehensively compare the aerosol acidity in China and the United States. Aerosol in China is significantly less acidic than that in the United States, with pH values 1–2 units higher. The abundance of ammonia and ammonium in China is the leading cause of the pH difference, and the large difference indicates potential distinctions in aerosol formation, composition, and toxicity between these two countries.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Preprint under review for ACP
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Yunle Chen, Masayuki Takeuchi, Theodora Nah, Lu Xu, Manjula R. Canagaratna, Harald Stark, Karsten Baumann, Francesco Canonaco, André S. H. Prévôt, L. Gregory Huey, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 20, 8421–8440, https://doi.org/10.5194/acp-20-8421-2020, https://doi.org/10.5194/acp-20-8421-2020, 2020
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Two online mass spectrometry instruments, an aerosol mass spectrometer and a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols, were deployed at Yorkville, GA, for a comprehensive characterization of organic aerosol. We observed notable secondary organic aerosol formation from isoprene and monoterpenes via different pathways during both day and night, and a series of highly oxidized acid-like compounds was found to be closely related to aged SOA.
Shunliu Zhao, Matthew G. Russell, Amir Hakami, Shannon L. Capps, Matthew D. Turner, Daven K. Henze, Peter B. Percell, Jaroslav Resler, Huizhong Shen, Armistead G. Russell, Athanasios Nenes, Amanda J. Pappin, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Charles O. Stanier, and Tianfeng Chai
Geosci. Model Dev., 13, 2925–2944, https://doi.org/10.5194/gmd-13-2925-2020, https://doi.org/10.5194/gmd-13-2925-2020, 2020
Jian Xu, Jia Chen, Na Zhao, Guochen Wang, Guangyuan Yu, Hao Li, Juntao Huo, Yanfen Lin, Qingyan Fu, Hongyu Guo, Congrui Deng, Shan-Hu Lee, Jianmin Chen, and Kan Huang
Atmos. Chem. Phys., 20, 7259–7269, https://doi.org/10.5194/acp-20-7259-2020, https://doi.org/10.5194/acp-20-7259-2020, 2020
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This study provided evidence that gas-particle partitioning of ammonia, as opposed to ammonia concentration, plays a critical role in the haze formation. A reduction in ammonia emissions alone may not reduce air pollution effectively, at least at rural agricultural sites in China.
Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Douglas A. Day, Jason C. Schroder, Jack E. Dibb, Maximilian Dollner, Bernadett Weinzierl, and Jose L. Jimenez
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-224, https://doi.org/10.5194/amt-2020-224, 2020
Revised manuscript accepted for AMT
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We utilize a set of high-quality datasets collected during the NASA ATom aircraft mission to investigate the impact of differences in observable particle sizes across aerosol instruments, in aerosol measurement comparisons. Very good agreement was found between chemically and physically derived submicron aerosol volume. Results support a lack of significant unknown biases in the response of Aerodyne Aerosol Mass Spectrometer (AMS) when sampling remote aerosols across the globe.
Dong Gao, Krystal J. Godri Pollitt, James A. Mulholland, Armistead G. Russell, and Rodney J. Weber
Atmos. Chem. Phys., 20, 5197–5210, https://doi.org/10.5194/acp-20-5197-2020, https://doi.org/10.5194/acp-20-5197-2020, 2020
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This study provides a direct intercomparison between two assays for quantifying oxidative potential (OP) of ambient particles: the synthetic respiratory-tract-lining fluid (RTLF) assay and the dithiothreitol (DTT) assay. The results suggest that the DTT assay and the ascorbic acid depletion in RTLF are associated with organic species, transition metal ions, and antagonistic interactions between species. The glutathione depletion in RTLF is strongly dependent on water-soluble copper.
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.
Athanasios Nenes, Spyros N. Pandis, Rodney J. Weber, and Armistead Russell
Atmos. Chem. Phys., 20, 3249–3258, https://doi.org/10.5194/acp-20-3249-2020, https://doi.org/10.5194/acp-20-3249-2020, 2020
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We show that aerosol acidity (pH) and liquid water content naturally emerge as previously ignored parameters that drive particulate matter formation in the atmosphere, and its sensitivity to emissions of ammonia and nitric acid. The simple framework presented is easily applied to ambient measurements or model output, and it provides the
chemical regimeof PM sensitivity to ammonia and nitric acid availability.
Mary Kacarab, K. Lee Thornhill, Amie Dobracki, Steven G. Howell, Joseph R. O'Brien, Steffen Freitag, Michael R. Poellot, Robert Wood, Paquita Zuidema, Jens Redemann, and Athanasios Nenes
Atmos. Chem. Phys., 20, 3029–3040, https://doi.org/10.5194/acp-20-3029-2020, https://doi.org/10.5194/acp-20-3029-2020, 2020
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We find that extensive biomass burning aerosol plumes from southern Africa can profoundly influence clouds in the southeastern Atlantic. Concurrent variations in vertical velocity, however, are found to magnify the relationship between boundary layer aerosol and the cloud droplet number. Neglecting these covariances may strongly bias the sign and magnitude of aerosol impacts on the cloud droplet number.
Aoxing Zhang, Yuhang Wang, Yuzhong Zhang, Rodney J. Weber, Yongjia Song, Ziming Ke, and Yufei Zou
Atmos. Chem. Phys., 20, 1901–1920, https://doi.org/10.5194/acp-20-1901-2020, https://doi.org/10.5194/acp-20-1901-2020, 2020
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Black carbon (BC) and brown carbon (BrC) are light-absorbing carbonaceous aerosols. We developed a module to simulate the emissions, atmospheric processing and direct radiative effect of BrC in the Community Earth System Model (CESM). We found that globally BrC is a significant absorber and is more centered in the tropical free troposphere compared to BC. The contribution of BrC heating to the Hadley circulation and latitudinal expansion of the tropics is comparable to BC heating.
Arnaldo Negron, Natasha DeLeon-Rodriguez, Samantha M. Waters, Luke D. Ziemba, Bruce Anderson, Michael Bergin, Konstantinos T. Konstantinidis, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1817–1838, https://doi.org/10.5194/acp-20-1817-2020, https://doi.org/10.5194/acp-20-1817-2020, 2020
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Airborne biological particles impact human health, cloud formation, and ecosystems, but few techniques are available to characterize their atmospheric abundance. Combining a newly developed high-volume sampling/flow cytometry technique together with an laser-induced fluorescence instrument, we detect a highly dynamic bioaerosol community over urban Atlanta, composed of pollen, fungi, and bacteria with low and high nucleic acid content.
Georgia Sotiropoulou, Sylvia Sullivan, Julien Savre, Gary Lloyd, Thomas Lachlan-Cope, Annica M. L. Ekman, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1301–1316, https://doi.org/10.5194/acp-20-1301-2020, https://doi.org/10.5194/acp-20-1301-2020, 2020
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Arctic clouds constitute a large source of uncertainty in predictions of future climate. Observations indicate that the number concentration of cloud ice crystals exceeds the concentration of aerosols that can act as ice-nucleating particles (INPs). We show that ice multiplication due to mechanical break-up upon collisions between the few primary ice crystals (formed from INPs) can explain the discrepancy. Including a description of the process in climate models can improve cloud representation.
Michael A. Battaglia Jr., Rodney J. Weber, Athanasios Nenes, and Christopher J. Hennigan
Atmos. Chem. Phys., 19, 14607–14620, https://doi.org/10.5194/acp-19-14607-2019, https://doi.org/10.5194/acp-19-14607-2019, 2019
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The effects of water-soluble organic carbon (WSOC) on aerosol pH were characterized for aqueous-phase particles containing a mixture of inorganics and organics. The ISORROPIA-II and E-AIM models were used in conjunction with AIOMFAC to quantify the effect of organics on aerosol pH through (1) changes to the aerosol liquid water content and (2) changes to the hydrogen ion activity coefficient. The study included both organic acids and nonacids, at RH levels ranging from 70 to 90 %.
Eleni Marinou, Matthias Tesche, Athanasios Nenes, Albert Ansmann, Jann Schrod, Dimitra Mamali, Alexandra Tsekeri, Michael Pikridas, Holger Baars, Ronny Engelmann, Kalliopi-Artemis Voudouri, Stavros Solomos, Jean Sciare, Silke Groß, Florian Ewald, and Vassilis Amiridis
Atmos. Chem. Phys., 19, 11315–11342, https://doi.org/10.5194/acp-19-11315-2019, https://doi.org/10.5194/acp-19-11315-2019, 2019
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We assess the feasibility of ground-based and spaceborne lidars to retrieve profiles of cloud-relevant aerosol concentrations and ice-nucleating particles. The retrieved profiles are in good agreement with airborne in situ measurements. Our methodology will be applied to satellite observations in the future so as to provide a global 3D product of cloud-relevant properties.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Jenny P. S. Wong, Maria Tsagkaraki, Irini Tsiodra, Nikolaos Mihalopoulos, Kalliopi Violaki, Maria Kanakidou, Jean Sciare, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 19, 7319–7334, https://doi.org/10.5194/acp-19-7319-2019, https://doi.org/10.5194/acp-19-7319-2019, 2019
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Biomass burning is a major source of light-absorbing organic species in atmospheric aerosols, and it can play an important role in climate and atmospheric chemistry. Through a combination of laboratory experiments and field observations, this work demonstrated that the light absorption properties of aged biomass burning organic aerosols are dominated by high-molecular-weight compounds. In addition, we found that total hydrated sugars may be a robust tracer for aged biomass burning aerosols.
Panayiotis Kalkavouras, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Maria Tombrou, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 6185–6203, https://doi.org/10.5194/acp-19-6185-2019, https://doi.org/10.5194/acp-19-6185-2019, 2019
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We study how new particle formation (NPF) events affect clouds throughout the year at a ground site in the E Mediterranean. Using a new tools and evaluation metrics, NPF is found to affect only evening and nocturnal clouds by modestly increasing droplet number by 7 to 12 %. A conventional analysis based on CCN concentration at prescribed supersaturation levels or aerosol size can considerably bias the perceived influence of NPF events on regional clouds, the hydrological cycle, and climate.
Nønne L. Prisle, Jack J. Lin, Sara Purdue, Haisheng Lin, J. Carson Meredith, and Athanasios Nenes
Atmos. Chem. Phys., 19, 4741–4761, https://doi.org/10.5194/acp-19-4741-2019, https://doi.org/10.5194/acp-19-4741-2019, 2019
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We measure surface activity and cloud-forming potential of pollenkitt, an organic mixture coating pollen grains. Cloud droplet formation is affected through both surface tension and bulk depletion, with a consistent particle size-dependent signature. We observe nonideal solution effects in pollenkitt mixtures with ammonium sulfate salt. Our results suggest sensitivity of general water interactions, including cloud formation by pollen and their fragments, to both atmospheric humidity and aging.
Sylvia C. Sullivan, Christian Barthlott, Jonathan Crosier, Ilya Zhukov, Athanasios Nenes, and Corinna Hoose
Atmos. Chem. Phys., 18, 16461–16480, https://doi.org/10.5194/acp-18-16461-2018, https://doi.org/10.5194/acp-18-16461-2018, 2018
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Ice crystal formation in clouds can occur via thermodynamic nucleation, but also via mechanical collisions between pre-existing crystals or co-existing droplets. When descriptions of this mechanical ice generation are implemented into the COSMO weather model, we find that the contributions to crystal number from thermodynamic and mechanical processes are of the same order. Mechanical ice generation also intensifies differences in precipitation intensity between dynamic and quiescent regions.
Stelios Myriokefalitakis, Akinori Ito, Maria Kanakidou, Athanasios Nenes, Maarten C. Krol, Natalie M. Mahowald, Rachel A. Scanza, Douglas S. Hamilton, Matthew S. Johnson, Nicholas Meskhidze, Jasper F. Kok, Cecile Guieu, Alex R. Baker, Timothy D. Jickells, Manmohan M. Sarin, Srinivas Bikkina, Rachel Shelley, Andrew Bowie, Morgane M. G. Perron, and Robert A. Duce
Biogeosciences, 15, 6659–6684, https://doi.org/10.5194/bg-15-6659-2018, https://doi.org/10.5194/bg-15-6659-2018, 2018
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The first atmospheric iron (Fe) deposition model intercomparison is presented in this study, as a result of the deliberations of the United Nations Joint Group of Experts on the Scientific Aspects of Marine Environmental Protection (GESAMP; http://www.gesamp.org/) Working Group 38. We conclude that model diversity over remote oceans reflects uncertainty in the Fe content parameterizations of dust aerosols, combustion aerosol emissions and the size distribution of transported aerosol Fe.
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
Theodora Nah, Yi Ji, David J. Tanner, Hongyu Guo, Amy P. Sullivan, Nga Lee Ng, Rodney J. Weber, and L. Gregory Huey
Atmos. Meas. Tech., 11, 5087–5104, https://doi.org/10.5194/amt-11-5087-2018, https://doi.org/10.5194/amt-11-5087-2018, 2018
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The sources and atmospheric chemistry of gas-phase organic acids are currently poorly understood, due in part to the limited range of measurement techniques available. We evaluated the use of SF6− as a sensitive and selective chemical ionization reagent ion for real-time measurements of gas-phase organic acids at a rural site in Yorkville, Georgia. We found that ambient concentrations of organic acids ranged from a few ppt to several ppb, and are dependent on ambient temperature.
Petros Vasilakos, Armistead Russell, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys., 18, 12765–12775, https://doi.org/10.5194/acp-18-12765-2018, https://doi.org/10.5194/acp-18-12765-2018, 2018
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In this work, we investigated the role of emission reductions on aerosol acidity and particulate nitrate. We found that models exhibit positive biases in pH predictions, attributed to very high levels of crustal elements (Mg, Ca, K) in model simulations, which in turn led to an increasing aerosol pH trend over the past decade and allowed nitrate to become an important component of aerosol, which is inconsistent with the measurements, highlighting the importance of accurate pH prediction.
Hongyu Guo, Rene Otjes, Patrick Schlag, Astrid Kiendler-Scharr, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 12241–12256, https://doi.org/10.5194/acp-18-12241-2018, https://doi.org/10.5194/acp-18-12241-2018, 2018
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Reduction in ammonia has been proposed as a way to lower fine particle mass and improve air quality, but gas-phase ammonia is linked to agricultural productivity. We assess the feasibility of ammonia control at a variety of locations through an aerosol thermodynamic analysis. We show that aerosol response to ammonia control is highly nonlinear and only becomes effective when ambient particle pH drops below approximately 3. Particle pH is a relevant aerosol air quality parameter.
Theodora Nah, Hongyu Guo, Amy P. Sullivan, Yunle Chen, David J. Tanner, Athanasios Nenes, Armistead Russell, Nga Lee Ng, L. Gregory Huey, and Rodney J. Weber
Atmos. Chem. Phys., 18, 11471–11491, https://doi.org/10.5194/acp-18-11471-2018, https://doi.org/10.5194/acp-18-11471-2018, 2018
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We present measurements from a field study conducted in an agriculturally intensive region in the southeastern US during the fall of 2016 to investigate how NH3 affects particle acidity and SOA formation via gas–particle partitioning of semi-volatile organic acids. For this study, higher NH3 concentrations relative to what has been measured in the region in previous studies had minor effects on PM1 organic acids and their influence on the overall organic aerosol and PM1 mass concentrations.
Evangelia Kostenidou, Eleni Karnezi, James R. Hite Jr., Aikaterini Bougiatioti, Kate Cerully, Lu Xu, Nga L. Ng, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 5799–5819, https://doi.org/10.5194/acp-18-5799-2018, https://doi.org/10.5194/acp-18-5799-2018, 2018
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The volatility distribution of organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS) was estimated. The volatility distribution of all components covered a wide range including both semi-volatile and low-volatility components. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.
Haiyan Li, Qiang Zhang, Bo Zheng, Chunrong Chen, Nana Wu, Hongyu Guo, Yuxuan Zhang, Yixuan Zheng, Xin Li, and Kebin He
Atmos. Chem. Phys., 18, 5293–5306, https://doi.org/10.5194/acp-18-5293-2018, https://doi.org/10.5194/acp-18-5293-2018, 2018
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This study revealed the driving role of nitrate in urban haze development in the North China Plain (NCP) during summertime. Several factors favoring the rapid nitrate formation were investigated in detail. The higher concentration and, in particular, the higher contribution of nitrate in PM1 suggest an urgent need to initiate ammonia emission control measures and further reduce NOx emissions over the NCP region.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Sylvia C. Sullivan, Corinna Hoose, Alexei Kiselev, Thomas Leisner, and Athanasios Nenes
Atmos. Chem. Phys., 18, 1593–1610, https://doi.org/10.5194/acp-18-1593-2018, https://doi.org/10.5194/acp-18-1593-2018, 2018
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Ice multiplication (IM) processes can have a profound impact on cloud and precipitation development but are poorly understood. Here we study whether a lower limit of ice nuclei exists to initiate IM. The lower limit is found to be extremely low (0.01 per liter or less). A counterintuitive but profound conclusion thus emerges: IM requires cloud formation around a thermodynamic
sweet spotand is sensitive to fluctuations in cloud condensation nuclei concentration alone.
Xuan Wang, Colette L. Heald, Jiumeng Liu, Rodney J. Weber, Pedro Campuzano-Jost, Jose L. Jimenez, Joshua P. Schwarz, and Anne E. Perring
Atmos. Chem. Phys., 18, 635–653, https://doi.org/10.5194/acp-18-635-2018, https://doi.org/10.5194/acp-18-635-2018, 2018
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Brown carbon (BrC) contributes significantly to uncertainty in estimating the global direct radiative effect (DRE) of aerosols. We develop a global model simulation of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental United States. We suggest that BrC DRE has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.
Dong Gao, Ting Fang, Vishal Verma, Linghan Zeng, and Rodney J. Weber
Atmos. Meas. Tech., 10, 2821–2835, https://doi.org/10.5194/amt-10-2821-2017, https://doi.org/10.5194/amt-10-2821-2017, 2017
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This work compares three methods to determine the optimal approach for quantifying the total oxidative potential (OP) of fine particles collected with filters using the dithiothreitol (DTT) assay. An automated system has been developed to facilitate the total OP measurements for use in generation of large data sets needed for epidemiology studies. The results from this study show that the water-insoluble components contribute to PM2.5 OP and the related DTT-active species are largely secondary.
Khairunnisa Yahya, Timothy Glotfelty, Kai Wang, Yang Zhang, and Athanasios Nenes
Geosci. Model Dev., 10, 2333–2363, https://doi.org/10.5194/gmd-10-2333-2017, https://doi.org/10.5194/gmd-10-2333-2017, 2017
Petros Vasilakos, Yong-Ηa Kim, Jeffrey R. Pierce, Sotira Yiacoumi, Costas Tsouris, and Athanasios Nenes
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2017-96, https://doi.org/10.5194/gmd-2017-96, 2017
Revised manuscript not accepted
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Radioactive charging can significantly impact the way radioactive aerosols behave, and as a result their lifetime, but such effects are neglected in predictive model studies of radioactive plumes. We extend a well-established model that simulates the evolution of atmospheric particulate matter to account for radioactive charging effects in an accurate and computationally efficient way. It is shown that radioactivity can strongly impact the deposition patterns of aerosol.
Hongyu Guo, Jiumeng Liu, Karl D. Froyd, James M. Roberts, Patrick R. Veres, Patrick L. Hayes, Jose L. Jimenez, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 17, 5703–5719, https://doi.org/10.5194/acp-17-5703-2017, https://doi.org/10.5194/acp-17-5703-2017, 2017
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Fine particle pH is linked to many environmental impacts by affecting particle concentration and composition. Predicted Pasadena, CA (CalNex campaign), PM1 pH is 1.9 and PM2.5 pH 2.7, the latter higher due to sea salts. The model predicted gas–particle partitionings of HNO3–NO3−, NH3–NH4+, and HCl–Cl− are in good agreement, verifying the model predictions. A summary of contrasting locations in the US and eastern Mediterranean shows fine particles are generally highly acidic, with pH below 3.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Wing Y. Tuet, Yunle Chen, Lu Xu, Shierly Fok, Dong Gao, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 17, 839–853, https://doi.org/10.5194/acp-17-839-2017, https://doi.org/10.5194/acp-17-839-2017, 2017
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Secondary organic aerosols (SOA) comprise a significant fraction of particulate matter (PM) and may have health implications. The water-soluble oxidative potentials of various SOA systems were determined using dithiothreitol consumption. Results from this study demonstrate that precursor identity was more influential than reaction condition in determining SOA oxidative potential and highlight a need to consider SOA contributions from anthropogenic hydrocarbons to PM-induced health effects.
Alexandra Tsekeri, Vassilis Amiridis, Franco Marenco, Athanasios Nenes, Eleni Marinou, Stavros Solomos, Phil Rosenberg, Jamie Trembath, Graeme J. Nott, James Allan, Michael Le Breton, Asan Bacak, Hugh Coe, Carl Percival, and Nikolaos Mihalopoulos
Atmos. Meas. Tech., 10, 83–107, https://doi.org/10.5194/amt-10-83-2017, https://doi.org/10.5194/amt-10-83-2017, 2017
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The In situ/Remote sensing aerosol Retrieval Algorithm (IRRA) provides vertical profiles of aerosol optical, microphysical and hygroscopic properties from airborne in situ and remote sensing measurements. The algorithm is highly advantageous for aerosol characterization in humid conditions, employing the ISORROPIA II model for acquiring the particle hygroscopic growth. IRRA can find valuable applications in aerosol–cloud interaction schemes and in validation of active space-borne sensors.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Panayiotis Kalkavouras, Elissavet Bossioli, Spiros Bezantakos, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Giorgos Kouvarakis, Anna P. Protonotariou, Aggeliki Dandou, George Biskos, Nikolaos Mihalopoulos, Athanasios Nenes, and Maria Tombrou
Atmos. Chem. Phys., 17, 175–192, https://doi.org/10.5194/acp-17-175-2017, https://doi.org/10.5194/acp-17-175-2017, 2017
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Concentrations of chemically and size-resolved submicron aerosol particles along with concentrations of gases and meteorological variables were measured at Santorini and Finokalia (central and southern Aegean Sea) during the Etesians. Particle nucleation bursts were recorded. The NPF can double CCN number (at 0.1 % supersaturation), but the resulting strong competition for water vapor in cloudy updrafts decreases maximum supersaturation by 14 % and augments the potential droplet number by 12 %.
Stelios Myriokefalitakis, Athanasios Nenes, Alex R. Baker, Nikolaos Mihalopoulos, and Maria Kanakidou
Biogeosciences, 13, 6519–6543, https://doi.org/10.5194/bg-13-6519-2016, https://doi.org/10.5194/bg-13-6519-2016, 2016
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The global atmospheric cycle of P is simulated accounting for natural and anthropogenic sources, acid dissolution of dust aerosol and changes in atmospheric acidity. Simulations show that P-containing dust dissolution flux may have increased in the last 150 years but is expected to decrease in the future, and biological particles are important carriers of bioavailable P to the ocean. These insights to the P cycle have important implications for marine ecosystem responses to climate change.
Amelia F. Longo, David J. Vine, Laura E. King, Michelle Oakes, Rodney J. Weber, Lewis Gregory Huey, Armistead G. Russell, and Ellery D. Ingall
Atmos. Chem. Phys., 16, 13389–13398, https://doi.org/10.5194/acp-16-13389-2016, https://doi.org/10.5194/acp-16-13389-2016, 2016
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New synchrotron-based techniques were applied to characterize the oxidation state and composition of sulfur in ambient aerosol and emission sources. Individual particles were found to contain surprisingly high levels of elemental sulfur, a form of sulfur found in only one of the emission sources analyzed. We also show metal sulfates as a key component of urban aerosols. These metal sulfate phases are highly soluble and are indicative of acidic processes transforming metals in the environment.
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.
Aikaterini Bougiatioti, Spiros Bezantakos, Iasonas Stavroulas, Nikos Kalivitis, Panagiotis Kokkalis, George Biskos, Nikolaos Mihalopoulos, Alexandros Papayannis, and Athanasios Nenes
Atmos. Chem. Phys., 16, 7389–7409, https://doi.org/10.5194/acp-16-7389-2016, https://doi.org/10.5194/acp-16-7389-2016, 2016
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BBOA from long-range transport exhibits increased CCN concentrations for particles larger than 100 nm. At the same time the hygroscopicity parameter decreased for all particle sizes, as sub-100 nm particles appear to be richer in less hygroscopic organic material, while larger particles become less hygroscopic due to condensation of less hygroscopic gaseous compounds. Finally, atmospheric processing of freshly emitted BBOA to more oxidized organic aerosol can result in a 2-fold increase of κ.
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237, https://doi.org/10.5194/acp-16-7213-2016, https://doi.org/10.5194/acp-16-7213-2016, 2016
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We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
Weruka Rattanavaraha, Kevin Chu, Sri Hapsari Budisulistiorini, Matthieu Riva, Ying-Hsuan Lin, Eric S. Edgerton, Karsten Baumann, Stephanie L. Shaw, Hongyu Guo, Laura King, Rodney J. Weber, Miranda E. Neff, Elizabeth A. Stone, John H. Offenberg, Zhenfa Zhang, Avram Gold, and Jason D. Surratt
Atmos. Chem. Phys., 16, 4897–4914, https://doi.org/10.5194/acp-16-4897-2016, https://doi.org/10.5194/acp-16-4897-2016, 2016
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The mechanisms by which specific anthropogenic pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected from Birmingham, AL, during the 2013 Southern Oxidant and Aerosol Study (SOAS). Isoprene SOA tracers were measured from these samples and compared to gas and aerosol data collected from the SEARCH network.
Aikaterini Bougiatioti, Panayiota Nikolaou, Iasonas Stavroulas, Giorgos Kouvarakis, Rodney Weber, Athanasios Nenes, Maria Kanakidou, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 16, 4579–4591, https://doi.org/10.5194/acp-16-4579-2016, https://doi.org/10.5194/acp-16-4579-2016, 2016
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Atmospheric aerosols and relevant parameters were measured in the eastern Mediterranean during summer and fall 2012. Submicron aerosol water can contribute up to 33 % of total mass, and 27.5 % of this can be associated with organics. Using these data, the pH of the submicron aerosols was calculated to be highly acidic, varying from 0.5 to 2.8 and independently of air masses origin. Such pH values could increase nutrient availability and thus sea water productivity of the Mediterranean Sea.
Christopher R. Hoyle, Clare S. Webster, Harald E. Rieder, Athanasios Nenes, Emanuel Hammer, Erik Herrmann, Martin Gysel, Nicolas Bukowiecki, Ernest Weingartner, Martin Steinbacher, and Urs Baltensperger
Atmos. Chem. Phys., 16, 4043–4061, https://doi.org/10.5194/acp-16-4043-2016, https://doi.org/10.5194/acp-16-4043-2016, 2016
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A simple statistical model to predict the number of aerosols which activate to form cloud droplets in warm clouds has been established, based on regression analysis of data from the high-altitude site Jungfraujoch. It is found that cloud droplet formation at the Jungfraujoch is predominantly controlled by the number concentration of aerosol particles. A statistical model based on only the number of particles larger than 80nm can explain 79 % of the observed variance in droplet numbers.
Ting Fang, Vishal Verma, Josephine T. Bates, Joseph Abrams, Mitchel Klein, Matthew J. Strickland, Stefanie E. Sarnat, Howard H. Chang, James A. Mulholland, Paige E. Tolbert, Armistead G. Russell, and Rodney J. Weber
Atmos. Chem. Phys., 16, 3865–3879, https://doi.org/10.5194/acp-16-3865-2016, https://doi.org/10.5194/acp-16-3865-2016, 2016
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Ascorbic acid (AA) and Dithiothreitol (DTT) assay measures of water-soluble PM2.5 oxidative potential (OP) are compared in terms of spatiotemporal trends, chemical selectivity, sources, and health impacts based on an epidemiological study with backcast estimated OP. Both assays point to metals from brake/tire wear, but only the DTT assay also identifies organics from combustion. DTT is associated with emergency department visits for asthma/wheeze and congestive heart failure, whereas AA is not.
Yong-ha Kim, Sotira Yiacoumi, Athanasios Nenes, and Costas Tsouris
Atmos. Chem. Phys., 16, 3449–3462, https://doi.org/10.5194/acp-16-3449-2016, https://doi.org/10.5194/acp-16-3449-2016, 2016
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Three microphysical approaches are proposed to incorporate mutual effects of particle charging and coagulation in predictions of transient charge and size distributions of atmospheric particles, including radioactive aerosols. The three approaches have different levels of complexities and are applicable to various laboratory and field atmospheric studies. Also, these approaches can be easily incorporated into aerosol transport models at different scales to account for particle charging effects.
Sylvia C. Sullivan, Ricardo Morales Betancourt, Donifan Barahona, and Athanasios Nenes
Atmos. Chem. Phys., 16, 2611–2629, https://doi.org/10.5194/acp-16-2611-2016, https://doi.org/10.5194/acp-16-2611-2016, 2016
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We use the adjoint model of a cirrus parameterization to quantify sources of crystal variability for various ice-nucleating spectra and output from CAM5.
The sensitivities can be directly linked to nucleation regime and
efficiency of various INP.
The lab-based spectrum calculates much higher INP efficiencies than field-based ones, owing to aerosol surface properties.
The sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters.
L. M. Zamora, R. A. Kahn, M. J. Cubison, G. S. Diskin, J. L. Jimenez, Y. Kondo, G. M. McFarquhar, A. Nenes, K. L. Thornhill, A. Wisthaler, A. Zelenyuk, and L. D. Ziemba
Atmos. Chem. Phys., 16, 715–738, https://doi.org/10.5194/acp-16-715-2016, https://doi.org/10.5194/acp-16-715-2016, 2016
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Based on extensive aircraft campaigns, we quantify how biomass burning smoke affects subarctic and Arctic liquid cloud microphysical properties. Enhanced cloud albedo may decrease short-wave radiative flux by between 2 and 4 Wm2 or more in some subarctic conditions. Smoke halved average cloud droplet diameter. In one case study, it also appeared to limit droplet formation. Numerous Arctic background Aitken particles can also interact with combustion particles, perhaps affecting their properties.
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
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The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
T. Fang, H. Guo, V. Verma, R. E. Peltier, and R. J. Weber
Atmos. Chem. Phys., 15, 11667–11682, https://doi.org/10.5194/acp-15-11667-2015, https://doi.org/10.5194/acp-15-11667-2015, 2015
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This work presented a new method of quantifying water-soluble elements in PM2.5 aqueous extracts (N~500) with an X-ray fluorescence analyzer. The results indicate that water-soluble elements had marked spatial and temporal patterns. Four sources were resolved: brake/tire wear, biomass burning, secondary formation, and mineral dust. The findings have informed studies on aerosol oxidative potential and provided insights into the health effects of water-soluble metals, especially Cu, Fe, Mn and Zn.
N. Kalivitis, V.-M. Kerminen, G. Kouvarakis, I. Stavroulas, A. Bougiatioti, A. Nenes, H. E. Manninen, T. Petäjä, M. Kulmala, and N. Mihalopoulos
Atmos. Chem. Phys., 15, 9203–9215, https://doi.org/10.5194/acp-15-9203-2015, https://doi.org/10.5194/acp-15-9203-2015, 2015
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Cloud condensation nuclei (CCN) production associated with atmospheric new particle formation (NPF) is presented, and this is the first direct evidence of CCN production resulting from NPF in the eastern Mediterranean atmosphere. We show that condensation of both gaseous sulfuric acid and organic compounds from multiple sources leads to the rapid growth of nucleated particles. Sub-100nm particles were found to be substantially less hygroscopic than larger particles during the active NPF period.
S. H. Budisulistiorini, X. Li, S. T. Bairai, J. Renfro, Y. Liu, Y. J. Liu, K. A. McKinney, S. T. Martin, V. F. McNeill, H. O. T. Pye, A. Nenes, M. E. Neff, E. A. Stone, S. Mueller, C. Knote, S. L. Shaw, Z. Zhang, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 15, 8871–8888, https://doi.org/10.5194/acp-15-8871-2015, https://doi.org/10.5194/acp-15-8871-2015, 2015
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Isoprene epoxydiols (IEPOX) are major gas-phase products from the atmospheric oxidation of isoprene that yield secondary organic aerosol (SOA) by reactive uptake onto acidic sulfate aerosol. We report a substantial contribution of IEPOX-derived SOA to the total fine aerosol collected during summer. IEPOX-derived SOA measured by online and offline mass spectrometry techniques is correlated with acidic sulfate aerosol, demonstrating the critical role of anthropogenic emissions in its formation.
K. M. Cerully, A. Bougiatioti, J. R. Hite Jr., H. Guo, L. Xu, N. L. Ng, R. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 8679–8694, https://doi.org/10.5194/acp-15-8679-2015, https://doi.org/10.5194/acp-15-8679-2015, 2015
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The hygroscopicity of SE US aerosol is mostly water-soluble, with a hygroscopicity that is insensitive to partial volatilization in a thermodenuder.
The most and least oxidized components of the aerosol are the most hygroscopic of organic constituents.
No clear relationship was found between organic aerosol hygroscopicity and oxygen-to-carbon ratio.
The aerosol factors covary in a way that induces the observed diurnal invariance in total organic hygroscopicity.
L. Hildebrandt Ruiz, A. L. Paciga, K. M. Cerully, A. Nenes, N. M. Donahue, and S. N. Pandis
Atmos. Chem. Phys., 15, 8301–8313, https://doi.org/10.5194/acp-15-8301-2015, https://doi.org/10.5194/acp-15-8301-2015, 2015
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Secondary organic aerosol (SOA) is transformed after its initial formation. We explored the effects of this chemical aging on the composition, mass yield, volatility, and hygroscopicity of SOA formed from the photo-oxidation of small aromatic volatile organic compounds. Higher exposure to the hydroxyl radical resulted in different SOA composition, average carbon oxidation state, and mass yield. The vapor pressure of SOA formed under different conditions varied by as much as a factor of 30.
J. Liu, E. Scheuer, J. Dibb, G. S. Diskin, L. D. Ziemba, K. L. Thornhill, B. E. Anderson, A. Wisthaler, T. Mikoviny, J. J. Devi, M. Bergin, A. E. Perring, M. Z. Markovic, J. P. Schwarz, P. Campuzano-Jost, D. A. Day, J. L. Jimenez, and R. J. Weber
Atmos. Chem. Phys., 15, 7841–7858, https://doi.org/10.5194/acp-15-7841-2015, https://doi.org/10.5194/acp-15-7841-2015, 2015
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Brown carbon (BrC) is found throughout the US continental troposphere during a summer of extensive biomass burning and its prevalence relative to black carbon (BC) increases with altitude. A radiative transfer model based on direct measurements of aerosol scattering and absorption by BC and BrC shows BrC reduces top-of-atmosphere forcing by 20%. A method to estimate BrC radiative forcing efficiencies from surface-based measurements is provided.
Y. Shinozuka, A. D. Clarke, A. Nenes, A. Jefferson, R. Wood, C. S. McNaughton, J. Ström, P. Tunved, J. Redemann, K. L. Thornhill, R. H. Moore, T. L. Lathem, J. J. Lin, and Y. J. Yoon
Atmos. Chem. Phys., 15, 7585–7604, https://doi.org/10.5194/acp-15-7585-2015, https://doi.org/10.5194/acp-15-7585-2015, 2015
L. Xu, S. Suresh, H. Guo, R. J. Weber, and N. L. Ng
Atmos. Chem. Phys., 15, 7307–7336, https://doi.org/10.5194/acp-15-7307-2015, https://doi.org/10.5194/acp-15-7307-2015, 2015
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Year-long comprehensive characterization of ambient aerosol was performed in both rural and urban sites in the southeastern US as part of Southeastern Center of Air Pollution and Epidemiology (SCAPE) study and Southeastern Oxidant and Aerosol Study (SOAS). Three independent methods were applied to estimate the concentration of particle-phase organic nitrates. The spatial distribution of organic aerosol is investigated by comparing simultaneous HR-ToF-AMS and ACSM measurements at different sites.
S. Myriokefalitakis, N. Daskalakis, N. Mihalopoulos, A. R. Baker, A. Nenes, and M. Kanakidou
Biogeosciences, 12, 3973–3992, https://doi.org/10.5194/bg-12-3973-2015, https://doi.org/10.5194/bg-12-3973-2015, 2015
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The global atmospheric cycle of Fe is simulated accounting for natural and combustion sources, proton- and organic ligand-promoted Fe dissolution from dust aerosol and changes in anthropogenic emissions, and thus in atmospheric acidity. Simulations show that Fe dissolution may have increased in the last 150 years and is expected to decrease due to air pollution regulations. Reductions in dissolved-Fe deposition can further limit the primary productivity over high-nutrient-low-chlorophyll water.
H. Guo, L. Xu, A. Bougiatioti, K. M. Cerully, S. L. Capps, J. R. Hite Jr., A. G. Carlton, S.-H. Lee, M. H. Bergin, N. L. Ng, A. Nenes, and R. J. Weber
Atmos. Chem. Phys., 15, 5211–5228, https://doi.org/10.5194/acp-15-5211-2015, https://doi.org/10.5194/acp-15-5211-2015, 2015
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Particle pH can affect many aerosol processes, including gas-particle partitioning, SOA formation, and mobilization of toxic redox metals. pH is challenging to directly measure and often improperly characterized by proxies like ion balances or molar ratios of measured aerosol ionic species. We present a detailed analysis predicting pH with a thermodynamic model, verify the prediction, and test pH sensitivity to model inputs based on data from the SOAS field campaign.
J. W. Taylor, J. D. Allan, D. Liu, M. Flynn, R. Weber, X. Zhang, B. L. Lefer, N. Grossberg, J. Flynn, and H. Coe
Atmos. Meas. Tech., 8, 1701–1718, https://doi.org/10.5194/amt-8-1701-2015, https://doi.org/10.5194/amt-8-1701-2015, 2015
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When using the SP2 to report black carbon core/shell coating thickness, the core density and refractive index must be estimated from literature values. We systematically vary the assumed parameters and the instrument calibration, and quantify the effects in the derived coatings. The technique is highly sensitive to the core refractive index but has only a minor sensitivity to the core density and coating refractive index. We identify the most appropriate values to use in future analysis.
C. J. Hennigan, J. Izumi, A. P. Sullivan, R. J. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 2775–2790, https://doi.org/10.5194/acp-15-2775-2015, https://doi.org/10.5194/acp-15-2775-2015, 2015
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We show that the ion balance and molar ratio methods are unsuitable for use as aerosol pH proxies. Our recommendation is that 1) thermodynamic equilibrium models constrained by both gas and aerosol inputs run in the forward (open) mode, and 2) the phase partitioning of ammonia provides the best predictions of aerosol pH. Given the significance of acidity for numerous chemical processes in the atmosphere, the implications of this study are important and far reaching.
B. Yuan, P. R. Veres, C. Warneke, J. M. Roberts, J. B. Gilman, A. Koss, P. M. Edwards, M. Graus, W. C. Kuster, S.-M. Li, R. J. Wild, S. S. Brown, W. P. Dubé, B. M. Lerner, E. J. Williams, J. E. Johnson, P. K. Quinn, T. S. Bates, B. Lefer, P. L. Hayes, J. L. Jimenez, R. J. Weber, R. Zamora, B. Ervens, D. B. Millet, B. Rappenglück, and J. A. de Gouw
Atmos. Chem. Phys., 15, 1975–1993, https://doi.org/10.5194/acp-15-1975-2015, https://doi.org/10.5194/acp-15-1975-2015, 2015
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In this work, secondary formation of formic acid at an urban site and a site in an oil and gas production region is studied. We investigated various gas phase formation pathways of formic acid, including those recently proposed, using a box model. The contributions from aerosol-related processes, fog events and air-snow exchange to formic acid are also quantified.
T. Fang, V. Verma, H. Guo, L. E. King, E. S. Edgerton, and R. J. Weber
Atmos. Meas. Tech., 8, 471–482, https://doi.org/10.5194/amt-8-471-2015, https://doi.org/10.5194/amt-8-471-2015, 2015
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This work summarizes a newly developed semi-automated system for quantifying the oxidative potential of aerosol aqueous extracts using the dithiothreitol (DTT) assay. 500 sample analyses indicate that DTT activity in the southeast US is likely not dominated by a unique local source, and sources change with season. The unique large data set generated with the technique described in this paper allows new studies on DTT sources and investigating linkages between reactive oxygen species and health.
V. Verma, T. Fang, H. Guo, L. King, J. T. Bates, R. E. Peltier, E. Edgerton, A. G. Russell, and R. J. Weber
Atmos. Chem. Phys., 14, 12915–12930, https://doi.org/10.5194/acp-14-12915-2014, https://doi.org/10.5194/acp-14-12915-2014, 2014
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The major emission sources of the reactive oxygen species (ROS) associated with ambient particulate matter in the southeastern United States were identified. The study shows biomass burning and secondary aerosol formation as the major sources contributing to the ROS-generating capability of ambient particles. The ubiquitous nature of these two sources suggests widespread population exposures to the toxic aerosol components.
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
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Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
T. K. V. Nguyen, M. D. Petters, S. R. Suda, H. Guo, R. J. Weber, and A. G. Carlton
Atmos. Chem. Phys., 14, 10911–10930, https://doi.org/10.5194/acp-14-10911-2014, https://doi.org/10.5194/acp-14-10911-2014, 2014
R. Morales Betancourt and A. Nenes
Geosci. Model Dev., 7, 2345–2357, https://doi.org/10.5194/gmd-7-2345-2014, https://doi.org/10.5194/gmd-7-2345-2014, 2014
D. Barahona, A. Molod, J. Bacmeister, A. Nenes, A. Gettelman, H. Morrison, V. Phillips, and A. Eichmann
Geosci. Model Dev., 7, 1733–1766, https://doi.org/10.5194/gmd-7-1733-2014, https://doi.org/10.5194/gmd-7-1733-2014, 2014
B. Gantt, J. He, X. Zhang, Y. Zhang, and A. Nenes
Atmos. Chem. Phys., 14, 7485–7497, https://doi.org/10.5194/acp-14-7485-2014, https://doi.org/10.5194/acp-14-7485-2014, 2014
S. H. Budisulistiorini, M. R. Canagaratna, P. L. Croteau, K. Baumann, E. S. Edgerton, M. S. Kollman, N. L. Ng, V. Verma, S. L. Shaw, E. M. Knipping, D. R. Worsnop, J. T. Jayne, R.J. Weber, and J. D. Surratt
Atmos. Meas. Tech., 7, 1929–1941, https://doi.org/10.5194/amt-7-1929-2014, https://doi.org/10.5194/amt-7-1929-2014, 2014
G. Drozd, J. Woo, S. A. K. Häkkinen, A. Nenes, and V. F. McNeill
Atmos. Chem. Phys., 14, 5205–5215, https://doi.org/10.5194/acp-14-5205-2014, https://doi.org/10.5194/acp-14-5205-2014, 2014
S. Romakkaniemi, A. Jaatinen, A. Laaksonen, A. Nenes, and T. Raatikainen
Atmos. Meas. Tech., 7, 1377–1384, https://doi.org/10.5194/amt-7-1377-2014, https://doi.org/10.5194/amt-7-1377-2014, 2014
A. Bougiatioti, I. Stavroulas, E. Kostenidou, P. Zarmpas, C. Theodosi, G. Kouvarakis, F. Canonaco, A. S. H. Prévôt, A. Nenes, S. N. Pandis, and N. Mihalopoulos
Atmos. Chem. Phys., 14, 4793–4807, https://doi.org/10.5194/acp-14-4793-2014, https://doi.org/10.5194/acp-14-4793-2014, 2014
R. Morales Betancourt and A. Nenes
Atmos. Chem. Phys., 14, 4809–4826, https://doi.org/10.5194/acp-14-4809-2014, https://doi.org/10.5194/acp-14-4809-2014, 2014
J. Liu, M. Bergin, H. Guo, L. King, N. Kotra, E. Edgerton, and R. J. Weber
Atmos. Chem. Phys., 13, 12389–12404, https://doi.org/10.5194/acp-13-12389-2013, https://doi.org/10.5194/acp-13-12389-2013, 2013
M. Trail, A. P. Tsimpidi, P. Liu, K. Tsigaridis, Y. Hu, A. Nenes, and A. G. Russell
Geosci. Model Dev., 6, 1429–1445, https://doi.org/10.5194/gmd-6-1429-2013, https://doi.org/10.5194/gmd-6-1429-2013, 2013
Y. Cheng, G. Engling, K.-B. He, F.-K. Duan, Y.-L. Ma, Z.-Y. Du, J.-M. Liu, M. Zheng, and R. J. Weber
Atmos. Chem. Phys., 13, 7765–7781, https://doi.org/10.5194/acp-13-7765-2013, https://doi.org/10.5194/acp-13-7765-2013, 2013
L. E. King and R. J. Weber
Atmos. Meas. Tech., 6, 1647–1658, https://doi.org/10.5194/amt-6-1647-2013, https://doi.org/10.5194/amt-6-1647-2013, 2013
S. Lance, T. Raatikainen, T. B. Onasch, D. R. Worsnop, X.-Y. Yu, M. L. Alexander, M. R. Stolzenburg, P. H. McMurry, J. N. Smith, and A. Nenes
Atmos. Chem. Phys., 13, 5049–5062, https://doi.org/10.5194/acp-13-5049-2013, https://doi.org/10.5194/acp-13-5049-2013, 2013
R. H. Moore, V. A. Karydis, S. L. Capps, T. L. Lathem, and A. Nenes
Atmos. Chem. Phys., 13, 4235–4251, https://doi.org/10.5194/acp-13-4235-2013, https://doi.org/10.5194/acp-13-4235-2013, 2013
T. L. Lathem, A. J. Beyersdorf, K. L. Thornhill, E. L. Winstead, M. J. Cubison, A. Hecobian, J. L. Jimenez, R. J. Weber, B. E. Anderson, and A. Nenes
Atmos. Chem. Phys., 13, 2735–2756, https://doi.org/10.5194/acp-13-2735-2013, https://doi.org/10.5194/acp-13-2735-2013, 2013
M. Frosch, M. Bilde, A. Nenes, A. P. Praplan, Z. Jurányi, J. Dommen, M. Gysel, E. Weingartner, and U. Baltensperger
Atmos. Chem. Phys., 13, 2283–2297, https://doi.org/10.5194/acp-13-2283-2013, https://doi.org/10.5194/acp-13-2283-2013, 2013
Y. C. Sud, D. Lee, L. Oreopoulos, D. Barahona, A. Nenes, and M. J. Suarez
Geosci. Model Dev., 6, 57–79, https://doi.org/10.5194/gmd-6-57-2013, https://doi.org/10.5194/gmd-6-57-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Measurement report: Fourteen months of real-time characterisation of the submicronic aerosol and its atmospheric dynamics at the Marseille–Longchamp supersite
Trends, composition, and sources of carbonaceous aerosol at the Birkenes Observatory, northern Europe, 2001–2018
Enhancement of nanoparticle formation and growth during the COVID-19 lockdown period in urban Beijing
Chemical composition and source attribution of sub-micrometre aerosol particles in the summertime Arctic lower troposphere
In-depth characterization of submicron particulate matter inter-annual variations at a street canyon site in northern Europe
Measurement report: Firework impacts on air quality in Metro Manila, Philippines, during the 2019 New Year revelry
Chemical composition of PM2.5 in October 2017 Northern California wildfire plumes
Atmospheric conditions and composition that influence PM2.5 oxidative potential in Beijing, China
Organic aerosol volatility and viscosity in the North China Plain: contrast between summer and winter
Disparities in particulate matter (PM10) origins and oxidative potential at a city scale (Grenoble, France) – Part 1: Source apportionment at three neighbouring sites
Measurement report: Comparison of wintertime individual particles at ground level and above the mixed layer in urban Beijing
Aerosol characteristics at the Southern Great Plains site during the HI-SCALE campaign
A two-component parameterization of marine ice-nucleating particles based on seawater biology and sea spray aerosol measurements in the Mediterranean Sea
Seasonal variations in the highly time-resolved aerosol composition, sources and chemical processes of background submicron particles in the North China Plain
Concerted measurements of lipids in seawater and on submicrometer aerosol particles at the Cabo Verde islands: biogenic sources, selective transfer and high enrichments
Measurement report: Long-range transport patterns into the tropical northwest Pacific during the CAMP2Ex aircraft campaign: chemical composition, size distributions, and the impact of convection
Identification and source attribution of organic compounds in ultrafine particles near Frankfurt International Airport
Source apportionment and impact of long-range transport on carbonaceous aerosol particles in central Germany during HCCT-2010
Measurement report: PM2.5-bound nitrated aromatic compounds in Xi'an, Northwest China – seasonal variations and contributions to optical properties of brown carbon
Compositions and mixing states of aerosol particles by aircraft observations in the Arctic springtime, 2018
Measurement report: Chemical characteristics of PM2.5 during typical biomass burning season at an agricultural site of the North China Plain
Measurement report: Spatial variations in ionic chemistry and water-stable isotopes in the snowpack on glaciers across Svalbard during the 2015–2016 snow accumulation season
Organosulfates in atmospheric aerosols in Shanghai, China: seasonal and interannual variability, origin, and formation mechanisms
Measurement report: Hydrolyzed amino acids in fine and coarse atmospheric aerosol in Nanchang, China: concentrations, compositions, sources and possible bacterial degradation state
Sulfuric acid–amine nucleation in urban Beijing
Persistent residential burning-related primary organic particles during wintertime hazes in North China: insights into their aging and optical changes
Concentrations, particle-size distributions, and dry deposition fluxes of aerosol trace elements over the Antarctic Peninsula in austral summer
Characteristics, primary sources and secondary formation of water-soluble organic aerosols in downtown Beijing
Measurement report: Effects of photochemical aging on the formation and evolution of summertime secondary aerosol in Beijing
Increased new particle yields with largely decreased probability of survival to CCN size at the summit of Mt. Tai under reduced SO2 emissions
Physical and chemical properties of urban aerosols in São Paulo, Brazil: Links between composition and size distribution of submicron particles
Enhancement of secondary aerosol formation by reduced anthropogenic emissions during Spring Festival 2019 and enlightenment for regional PM2.5 control in Beijing
Linking marine phytoplankton emissions, meteorological processes, and downwind particle properties with FLEXPART
Highly time-resolved measurements of element concentrations in PM10 and PM2.5: comparison of Delhi, Beijing, London, and Krakow
Measurement report: Molecular composition, optical properties, and radiative effects of water-soluble organic carbon in snowpack samples from Northern Xinjiang, China
Atmospheric evolution of emissions from a boreal forest fire: the formation of highly functionalized oxygen-, nitrogen-, and sulfur-containing organic compounds
Concerted measurements of free amino acids at the Cabo Verde islands: high enrichments in submicron sea spray aerosol particles and cloud droplets
Investigating three patterns of new particles growing to the size of cloud condensation nuclei in Beijing's urban atmosphere
Cultivable, halotolerant ice nucleating bacteria and fungi in coastal precipitation
Substantial changes of gaseous pollutants and chemical compositions in fine particles in North China Plain during COVID-19 lockdown period: anthropogenic vs meteorological influences
Measurement report: dual-carbon isotopic characterization of carbonaceous aerosol reveals different primary and secondary sources in Beijing and Xi'an during severe haze events
North Atlantic marine organic aerosol characterized by novel offline thermal desorption mass spectrometry: polysaccharides, recalcitrant material, and secondary organics
Sources and characteristics of size-resolved particulate organic acids and methanesulfonate in a coastal megacity: Manila, Philippines
Effects of AIR pollution on cardiopuLmonary disEaSe in urban and peri-urban reSidents in Beijing: protocol for the AIRLESS study
Chemical composition and source apportionment of atmospheric aerosols on the Namibian coast
Exploring the drivers of the increased ozone production in Beijing in summertime during 2005–2016
Increase of secondary organic aerosol over four years in an urban environment
Optical source apportionment and radiative effect of light-absorbing carbonaceous aerosols in a tropical marine monsoon climate zone: the importance of ship emissions
Measurement report: Seasonality, distribution and sources of organophosphate esters in PM2.5 from an inland urban city in Southwest China
Nationwide increase of polycyclic aromatic hydrocarbons in ultrafine particles during winter over China revealed by size-segregated measurements
Benjamin Chazeau, Brice Temime-Roussel, Grégory Gille, Boualem Mesbah, Barbara D'Anna, Henri Wortham, and Nicolas Marchand
Atmos. Chem. Phys., 21, 7293–7319, https://doi.org/10.5194/acp-21-7293-2021, https://doi.org/10.5194/acp-21-7293-2021, 2021
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The temporal trends in the chemical composition and particle number of the submicron aerosols in a Mediterranean city, Marseille, are investigated over 14 months. Fifteen days were found to exceed the WHO PM2.5 daily limit (25 µg m−3) only during the cold period, with two distinct origins: local pollution events with an increased fraction of the carbonaceous fraction due to domestic wood burning and long-range pollution events with a high level of oxygenated organic aerosol and ammonium nitrate.
Karl Espen Yttri, Francesco Canonaco, Sabine Eckhardt, Nikolaos Evangeliou, Markus Fiebig, Hans Gundersen, Anne-Gunn Hjellbrekke, Cathrine Lund Myhre, Stephen Matthew Platt, André S. H. Prévôt, David Simpson, Sverre Solberg, Jason Surratt, Kjetil Tørseth, Hilde Uggerud, Marit Vadset, Xin Wan, and Wenche Aas
Atmos. Chem. Phys., 21, 7149–7170, https://doi.org/10.5194/acp-21-7149-2021, https://doi.org/10.5194/acp-21-7149-2021, 2021
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Carbonaceous aerosol sources and trends were studied at the Birkenes Observatory. A large decrease in elemental carbon (EC; 2001–2018) and a smaller decline in levoglucosan (2008–2018) suggest that organic carbon (OC)/EC from traffic/industry is decreasing, whereas the abatement of OC/EC from biomass burning has been less successful. Positive matrix factorization apportioned 72 % of EC to fossil fuel sources and 53 % (PM2.5) and 78 % (PM10–2.5) of OC to biogenic sources.
Xiaojing Shen, Junying Sun, Fangqun Yu, Ying Wang, Junting Zhong, Yangmei Zhang, Xinyao Hu, Can Xia, Sinan Zhang, and Xiaoye Zhang
Atmos. Chem. Phys., 21, 7039–7052, https://doi.org/10.5194/acp-21-7039-2021, https://doi.org/10.5194/acp-21-7039-2021, 2021
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In this work, we revealed the changes of PNSD and NPF events during the COVID-19 lockdown period in Beijing, China, to illustrate the impact of reduced primary emission and elavated atmospheric oxidized capicity on the nucleation and growth processes. The subsequent growth of nucleated particles and their contribution to the aerosol pollution formation were also explored, to highlight the necessity of controlling the nanoparticles in the future air quality management.
Franziska Köllner, Johannes Schneider, Megan D. Willis, Hannes Schulz, Daniel Kunkel, Heiko Bozem, Peter Hoor, Thomas Klimach, Frank Helleis, Julia Burkart, W. Richard Leaitch, Amir A. Aliabadi, Jonathan P. D. Abbatt, Andreas B. Herber, and Stephan Borrmann
Atmos. Chem. Phys., 21, 6509–6539, https://doi.org/10.5194/acp-21-6509-2021, https://doi.org/10.5194/acp-21-6509-2021, 2021
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We present in situ observations of vertically resolved particle chemical composition in the summertime Arctic lower troposphere. Our analysis demonstrates the strong vertical contrast between particle properties within the boundary layer and aloft. Emissions from vegetation fires and anthropogenic sources in northern Canada, Europe, and East Asia influenced particle composition in the free troposphere. Organics detected in Arctic aerosol particles can partly be identified as dicarboxylic acids.
Luis M. F. Barreira, Aku Helin, Minna Aurela, Kimmo Teinilä, Milla Friman, Leena Kangas, Jarkko V. Niemi, Harri Portin, Anu Kousa, Liisa Pirjola, Topi Rönkkö, Sanna Saarikoski, and Hilkka Timonen
Atmos. Chem. Phys., 21, 6297–6314, https://doi.org/10.5194/acp-21-6297-2021, https://doi.org/10.5194/acp-21-6297-2021, 2021
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We present results from the long-term measurements (5 years) of highly time-resolved atmospheric PM1 composition at an urban street canyon site. Overall, the results increased knowledge of the variability of PM1 concentration, composition, and sources in a traffic site and the implications for urban air quality. The investigation of pollution episodes showed that both local and long-range-transported pollutants can still cause elevated PM1 and PM2.5 concentrations in northern Europe.
Genevieve Rose Lorenzo, Paola Angela Bañaga, Maria Obiminda Cambaliza, Melliza Templonuevo Cruz, Mojtaba AzadiAghdam, Avelino Arellano, Grace Betito, Rachel Braun, Andrea F. Corral, Hossein Dadashazar, Eva-Lou Edwards, Edwin Eloranta, Robert Holz, Gabrielle Leung, Lin Ma, Alexander B. MacDonald, Jeffrey S. Reid, James Bernard Simpas, Connor Stahl, Shane Marie Visaga, and Armin Sorooshian
Atmos. Chem. Phys., 21, 6155–6173, https://doi.org/10.5194/acp-21-6155-2021, https://doi.org/10.5194/acp-21-6155-2021, 2021
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Firework emissions change the physicochemical and optical properties of water-soluble particles, which subsequently alters the background aerosol’s respirability, influence on surroundings, ability to uptake gases, and viability as cloud condensation nuclei (CCN). There was heavy aerosol loading due to fireworks in the boundary layer. The aerosol constituents were largely water-soluble and submicrometer in size due to both inorganic salts in firework materials and gas-to-particle conversion.
Yutong Liang, Coty N. Jen, Robert J. Weber, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 21, 5719–5737, https://doi.org/10.5194/acp-21-5719-2021, https://doi.org/10.5194/acp-21-5719-2021, 2021
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This article reports the molecular composition of smoke particles people in SF Bay Area were exposed to during northern California wildfires in Oct. 2017. Major components are sugars, acids, aromatics, and terpenoids. These observations can be used to better understand health impacts of smoke exposure. Tracer compounds indicate which fuels burned, including diterpenoids for softwood and syringyls for hardwood. A statistical analysis reveals a group of secondary compounds formed in daytime aging.
Steven J. Campbell, Kate Wolfer, Battist Utinger, Joe Westwood, Zhi-Hui Zhang, Nicolas Bukowiecki, Sarah S. Steimer, Tuan V. Vu, Jingsha Xu, Nicholas Straw, Steven Thomson, Atallah Elzein, Yele Sun, Di Liu, Linjie Li, Pingqing Fu, Alastair C. Lewis, Roy M. Harrison, William J. Bloss, Miranda Loh, Mark R. Miller, Zongbo Shi, and Markus Kalberer
Atmos. Chem. Phys., 21, 5549–5573, https://doi.org/10.5194/acp-21-5549-2021, https://doi.org/10.5194/acp-21-5549-2021, 2021
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In this study, we quantify PM2.5 oxidative potential (OP), a metric widely suggested as a potential measure of particle toxicity, in Beijing in summer and winter using four acellular assays. We correlate PM2.5 OP with a comprehensive range of atmospheric and particle composition measurements, demonstrating inter-assay differences and seasonal variation of PM2.5 OP. Using multivariate statistical analysis, we highlight specific particle chemical components and sources that influence OP.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Lucille Joanna S. Borlaza, Samuël Weber, Gaëlle Uzu, Véronique Jacob, Trishalee Cañete, Steve Micallef, Cécile Trébuchon, Rémy Slama, Olivier Favez, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 21, 5415–5437, https://doi.org/10.5194/acp-21-5415-2021, https://doi.org/10.5194/acp-21-5415-2021, 2021
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This study focuses on fully discriminating the origins of particulates by tackling specific secondary organic aerosol (SOA) sources that are difficult to resolve using traditional datasets, especially at a city scale. This is done through the use of additional fit-for-purpose tracers in the Positive Matrix Factorization (PMF) model, which can be obtained using simpler and more targeted techniques, and the comparison of the PMF models from sites in close range but with different urban typologies.
Wenhua Wang, Longyi Shao, Claudio Mazzoleni, Yaowei Li, Simone Kotthaus, Sue Grimmond, Janarjan Bhandari, Jiaoping Xing, Xiaolei Feng, Mengyuan Zhang, and Zongbo Shi
Atmos. Chem. Phys., 21, 5301–5314, https://doi.org/10.5194/acp-21-5301-2021, https://doi.org/10.5194/acp-21-5301-2021, 2021
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We compared the characteristics of individual particles at ground level and above the mixed-layer height. We found that the particles above the mixed-layer height during haze periods are more aged compared to ground level. More coal-combustion-related primary organic particles were found above the mixed-layer height. We suggest that the particles above the mixed-layer height are affected by the surrounding areas, and once mixed down to the ground, they might contribute to ground air pollution.
Jiumeng Liu, Liz Alexander, Jerome D. Fast, Rodica Lindenmaier, and John E. Shilling
Atmos. Chem. Phys., 21, 5101–5116, https://doi.org/10.5194/acp-21-5101-2021, https://doi.org/10.5194/acp-21-5101-2021, 2021
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To bridge the gaps in modeling and observational results due to insufficient understanding of aerosol properties, co-located measurements of aerosols and trace gases were conducted at SGP during the HI-SCALE campaign. Organic aerosols at the SGP site exhibited to be highly oxidized, and biogenic emissions appear to largely control the formation of organic aerosols. Seasonal variations of sources and meteorological impacts likely resulted in the highly oxygenated feature of aerosols.
Jonathan V. Trueblood, Alessia Nicosia, Anja Engel, Birthe Zäncker, Matteo Rinaldi, Evelyn Freney, Melilotus Thyssen, Ingrid Obernosterer, Julie Dinasquet, Franco Belosi, Antonio Tovar-Sánchez, Araceli Rodriguez-Romero, Gianni Santachiara, Cécile Guieu, and Karine Sellegri
Atmos. Chem. Phys., 21, 4659–4676, https://doi.org/10.5194/acp-21-4659-2021, https://doi.org/10.5194/acp-21-4659-2021, 2021
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Sea spray aerosols (SSAs) can be an important source of ice-nucleating particles (INPs) that impact cloud properties over the oceans. In the Mediterranean Sea, we found that the INPs in the seawater surface microlayer increased by an order of magnitude after a rain dust event that impacted iron and bacterial abundances. The INP properties of SSA (INPSSA) increased after a 3 d delay. Outside this event, INPSSA could be parameterized as a function of the seawater biogeochemistry.
Jiayun Li, Liming Cao, Wenkang Gao, Lingyan He, Yingchao Yan, Yuexin He, Yuepeng Pan, Dongsheng Ji, Zirui Liu, and Yuesi Wang
Atmos. Chem. Phys., 21, 4521–4539, https://doi.org/10.5194/acp-21-4521-2021, https://doi.org/10.5194/acp-21-4521-2021, 2021
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For the first time, we investigated the highly time-resolved chemical characterization, sources and evolution of atmospheric submicron aerosols at a regional background site in the North China Plain (NCP) using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer and evaluated the seasonal differentials of photochemical and aqueous-phase processing on SOA composition and oxidation degree of OA. The results will help to understand air pollution in the NCP on a regional scale.
Nadja Triesch, Manuela van Pinxteren, Sanja Frka, Christian Stolle, Tobias Spranger, Erik Hans Hoffmann, Xianda Gong, Heike Wex, Detlef Schulz-Bull, Blaženka Gašparović, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 4267–4283, https://doi.org/10.5194/acp-21-4267-2021, https://doi.org/10.5194/acp-21-4267-2021, 2021
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To investigate the source of lipids and their representatives in the marine atmosphere, concerted measurements of seawater and submicrometer aerosol particle sampling were carried out on the Cabo Verde islands. This field study describes the biogenic sources of lipids, their selective transfer from the ocean into the atmosphere and their enrichment as part of organic matter. A strong enrichment of the studied representatives of the lipid classes on submicrometer aerosol particles was observed.
Miguel Ricardo A. Hilario, Ewan Crosbie, Michael Shook, Jeffrey S. Reid, Maria Obiminda L. Cambaliza, James Bernard B. Simpas, Luke Ziemba, Joshua P. DiGangi, Glenn S. Diskin, Phu Nguyen, F. Joseph Turk, Edward Winstead, Claire E. Robinson, Jian Wang, Jiaoshi Zhang, Yang Wang, Subin Yoon, James Flynn, Sergio L. Alvarez, Ali Behrangi, and Armin Sorooshian
Atmos. Chem. Phys., 21, 3777–3802, https://doi.org/10.5194/acp-21-3777-2021, https://doi.org/10.5194/acp-21-3777-2021, 2021
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This study characterizes long-range transport from major Asian pollution sources into the tropical northwest Pacific and the impact of scavenging on these air masses. We combined aircraft observations, HYSPLIT trajectories, reanalysis, and satellite retrievals to reveal distinct composition and size distribution profiles associated with specific emission sources and wet scavenging. The results of this work have implications for international policymaking related to climate and health.
Florian Ungeheuer, Dominik van Pinxteren, and Alexander L. Vogel
Atmos. Chem. Phys., 21, 3763–3775, https://doi.org/10.5194/acp-21-3763-2021, https://doi.org/10.5194/acp-21-3763-2021, 2021
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We analysed the chemical composition of ultrafine particles from 10–56 nm near Frankfurt Airport based on cascade impactor samples. We used an offline non-target screening to determine size-resolved molecular fingerprints. Unambiguous attribution of two homologous ester series to jet engine oils enables a new strategy of source attribution and explains the majority of the detected compounds. In addition, we identified additives of jet oils and a detrimental thermal transformation product.
Laurent Poulain, Benjamin Fahlbusch, Gerald Spindler, Konrad Müller, Dominik van Pinxteren, Zhijun Wu, Yoshiteru Iinuma, Wolfram Birmili, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 3667–3684, https://doi.org/10.5194/acp-21-3667-2021, https://doi.org/10.5194/acp-21-3667-2021, 2021
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We present results from source apportionment analysis on the carbonaceous aerosol particles, including organic aerosol (OA) and equivalent black carbon (eBC), allowing us to distinguish local emissions from long-range transport for OA and eBC sources. By merging online chemical measurements and considering particle number size distribution, the different air masses reaching the sampling place were described and discussed, based on their respective chemical composition and size distribution.
Wei Yuan, Ru-Jin Huang, Lu Yang, Ting Wang, Jing Duan, Jie Guo, Haiyan Ni, Yang Chen, Qi Chen, Yongjie Li, Ulrike Dusek, Colin O'Dowd, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3685–3697, https://doi.org/10.5194/acp-21-3685-2021, https://doi.org/10.5194/acp-21-3685-2021, 2021
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We characterized the seasonal variations in nitrated aromatic compounds (NACs) in composition, sources, and their light absorption contribution to brown carbon (BrC) aerosol in Xi'an, Northwest China. Our results show that secondary formation and vehicular emission were dominant sources in summer (~80 %), and biomass burning and coal combustion were major sources in winter (~75 %), and they indicate that the composition and sources of NACs have a profound impact on the light absorption of BrC
Kouji Adachi, Naga Oshima, Sho Ohata, Atsushi Yoshida, Nobuhiro Moteki, and Makoto Koike
Atmos. Chem. Phys., 21, 3607–3626, https://doi.org/10.5194/acp-21-3607-2021, https://doi.org/10.5194/acp-21-3607-2021, 2021
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Aerosol particles influence the Arctic climate by interacting with solar radiation, forming clouds, and melting surface snow and ice. Individual-particle analyses using transmission electron microscopy (TEM) and model simulations provide evidence of biomass burning and anthropogenic contributions to the Arctic aerosols by showing a wide range of compositions and mixing states depending on sampling altitude. Our results reveal the aerosol aging processes and climate influences in the Arctic.
Linlin Liang, Guenter Engling, Chang Liu, Wanyun Xu, Xuyan Liu, Yuan Cheng, Zhenyu Du, Gen Zhang, Junying Sun, and Xiaoye Zhang
Atmos. Chem. Phys., 21, 3181–3192, https://doi.org/10.5194/acp-21-3181-2021, https://doi.org/10.5194/acp-21-3181-2021, 2021
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A unique episode with extreme biomass burning (BB) impact, with daily concentration of levoglucosan as high as 4.37 µg m-3, was captured at an area upwind of Beijing. How this extreme BB pollution event was generated and what were the chemical properties of PM2.5 under this kind severe BB pollution level in the real atmospheric environment were both presented in this measurement report. Moreover, the variation of the ratios of BB tracers during different BB pollution periods was also exhibited.
Elena Barbaro, Krystyna Koziol, Mats P. Björkman, Carmen P. Vega, Christian Zdanowicz, Tonu Martma, Jean-Charles Gallet, Daniel Kępski, Catherine Larose, Bartłomiej Luks, Florian Tolle, Thomas V. Schuler, Aleksander Uszczyk, and Andrea Spolaor
Atmos. Chem. Phys., 21, 3163–3180, https://doi.org/10.5194/acp-21-3163-2021, https://doi.org/10.5194/acp-21-3163-2021, 2021
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This paper shows the most comprehensive seasonal snow chemistry survey to date, carried out in April 2016 across 22 sites on 7 glaciers across Svalbard. The dataset consists of the concentration, mass loading, spatial and altitudinal distribution of major ion species (Ca2+, K+,
Na2+, Mg2+,
NH4+, SO42−,
Br−, Cl− and
NO3−), together with its stable oxygen and hydrogen isotope composition (δ18O and
δ2H) in the snowpack. This study was part of the larger Community Coordinated Snow Study in Svalbard.
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., 21, 2959–2980, https://doi.org/10.5194/acp-21-2959-2021, https://doi.org/10.5194/acp-21-2959-2021, 2021
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Organosulfates (OSs) are important constituents and tracers of secondary organic aerosols (SOAs) in the atmosphere. Here we characterized the OS species in ambient aerosols in Shanghai, China. We find that the contributions of OSs and SOAs to organic aerosols have increased in recent years and that OS production was largely controlled by the oxidant level (Ox), particularly in summer. We infer that mitigation of Ox pollution can effectively reduce the production of OSs and SOAs in eastern China.
Ren-Guo Zhu, Hua-Yun Xiao, Li Luo, Hongwei Xiao, Zequn Wen, Yuwen Zhu, Xiaozheng Fang, Yuanyuan Pan, and Zhenping Chen
Atmos. Chem. Phys., 21, 2585–2600, https://doi.org/10.5194/acp-21-2585-2021, https://doi.org/10.5194/acp-21-2585-2021, 2021
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Amino acids (AAs), as important organic nitrogen compounds, play key roles in the nitrogen cycles, climate change and public health. The sources and transformation of AAs in two size-segregated aerosol particles were explored. This study presents the first isotopic evidence that the sources of AAs for fine and coarse aerosol particles may be similar. And the potentially significant role of bacterial degradation processes in aerosol protein degradation state was suggested.
Runlong Cai, Chao Yan, Dongsen Yang, Rujing Yin, Yiqun Lu, Chenjuan Deng, Yueyun Fu, Jiaxin Ruan, Xiaoxiao Li, Jenni Kontkanen, Qiang Zhang, Juha Kangasluoma, Yan Ma, Jiming Hao, Douglas R. Worsnop, Federico Bianchi, Pauli Paasonen, Veli-Matti Kerminen, Yongchun Liu, Lin Wang, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 21, 2457–2468, https://doi.org/10.5194/acp-21-2457-2021, https://doi.org/10.5194/acp-21-2457-2021, 2021
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Based on long-term measurements, we discovered that the collision of H2SO4–amine clusters is the governing mechanism that initializes fast new particle formation in the polluted atmospheric environment of urban Beijing. The mechanism and the governing factors for H2SO4–amine nucleation in the polluted atmosphere are quantitatively investigated in this study.
Lei Liu, Jian Zhang, Yinxiao Zhang, Yuanyuan Wang, Liang Xu, Qi Yuan, Dantong Liu, Yele Sun, Pingqing Fu, Zongbo Shi, and Weijun Li
Atmos. Chem. Phys., 21, 2251–2265, https://doi.org/10.5194/acp-21-2251-2021, https://doi.org/10.5194/acp-21-2251-2021, 2021
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We found that large numbers of light-absorbing primary organic particles with high viscosity, especially tarballs, from domestic coal and biomass burning occurred in rural and even urban hazes in the winter of North China. For the first time, we characterized the atmospheric aging process of these burning-related primary organic particles by microscopic analysis and further evaluated their light absorption enhancement resulting from the “lensing effect” of secondary inorganic coatings.
Songyun Fan, Yuan Gao, Robert M. Sherrell, Shun Yu, and Kaixuan Bu
Atmos. Chem. Phys., 21, 2105–2124, https://doi.org/10.5194/acp-21-2105-2021, https://doi.org/10.5194/acp-21-2105-2021, 2021
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Aerosol sampling was carried out at Palmer Station in the west Antarctic Peninsula during the austral summer of 2016–2017. This study generated new data on the concentrations and particle-size distributions of aerosol trace elements in the marine atmosphere over this region. Measurement data allowed estimating the dry deposition fluxes. The new results are critically important to understanding the properties of aerosol particles and regional biogeochemical cycles.
Qing Yu, Jing Chen, Weihua Qin, Siming Cheng, Yuepeng Zhang, Yuewei Sun, Ke Xin, and Mushtaq Ahmad
Atmos. Chem. Phys., 21, 1775–1796, https://doi.org/10.5194/acp-21-1775-2021, https://doi.org/10.5194/acp-21-1775-2021, 2021
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Water-soluble organic aerosols have significant impacts on haze formation, climate change and human health. This study investigated the characteristics of WSOC in PM2.5 in Beijing to compare the source contributions of different WSOC fractions and the influencing factors for different secondary components in WSOC. Our results help to propose control measures for WSOC during severe haze episodes and underline the importance of SOA properties and heterogeneous reactions in different seasons.
Tianzeng Chen, Jun Liu, Qingxin Ma, Biwu Chu, Peng Zhang, Jinzhu Ma, Yongchun Liu, Cheng Zhong, Pengfei Liu, Yafei Wang, Yujing Mu, and Hong He
Atmos. Chem. Phys., 21, 1341–1356, https://doi.org/10.5194/acp-21-1341-2021, https://doi.org/10.5194/acp-21-1341-2021, 2021
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Effects of photochemical aging on the formation and evolution of summertime secondary aerosol were systematically investigated in a suburb of Beijing. Higher PM1 concentration accompanied longer photochemical age (ta). Sulfate and more-oxidized OOA formation were significantly sensitive to the increase in ta, and their contributions were greatly enhanced at elevated ta levels. Our results suggested that photochemical aging process played a crucial role in PM1 and O3 pollution in summertime.
Yujiao Zhu, Likun Xue, Jian Gao, Jianmin Chen, Hongyong Li, Yong Zhao, Zhaoxin Guo, Tianshu Chen, Liang Wen, Penggang Zheng, Ye Shan, Xinfeng Wang, Tao Wang, Xiaohong Yao, and Wenxing Wang
Atmos. Chem. Phys., 21, 1305–1323, https://doi.org/10.5194/acp-21-1305-2021, https://doi.org/10.5194/acp-21-1305-2021, 2021
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This work investigates the long-term changes in new particle formation (NPF) events under reduced SO2 emissions at the summit of Mt. Tai during seven campaigns from 2007 to 2018. We found the NPF intensity increased 2- to 3-fold in 2018 compared to 2007. In contrast, the probability of new particles growing to CCN size largely decreased. Changes to biogenic VOCs and anthropogenic emissions are proposed to explain the distinct NPF characteristics.
Djacinto Monteiro dos Santos, Luciana Varanda Rizzo, Samara Carbone, Patrick Schlag, and Paulo Artaxo
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-533, https://doi.org/10.5194/acp-2020-533, 2021
Revised manuscript accepted for ACP
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The Metropolitan Area of São Paulo (MASP), with very extensive biofuel use, has unique atmospheric chemistry among world megacities. In this study, we examine the complex relationships between aerosol chemical composition and particle size distribution. Our findings provide a better understanding of the dynamics of the physicochemical properties of submicron particles and highlight the key role of secondary organic aerosol formation in the pollution levels in São Paulo.
Yuying Wang, Zhanqing Li, Qiuyan Wang, Xiaoai Jin, Peng Yan, Maureen Cribb, Yanan Li, Cheng Yuan, Hao Wu, Tong Wu, Rongmin Ren, and Zhaoxin Cai
Atmos. Chem. Phys., 21, 915–926, https://doi.org/10.5194/acp-21-915-2021, https://doi.org/10.5194/acp-21-915-2021, 2021
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The unexpected increase in surface ozone concentration was found along with the reduced anthropogenic emissions during the 2019 Chinese Spring Festival in Beijing. The enhanced atmospheric oxidation capacity could promote the formation of secondary aerosols, especially sulfate, which offset the decrease in PM2.5 mass concentration. This phenomenon was likely to exist throughout the entire Beijing–Tianjin–Hebei (BTH) region to be a contributing factor to the haze during the COVID-19 lockdown.
Kevin J. Sanchez, Bo Zhang, Hongyu Liu, Georges Saliba, Chia-Li Chen, Savannah L. Lewis, Lynn M. Russell, Michael A. Shook, Ewan C. Crosbie, Luke D. Ziemba, Matthew D. Brown, Taylor J. Shingler, Claire E. Robinson, Elizabeth B. Wiggins, Kenneth L. Thornhill, Edward L. Winstead, Carolyn Jordan, Patricia K. Quinn, Timothy S. Bates, Jack Porter, Thomas G. Bell, Eric S. Saltzman, Michael J. Behrenfeld, and Richard H. Moore
Atmos. Chem. Phys., 21, 831–851, https://doi.org/10.5194/acp-21-831-2021, https://doi.org/10.5194/acp-21-831-2021, 2021
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Models describing atmospheric airflow were combined with satellite measurements representative of marine phytoplankton and other meteorological variables. These combined variables were compared to measured aerosol to identify upwind influences on aerosol concentrations. Results indicate that phytoplankton production rates upwind impact the aerosol mass. Also, results suggest that the condensation of mass onto short-lived large sea spray particles may be a significant sink of aerosol mass.
Pragati Rai, Jay G. Slowik, Markus Furger, Imad El Haddad, Suzanne Visser, Yandong Tong, Atinderpal Singh, Günther Wehrle, Varun Kumar, Anna K. Tobler, Deepika Bhattu, Liwei Wang, Dilip Ganguly, Neeraj Rastogi, Ru-Jin Huang, Jaroslaw Necki, Junji Cao, Sachchida N. Tripathi, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 717–730, https://doi.org/10.5194/acp-21-717-2021, https://doi.org/10.5194/acp-21-717-2021, 2021
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We present a simple conceptual framework based on elemental size distributions and enrichment factors that allows for a characterization of major sources, site-to-site similarities, and local differences and the identification of key information required for efficient policy development. Absolute concentrations are by far the highest in Delhi, followed by Beijing, and then the European cities.
Yue Zhou, Christopher P. West, Anusha P. S. Hettiyadura, Xiaoying Niu, Hui Wen, Jiecan Cui, Tenglong Shi, Wei Pu, Xin Wang, and Alexander Laskin
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1260, https://doi.org/10.5194/acp-2020-1260, 2021
Revised manuscript accepted for ACP
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We present a comprehensive characterization of water soluble organic carbon (WSOC) in seasonal snow of northwestern China. We applied complementary multi-modal analytical techniques to investigate bulk and molecular-level composition, optical properties, and sources of WSOC. For the first time, we estimated the extent of radiative forcing due to WSOC in snow using model simulation, and showed profound influences of WSOC on the energy budget of mid-latitude seasonal snowpack.
Jenna C. Ditto, Megan He, Tori N. Hass-Mitchell, Samar G. Moussa, Katherine Hayden, Shao-Meng Li, John Liggio, Amy Leithead, Patrick Lee, Michael J. Wheeler, Jeremy J. B. Wentzell, and Drew R. Gentner
Atmos. Chem. Phys., 21, 255–267, https://doi.org/10.5194/acp-21-255-2021, https://doi.org/10.5194/acp-21-255-2021, 2021
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Forest fires are an important source of reactive organic gases and aerosols to the atmosphere. We analyzed organic aerosols collected from an aircraft above a boreal forest fire and reported an increasing contribution from compounds containing oxygen, nitrogen, and sulfur as the plume aged, with sulfide and ring-bound nitrogen functionality. Our results demonstrated chemistry that is important in biomass burning but also in urban/developing regions with high local nitrogen and sulfur emissions.
Nadja Triesch, Manuela van Pinxteren, Anja Engel, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 163–181, https://doi.org/10.5194/acp-21-163-2021, https://doi.org/10.5194/acp-21-163-2021, 2021
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To investigate the sources of free amino acids (FAAs) in the marine atmosphere, concerted measurements (the simultaneous investigation of seawater, size-segregated aerosol particles and cloud water) were performed at the Cabo Verde islands. This study describes the transfer of FAAs as part of organic matter from the ocean into the atmosphere on a molecular level. In the investigated marine environment, a high enrichment of FAAs in submicron aerosol particles and in cloud droplets was observed.
Liya Ma, Yujiao Zhu, Mei Zheng, Yele Sun, Lei Huang, Xiaohuan Liu, Yang Gao, Yanjie Shen, Huiwang Gao, and Xiaohong Yao
Atmos. Chem. Phys., 21, 183–200, https://doi.org/10.5194/acp-21-183-2021, https://doi.org/10.5194/acp-21-183-2021, 2021
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In this study, we investigate three patterns of new particles growing to CCN (cloud condensation nuclei) size, i.e., one-stage growth and two-stage growth-A and growth-B patterns. Combining the observations of gaseous pollutants and measured or modeled particulate chemical species, the three growth patterns were discussed regarding the spatial heterogeneity, formation of secondary aerosols, and evaporation of semivolatile particulates as was the survival probability of new particles to CCN size.
Charlotte M. Beall, Jennifer M. Michaud, Meredith A. Fish, Julie Dinasquet, Gavin C. Cornwell, M. Dale Stokes, Michael D. Burkart, Thomas C. Hill, Paul J. DeMott, and Kimberly A. Prather
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1229, https://doi.org/10.5194/acp-2020-1229, 2021
Revised manuscript accepted for ACP
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Ice nucleating particles (INPs) can influence multiple climate-relevant cloud properties by triggering droplet freezing at relative humidities below or temperatures above the freezing point of water. The ocean is a significant INP source, yet the specific identities of marine INPs remain largely unknown. Here we identify 14 ice nucleating microbes from aerosol and precipitation samples collected at a coastal site in Southern California, two or more of which are marine.
Rui Li, Yilong Zhao, and Hongbo Fu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1199, https://doi.org/10.5194/acp-2020-1199, 2021
Revised manuscript accepted for ACP
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The rapid response to COVID-19 pandemic led to the unprecedented decreases of economic activities, thereby reducing the pollutant emissions. The strict lockdown measures significantly decreased primary components such as Cr (−201 %) and Fe (−154 %) in PM2.5, whereas the higher relative humidity (RH) and NH3 level, and the lower air temperature (T) enhanced the production of secondary aerosol including SO42− (47.2 %), NO3− (38.6 %), and NH4+ (22.7 %).
Haiyan Ni, Ru-Jin Huang, Max M. Cosijn, Lu Yang, Jie Guo, Junji Cao, and Ulrike Dusek
Atmos. Chem. Phys., 20, 16041–16053, https://doi.org/10.5194/acp-20-16041-2020, https://doi.org/10.5194/acp-20-16041-2020, 2020
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We investigated sources of carbonaceous aerosols in Beijing and Xi'an during severe winter haze. Elemental carbon (EC) was dominated by vehicle emissions in Xi’an and coal burning in Beijing. Organic carbon (OC) increment during haze days was driven by the increase in primary and secondary OC (SOC). SOC was more from fossil sources in Beijing than Xi’an, especially during haze days. In Xi’an, no strong day–night differences in EC or OC sources suggest a large accumulation of particles.
Michael J. Lawler, Savannah L. Lewis, Lynn M. Russell, Patricia K. Quinn, Timothy S. Bates, Derek J. Coffman, Lucia M. Upchurch, and Eric S. Saltzman
Atmos. Chem. Phys., 20, 16007–16022, https://doi.org/10.5194/acp-20-16007-2020, https://doi.org/10.5194/acp-20-16007-2020, 2020
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This work describes new measurements of aerosol (particles) composition over the North Atlantic Ocean. It provides concentrations of polysaccharide material likely made from organisms in the surface ocean and improves our understanding of the relative importance of such fresh biogenic material compared to more recalcitrant organic carbon in forming marine organic aerosol. We aim ultimately to understand the role that ocean biology plays in cloud formation in marine regions.
Connor Stahl, Melliza Templonuevo Cruz, Paola Angela Bañaga, Grace Betito, Rachel A. Braun, Mojtaba Azadi Aghdam, Maria Obiminda Cambaliza, Genevieve Rose Lorenzo, Alexander B. MacDonald, Miguel Ricardo A. Hilario, Preciosa Corazon Pabroa, John Robin Yee, James Bernard Simpas, and Armin Sorooshian
Atmos. Chem. Phys., 20, 15907–15935, https://doi.org/10.5194/acp-20-15907-2020, https://doi.org/10.5194/acp-20-15907-2020, 2020
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Long-term (16-month) high-frequency (weekly) measurements of size-resolved aerosol composition are reported. Important insights are discussed about factors (e.g., transport, fires, precipitation, photo-oxidation) impacting the mass size distributions of organic and sulfonic acids at a coastal megacity with diverse meteorology. The size-resolved nature of the data yielded one such finding that organic acids preferentially adsorb to dust rather than sea salt particles.
Yiqun Han, Wu Chen, Lia Chatzidiakou, Anika Krause, Li Yan, Hanbin Zhang, Queenie Chan, Ben Barratt, Rod Jones, Jing Liu, Yangfeng Wu, Meiping Zhao, Junfeng Zhang, Frank J. Kelly, Tong Zhu, and the AIRLESS team
Atmos. Chem. Phys., 20, 15775–15792, https://doi.org/10.5194/acp-20-15775-2020, https://doi.org/10.5194/acp-20-15775-2020, 2020
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Panel studies might be the most suitable way to link intensive air monitoring campaigns for a wide range of pollutant species and personal exposure in different micro-environments, together with epidemiological studies of detailed biological changes in humans. Panel studies are intensive, but related papers are very limited. With the successful collection of a rich dataset, we believe AIRLESS sets a good example for the design of a multidisciplinary study.
Danitza Klopper, Paola Formenti, Andreas Namwoonde, Mathieu Cazaunau, Servanne Chevaillier, Anaïs Feron, Cécile Gaimoz, Patrick Hease, Fadi Lahmidi, Cécile Mirande-Bret, Sylvain Triquet, Zirui Zeng, and Stuart J. Piketh
Atmos. Chem. Phys., 20, 15811–15833, https://doi.org/10.5194/acp-20-15811-2020, https://doi.org/10.5194/acp-20-15811-2020, 2020
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The chemical composition of aerosol particles is very important as it determines to which extent they can affect the Earth's climate by acting with solar light and modifying the properties of clouds. The South Atlantic region is a remote and under-explored region to date where these effects could be important. The measurements presented in this paper consist in the analysis of samples collected at a coastal site in Namibia. The first long-term source apportionment is presented and discussed.
Wenjie Wang, David D. Parrish, Xin Li, Min Shao, Ying Liu, Ziwei Mo, Sihua Lu, Min Hu, Xin Fang, Yusheng Wu, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 15617–15633, https://doi.org/10.5194/acp-20-15617-2020, https://doi.org/10.5194/acp-20-15617-2020, 2020
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During the past decade, China has devoted very substantial resources to improving the environment. These efforts have improved atmospheric particulate matter loading, but ambient ozone levels have continued to increase. In this paper we investigate the causes of the increasing ozone concentrations through analysis of a data set that is, to our knowledge, unique: a 12-year data set including ground-level O3, NOx, and VOC precursors collected at an urban site in Beijing.
Marta Via, María Cruz Minguillón, Cristina Reche, Xavier Querol, and Andrés Alastuey
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1244, https://doi.org/10.5194/acp-2020-1244, 2020
Revised manuscript accepted for ACP
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Atmospheric pollutants have been measured in an urban environment by means of state-of-the-art tecniques allowing to identify the origin and the sources of pollution. Last years are shown to be increasingly dominated by non-directly emitted particulate matter. Gathered knowledge about the sources of atmospheric pollutants is mandatory to design effective mitigation policies.
Qiyuan Wang, Huikun Liu, Ping Wang, Wenting Dai, Ting Zhang, Youzhi Zhao, Jie Tian, Wenyan Zhang, Yongming Han, and Junji Cao
Atmos. Chem. Phys., 20, 15537–15549, https://doi.org/10.5194/acp-20-15537-2020, https://doi.org/10.5194/acp-20-15537-2020, 2020
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Light-absorbing carbonaceous (LAC) aerosol is an important influencing factor for global climate forcing. In this study, we used a receptor model coupling multi-wavelength absorption with chemical species to explore the source-specific LAC optical properties at a tropical marine monsoon climate zone. The results can improve our understanding of the LAC radiative effects caused by ship emissions.
Hongling Yin, Jinfeng Liang, Di Wu, Shiping Li, Yi Luo, and Xu Deng
Atmos. Chem. Phys., 20, 14933–14945, https://doi.org/10.5194/acp-20-14933-2020, https://doi.org/10.5194/acp-20-14933-2020, 2020
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Samples were collected from six ground-based sites located in Chengdu, a typical rapidly developing metropolitan area in Southwest China, and were analysed for seven OPEs in atmospheric PM2.5 (Σ7 OPEs). The concentrations of Σ7 OPEs were higher in autumn and winter than in summer. In contrast to coastal cities, sustained and stable high local emissions in the inland city studied were identified, which is particularly noteworthy.
Qingqing Yu, Xiang Ding, Quanfu He, Weiqiang Yang, Ming Zhu, Sheng Li, Runqi Zhang, Ruqin Shen, Yanli Zhang, Xinhui Bi, Yuesi Wang, Ping'an Peng, and Xinming Wang
Atmos. Chem. Phys., 20, 14581–14595, https://doi.org/10.5194/acp-20-14581-2020, https://doi.org/10.5194/acp-20-14581-2020, 2020
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We carried out a 1-year PM concurrent observation at 12 sites across six regions of China, and size-segregated PAHs were measured. We found both PAHs and BaPeq were concentrated in PM1.1, and northern China had higher PAHs' pollution and inhalation cancer risk than southern China. Nationwide increases in both PAH levels and inhalation cancer risk occurred in winter. We suggest reducing coal and biofuel consumption in the residential sector is an important option to mitigate PAHs' health risks.
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Short summary
Overprediction of fine-particle ammonium-sulfate molar ratios (R) by thermodynamic models is suggested as evidence for organic aerosol limiting the condensation of ammonia onto particles, with significant impacts on aerosol chemistry. We find that the effects of small amounts of salt and dust, combined with measurement artifacts, explain the discrepancy in R. These results are highly insensitive to mixing state. This means that aerosol predictions are much more robust than thought before.
Overprediction of fine-particle ammonium-sulfate molar ratios (R) by thermodynamic models is...
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