Articles | Volume 15, issue 5
https://doi.org/10.5194/acp-15-2775-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-15-2775-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
10 Mar 2015
Research article |
| 10 Mar 2015
A critical evaluation of proxy methods used to estimate the acidity of atmospheric particles
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, MD, USA
J. Izumi
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, MD, USA
A. P. Sullivan
Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA
R. J. Weber
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, USA
Foundation for Research and Technology – Hellas, Patras, Greece
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Mária Lbadaoui-Darvas, Satoshi Takahama, and Athanasios Nenes
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Spiro D. Jorga, Kalliopi Florou, Christos Kaltsonoudis, John K. Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros N. Pandis
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Linghan Zeng, Amy P. Sullivan, Rebecca A. Washenfelder, Jack Dibb, Eric Scheuer, Teresa L. Campos, Joseph M. Katich, Ezra Levin, Michael A. Robinson, and Rodney J. Weber
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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
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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 using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Nicholas Balasus, Michael A. Battaglia Jr., Katherine Ball, Vanessa Caicedo, Ruben Delgado, Annmarie G. Carlton, and Christopher J. Hennigan
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Measurements of aerosol and gas composition were carried out at a land–water transition site near Baltimore, MD. Gas-phase ammonia concentrations were highly elevated compared to measurements at a nearby inland site. Our analysis reveals that NH2 was from both industrial and agricultural sources. This had a pronounced effect on aerosol chemical composition at the site, most notably contributing to episodic spikes of aerosol nitrate.
Yang Wang, Guangjie Zheng, Michael P. Jensen, Daniel A. Knopf, Alexander Laskin, Alyssa A. Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur J. Sedlacek, John E. Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria A. Zawadowicz, and Jian Wang
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Paraskevi Georgakaki, Aikaterini Bougiatioti, Jörg Wieder, Claudia Mignani, Fabiola Ramelli, Zamin A. Kanji, Jan Henneberger, Maxime Hervo, Alexis Berne, Ulrike Lohmann, and Athanasios Nenes
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Aerosol and cloud observations coupled with a droplet activation parameterization was used to investigate the aerosol–cloud droplet link in alpine mixed-phase 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 within 50 % of Ndlim. Identifying when dynamical changes control Nd variability is central for understanding aerosol–cloud interactions.
Georgia Sotiropoulou, Luisa Ickes, Athanasios Nenes, and Annica M. L. Ekman
Atmos. Chem. Phys., 21, 9741–9760, https://doi.org/10.5194/acp-21-9741-2021, https://doi.org/10.5194/acp-21-9741-2021, 2021
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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 breakup upon collision of two ice particles in a high-resolution model improves cloud ice phase representation; however, cloud liquid remains overestimated.
Yuhan Yang, Dong Gao, and Rodney J. Weber
Atmos. Meas. Tech., 14, 4707–4719, https://doi.org/10.5194/amt-14-4707-2021, https://doi.org/10.5194/amt-14-4707-2021, 2021
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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 benchtop 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.
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.
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.
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.
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.
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
Publication in ACP not foreseen
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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
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.
Hongyu Guo, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 17307–17323, https://doi.org/10.5194/acp-18-17307-2018, https://doi.org/10.5194/acp-18-17307-2018, 2018
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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.
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.
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.
Marwa M. H. El-Sayed, Diana L. Ortiz-Montalvo, and Christopher J. Hennigan
Atmos. Chem. Phys., 18, 1171–1184, https://doi.org/10.5194/acp-18-1171-2018, https://doi.org/10.5194/acp-18-1171-2018, 2018
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We characterized the reversibility of aqSOA formed from isoprene at a location in the eastern United States. WSOCp evaporation with drying was observed systematically throughout the late spring and summer, indicating reversible aqSOA formation. The absolute reversible aqSOA concentrations, as well as the relative amount of reversible aqSOA, increased with decreasing NOx / isoprene ratios, suggesting that IEPOX or other low-NOx oxidation products were responsible for these effects.
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.
A. Hecobian, A. Evanoski-Cole, A. Eiguren-Fernandez, A. P. Sullivan, G. S. Lewis, S. V. Hering, and J. L. Collett Jr.
Atmos. Meas. Tech., 9, 525–533, https://doi.org/10.5194/amt-9-525-2016, https://doi.org/10.5194/amt-9-525-2016, 2016
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A newly developed instrument, the Sequential Spot Sampler (S3) was evaluated in the laboratory and field for the hourly measurement of ambient PM2.5 nitrate and sulfate concentrations. The results from the comparison of two S3s and the S3s with other well-established methods show that this instrument is suitable for deployment; provides high-resolution aerosol nitrate and sulfate concentrations while requiring minimal operator involvement and low power input; and has a small footprint.
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.
A. A. May, T. Lee, G. R. McMeeking, S. Akagi, A. P. Sullivan, S. Urbanski, R. J. Yokelson, and S. M. Kreidenweis
Atmos. Chem. Phys., 15, 6323–6335, https://doi.org/10.5194/acp-15-6323-2015, https://doi.org/10.5194/acp-15-6323-2015, 2015
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Smoke plumes from some prescribed fires in the southeastern United States were sampled via aircraft to observe changes in organic aerosol (OA) with atmospheric transport. These plumes underwent rapid mixing, and, hence, substantial dilution with background air occurred. Dilution-driven evaporation appears to be the primary driver of OA transformations within the sampled plumes rather than photochemistry.
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.
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
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
R. Saleh, C. J. Hennigan, G. R. McMeeking, W. K. Chuang, E. S. Robinson, H. Coe, N. M. Donahue, and A. L. Robinson
Atmos. Chem. Phys., 13, 7683–7693, https://doi.org/10.5194/acp-13-7683-2013, https://doi.org/10.5194/acp-13-7683-2013, 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
S. K. Akagi, R. J. Yokelson, I. R. Burling, S. Meinardi, I. Simpson, D. R. Blake, G. R. McMeeking, A. Sullivan, T. Lee, S. Kreidenweis, S. Urbanski, J. Reardon, D. W. T. Griffith, T. J. Johnson, and D. R. Weise
Atmos. Chem. Phys., 13, 1141–1165, https://doi.org/10.5194/acp-13-1141-2013, https://doi.org/10.5194/acp-13-1141-2013, 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)
Source apportionment of soot particles and aqueous-phase processing of black carbon coatings in an urban environment
Seasonal variations in composition and sources of atmospheric ultrafine particles in urban Beijing based on near-continuous measurements
Summertime response of ozone and fine particulate matter to mixing layer meteorology over the North China Plain
Trace elements in PM2.5 aerosols in East Asian outflow in the spring of 2018: emission, transport, and source apportionment
Measurement Report: Investigation on the sources and formation processes of dicarboxylic acids and related species in urban aerosols before and during the COVID-19 lockdown in Jinan, East China
pH dependence of brown-carbon optical properties in cloud water
Oxidative potential in rural, suburban and city centre atmospheric environments in central Europe
Secondary aerosol formation during a special dust transport event: impacts from unusually enhanced ozone and dust backflows over the ocean
Intra-event evolution of elemental and ionic concentrations in wet deposition in an urban environment
Spatial and diurnal variations of aerosol organosulfates in summertime Shanghai, China: potential influence of photochemical processes and anthropogenic sulfate pollution
Characterizing water-soluble brown carbon in fine particles in four typical cities in northwestern China during wintertime: integrating optical properties with chemical processes
Chemical composition-dependent hygroscopic behavior of individual ambient aerosol particles collected at a coastal site
Gas–particle partitioning of semivolatile organic compounds when wildfire smoke comes to town
Enrichment of calcium in sea spray aerosol: insights from bulk measurements and individual particle analysis during the R/V Xuelong cruise in the summertime in Ross Sea, Antarctica
Source apportionment study on particulate air pollution in two high-altitude Bolivian cities: La Paz and El Alto
Morphological features and water solubility of iron in aged fine aerosol particles over the Indian Ocean
Short-term Source Apportionment of Fine Particulate Matter with Time-dependent Profiles Using SoFi: Exploring the Reliability of Rolling Positive Matrix Factorization (PMF) Applied to Bihourly Molecular and Elemental Tracer Data
What chemical species are responsible for new particle formation and growth in the Netherlands? A hybrid positive matrix factorization (PMF) analysis using aerosol composition (ACSM) and size (SMPS)
Measurement report: Stoichiometry of dissolved iron and aluminum as an indicator of the factors controlling the fractional solubility of aerosol iron – results of the annual observations of size-fractionated aerosol particles in Japan
In-depth study of the formation processes of single atmospheric particles in the south-eastern margin of the Tibetan Plateau
Climatology of aerosol properties at an atmospheric monitoring site on the northern California coast
Concurrent photochemical whitening and darkening of ambient brown carbon
High-time-resolution chemical composition and source apportionment of PM2.5 in northern Chinese cities: implications for policy
Measurement report: New insights into the mixing structures of black carbon on the eastern Tibetan Plateau – soot redistribution and fractal dimension enhancement by liquid–liquid phase separation
Seasonal variations in the production of singlet oxygen and organic triplet excited states in aqueous PM2.5 in Hong Kong SAR, South China
Fractional solubility of iron in mineral dust aerosols over coastal Namibia: a link with marine biogenic emissions?
Nighttime NO emissions strongly suppress chlorine and nitrate radical formation during the winter in Delhi
Influence of natural and anthropogenic aerosols on cloud base droplet size distributions in clouds over the South China Sea and West Pacific
The important contribution of secondary formation and biomass burning to oxidized organic nitrogen (OON) in a polluted urban area: insights from in situ measurements of a chemical ionization mass spectrometer (CIMS)
Measurement report: A 1-year study to estimate maritime contributions to PM10 in a coastal area in northern France
Marine Carbohydrates in Arctic Aerosol Particles and Fog – Diversity of Oceanic Sources and Atmospheric Transformations
Evolution and chemical characteristics of organic aerosols during wintertime PM2.5 episodes in Shanghai, China: insights gained from online measurements of organic molecular markers
Arctic observations of hydroperoxymethyl thioformate (HPMTF) – seasonal behavior and relationship to other oxidation products of dimethyl sulfide at the Zeppelin Observatory, Svalbard
A 1-year aerosol chemical speciation monitor (ACSM) source analysis of organic aerosol particle contributions from anthropogenic sources after long-range transport at the TROPOS research station Melpitz
Contributions of primary emissions and secondary formation to nitrated aromatic compounds in themountain background region of Southeast China
Mist cannon trucks can exacerbate the formation of water-soluble organic aerosol and PM2.5 pollution in the road environment
Amino acids, carbohydrates, and lipids in the tropical oligotrophic Atlantic Ocean: sea-to-air transfer and atmospheric in situ formation
Ambient carbonaceous aerosol levels in Cyprus and the role of pollution transport from the Middle East
High contribution of anthropogenic combustion sources to atmospheric inorganic reactive nitrogen in South China evidenced by isotopes
Measurement report: Diurnal variations of brown carbon during two distinct seasons in a megacity in northeast China
Source Apportionment of PM2.5 in Montréal, Canada and Health Risk Assessment for Potentially Toxic Elements
Characterization of water-soluble brown carbon chromophores from wildfire plumes in the western US using size exclusion chromatography
Comprehensive mass spectrometric analysis of unprecedented high levels of carbonaceous aerosol particles long-range transported from wildfires in the Siberian Arctic
Vertical profiles of volatile organic compounds and fine particles in atmospheric air by using an aerial drone with miniaturized samplers and portable devices
Multiple pathways for the formation of secondary organic aerosol in the North China Plain in summer
Insights into characteristics and formation mechanisms of secondary organic aerosols in the Guangzhou urban area
Particulate-bound alkyl nitrate pollution and formation mechanisms in Beijing, China
An attribution of the low single-scattering albedo of biomass burning aerosol over the southeastern Atlantic
Measurement report: Rapid changes of chemical characteristics and health risks for highly time resolved trace elements in PM2.5 in a typical industrial city in response to stringent clean air actions
Measurement report: Summertime fluorescence characteristics of atmospheric water-soluble organic carbon in the marine boundary layer of the western Arctic Ocean
Ryan N. Farley, Sonya Collier, Christopher D. Cappa, Leah R. Williams, Timothy B. Onasch, Lynn M. Russell, Hwajin Kim, and Qi Zhang
Atmos. Chem. Phys., 23, 15039–15056, https://doi.org/10.5194/acp-23-15039-2023, https://doi.org/10.5194/acp-23-15039-2023, 2023
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Soot particles, also known as black carbon (BC), have important implications for global climate and regional air quality. After the particles are emitted, BC can be coated with other material, impacting the aerosol properties. We selectively measured the composition of particles containing BC to explore their sources and chemical transformations in the atmosphere. We focus on a persistent, multiday fog event in order to study the effects of chemical reactions occurring within liquid droplets.
Xiaoxiao Li, Yijing Chen, Yuyang Li, Runlong Cai, Yiran Li, Chenjuan Deng, Jin Wu, Chao Yan, Hairong Cheng, Yongchun Liu, Markku Kulmala, Jiming Hao, James N. Smith, and Jingkun Jiang
Atmos. Chem. Phys., 23, 14801–14812, https://doi.org/10.5194/acp-23-14801-2023, https://doi.org/10.5194/acp-23-14801-2023, 2023
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Near-continuous measurements show the composition, sources, and seasonal variations of ultrafine particles (UFPs) in urban Beijing. Vehicle and cooking emissions and new particle formation are the main sources of UFPs, and aqueous/heterogeneous processes increase UFP mode diameters. UFPs are the highest in winter due to the highest primary particle emission rates and new particle formation rates, and CHO fractions are the highest in summer due to the strongest photooxidation.
Jiaqi Wang, Jian Gao, Fei Che, Xin Yang, Yuanqin Yang, Lei Liu, Yan Xiang, and Haisheng Li
Atmos. Chem. Phys., 23, 14715–14733, https://doi.org/10.5194/acp-23-14715-2023, https://doi.org/10.5194/acp-23-14715-2023, 2023
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Regional-scale observations of surface O3, PM2.5 and its major chemical species, mixing layer height (MLH), and other meteorological parameters were made in the North China Plain during summer. Unlike the cold season, synchronized increases in MDA8 O3 and PM2.5 under medium MLH conditions have been witnessed. The increasing trend of PM2.5 was associated with enhanced secondary chemical formation. The correlation between MLH and secondary air pollutants should be treated with care in hot seasons.
Takuma Miyakawa, Akinori Ito, Chunmao Zhu, Atsushi Shimizu, Erika Matsumoto, Yusuke Mizuno, and Yugo Kanaya
Atmos. Chem. Phys., 23, 14609–14626, https://doi.org/10.5194/acp-23-14609-2023, https://doi.org/10.5194/acp-23-14609-2023, 2023
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This study conducted semi-continuous measurements of PM2.5 aerosols and their elemental composition in western Japan, during spring 2018. It analyzed the emissions, transport, and wet removal of elements such as Pb, Cu, Fe, and Mn. It also assessed the accuracy of modeled concentrations and found overestimations of BC and underestimations of Cu and anthropogenic Fe in East Asia. Insights into emissions, removals, and source apportionment of trace metals in the East Asian outflow were provided.
Jingjing Meng, Yachen Wang, Yuanyuan Li, Tonglin Huang, Zhifei Wang, Yiqiu Wang, Min Chen, Zhanfang Hou, Houhua Zhou, Keding Lu, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 23, 14481–14503, https://doi.org/10.5194/acp-23-14481-2023, https://doi.org/10.5194/acp-23-14481-2023, 2023
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This study investigated the effect of COVID-19 lockdown (LCD) measures on the formation and evolutionary process of diacids and related compounds from field observations. Results demonstrate that more aged organic aerosols are observed during the LCD due to the enhanced photochemical oxidation. Our study also found that the reactivity of 13C was higher than that of 12C in the gaseous photochemical oxidation, leading to higher δ13C values of C2 during the LCD than before the LCD.
Christopher J. Hennigan, Michael McKee, Vikram Pratap, Bryanna Boegner, Jasper Reno, Lucia Garcia, Madison McLaren, and Sara M. Lance
Atmos. Chem. Phys., 23, 14437–14449, https://doi.org/10.5194/acp-23-14437-2023, https://doi.org/10.5194/acp-23-14437-2023, 2023
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This study characterized the optical properties of light-absorbing organic compounds, called brown carbon (BrC), in atmospheric cloud water samples. In all samples, light absorption by BrC increased linearly with increasing pH. There was variability in the sensitivity of the absorption–pH relationship, depending on the degree of influence from fire emissions. Overall, these results show that the climate forcing of BrC is quite strongly affected by its pH-dependent absorption.
Máté Vörösmarty, Gaëlle Uzu, Jean-Luc Jaffrezo, Pamela Dominutti, Zsófia Kertész, Enikő Papp, and Imre Salma
Atmos. Chem. Phys., 23, 14255–14269, https://doi.org/10.5194/acp-23-14255-2023, https://doi.org/10.5194/acp-23-14255-2023, 2023
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Poor air quality caused by high concentrations of particulate matter is one of the most severe public health concerns for humans worldwide. One of the most important biological mechanisms inducing adverse health effects is the oxidant–antioxidant imbalance. We showed that the oxidative stress changed substantially and in a complex manner with location and season. Biomass burning exhibited the dominant influence, while motor vehicles played an important role in the non-heating period.
Da Lu, Hao Li, Mengke Tian, Guochen Wang, Xiaofei Qin, Na Zhao, Juntao Huo, Fan Yang, Yanfen Lin, Jia Chen, Qingyan Fu, Yusen Duan, Xinyi Dong, Congrui Deng, Sabur F. Abdullaev, and Kan Huang
Atmos. Chem. Phys., 23, 13853–13868, https://doi.org/10.5194/acp-23-13853-2023, https://doi.org/10.5194/acp-23-13853-2023, 2023
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Environmental conditions during dust are usually not favorable for secondary aerosol formation. However in this study, an unusual dust event was captured in a Chinese mega-city and showed “anomalous” meteorology and a special dust backflow transport pathway. The underlying formation mechanisms of secondary aerosols are probed in the context of this special dust event. This study shows significant implications for the varying dust aerosol chemistry in the future changing climate.
Thomas Audoux, Benoit Laurent, Karine Desboeufs, Gael Noyalet, Franck Maisonneuve, Olivier Lauret, and Servanne Chevaillier
Atmos. Chem. Phys., 23, 13485–13503, https://doi.org/10.5194/acp-23-13485-2023, https://doi.org/10.5194/acp-23-13485-2023, 2023
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In the Paris region, a campaign was conducted to study wet deposition of aerosol particles during rainfall events. Simultaneous measurements of aerosol and wet deposition allowed us to discuss their transfer from the atmosphere to rain. Chemical evolution within events revealed meteorology, atmospheric conditions and local vs. long range sources as key factors. This study highlights the variability of wet deposition and the need to consider event-specific factors to understand its mechanisms.
Ting Yang, Yu Xu, Qing Ye, Yi-Jia Ma, Yu-Chen Wang, Jian-Zhen Yu, Yu-Sen Duan, Chen-Xi Li, Hong-Wei Xiao, Zi-Yue Li, Yue Zhao, and Hua-Yun Xiao
Atmos. Chem. Phys., 23, 13433–13450, https://doi.org/10.5194/acp-23-13433-2023, https://doi.org/10.5194/acp-23-13433-2023, 2023
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In this study, 130 OS species were quantified in ambient fine particulate matter (PM2.5) collected in urban and suburban Shanghai (East China) in the summer of 2021. The daytime OS formation was concretized based on the interactions among OSs, ultraviolet (UV), ozone (O3), and sulfate. Our finding provides field evidence for the influence of photochemical process and anthropogenic sulfate on OS formation and has important implications for the mitigation of organic particulate pollution.
Miao Zhong, Jianzhong Xu, Huiqin Wang, Li Gao, Haixia Zhu, Lixiang Zhai, Xinghua Zhang, and Wenhui Zhao
Atmos. Chem. Phys., 23, 12609–12630, https://doi.org/10.5194/acp-23-12609-2023, https://doi.org/10.5194/acp-23-12609-2023, 2023
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This study focus on coal-combustion-dominated aerosol in urban areas in northwestern China and combines the results of optical measurement and chemical analysis to deduce the evolution of these characteristics in the atmosphere, which has previously been unknown. The results provide insights into the effects of atmospheric processes and emissions on brown carbon properties.
Li Wu, Hyo-Jin Eom, Hanjin Yoo, Dhrubajyoti Gupta, Hye-Rin Cho, Pingqing Fu, and Chul-Un Ro
Atmos. Chem. Phys., 23, 12571–12588, https://doi.org/10.5194/acp-23-12571-2023, https://doi.org/10.5194/acp-23-12571-2023, 2023
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Hygroscopicity of ambient marine aerosols is of critical relevance to investigate their atmospheric impacts, which, however, remain uncertain due to their complex compositions and mixing states. Therefore, a study on the hygroscopic behavior of ambient marine aerosols for understanding the phase states when interacting with water vapor at different RH levels and their subsequent impacts on the heterogeneous chemical reactions, atmospheric environment, and human health is of vital importance.
Yutong Liang, Rebecca A. Wernis, Kasper Kristensen, Nathan M. Kreisberg, Philip L. Croteau, Scott C. Herndon, Arthur W. H. Chan, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 23, 12441–12454, https://doi.org/10.5194/acp-23-12441-2023, https://doi.org/10.5194/acp-23-12441-2023, 2023
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We measured the gas–particle partitioning behaviors of biomass burning markers and examined the effect of wildfire organic aerosol on the partitioning of semivolatile organic compounds. Most compounds measured are less volatile than model predictions. Wildfire aerosol enhanced the condensation of polar compounds and caused some nonpolar (e.g., polycyclic aromatic hydrocarbons) compounds to partition into the gas phase, thus affecting their lifetimes in the atmosphere and the mode of exposure.
Bojiang Su, Xinhui Bi, Zhou Zhang, Yue Liang, Congbo Song, Tao Wang, Yaohao Hu, Lei Li, Zhen Zhou, Jinpei Yan, Xinming Wang, and Guohua Zhang
Atmos. Chem. Phys., 23, 10697–10711, https://doi.org/10.5194/acp-23-10697-2023, https://doi.org/10.5194/acp-23-10697-2023, 2023
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During the R/V Xuelong cruise observation over the Ross Sea, Antarctica, the mass concentrations of water-soluble Ca2+ and the mass spectra of individual calcareous particles were measured. Our results indicated that lower temperature, lower wind speed, and the presence of sea ice may facilitate Ca2+ enrichment in sea spray aerosols and highlighted the potential contribution of organically complexed calcium to calcium enrichment, which is inaccurate based solely on water-soluble Ca2+ estimation.
Valeria Mardoñez, Marco Pandolfi, Lucille Joanna S. Borlaza, Jean-Luc Jaffrezo, Andrés Alastuey, Jean-Luc Besombes, Isabel Moreno R., Noemi Perez, Griša Močnik, Patrick Ginot, Radovan Krejci, Vladislav Chrastny, Alfred Wiedensohler, Paolo Laj, Marcos Andrade, and Gaëlle Uzu
Atmos. Chem. Phys., 23, 10325–10347, https://doi.org/10.5194/acp-23-10325-2023, https://doi.org/10.5194/acp-23-10325-2023, 2023
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La Paz and El Alto are two fast-growing, high-altitude Bolivian cities forming the second-largest metropolitan area in the country. The sources of particulate matter (PM) in this conurbation were not previously investigated. This study identified 11 main sources of PM, of which dust and vehicular emissions stand out as the main ones. The influence of regional biomass combustion and local waste combustion was also observed, with the latter being a major source of hazardous compounds.
Sayako Ueda, Yoko Iwamoto, Fumikazu Taketani, Mingxu Liu, and Hitoshi Matsui
Atmos. Chem. Phys., 23, 10117–10135, https://doi.org/10.5194/acp-23-10117-2023, https://doi.org/10.5194/acp-23-10117-2023, 2023
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We examine iron in atmospheric fine aerosol particles collected over the Indian Ocean during shipborne observations in November 2018. Transmission electron microscopy analysis with water dialysis shows that various types of iron (fly ash, iron oxide, and mineral dust) co-exist with ammonium sulfate and that their solubility differs depending on the iron type. Using PM2.5 bulk samples and global model simulations, we elucidate their origins, aging, and implications for present iron simulations.
Qiongqiong Wang, Shuhui Zhu, Shan Wang, Cheng Huang, Yunsen Duan, and Jian Zhen Yu
EGUsphere, https://doi.org/10.5194/egusphere-2023-1846, https://doi.org/10.5194/egusphere-2023-1846, 2023
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We investigated short-term source apportionment of PM2.5 utilizing rolling positive matrix factorization (PMF) and online PM chemical speciation data, which included source-specific organic tracers collected over a period of 37 days during the winter of 2019–2020 in suburban Shanghai, China. The findings highlight that by imposing constraints on the primary source profiles, short-term PMF analysis successfully replicated both the individual primary sources and the total secondary sources.
Farhan R. Nursanto, Roy Meinen, Rupert Holzinger, Maarten C. Krol, Xinya Liu, Ulrike Dusek, Bas Henzing, and Juliane L. Fry
Atmos. Chem. Phys., 23, 10015–10034, https://doi.org/10.5194/acp-23-10015-2023, https://doi.org/10.5194/acp-23-10015-2023, 2023
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Particulate matter (PM) is a harmful air pollutant that depends on the complex mixture of natural and anthropogenic emissions into the atmosphere. Thus, in different regions and seasons, the way that PM is formed and grows can differ. In this study, we use a combined statistical analysis of the chemical composition and particle size distribution to determine what drives particle formation and growth across seasons, using varying wind directions to elucidate the role of different sources.
Kohei Sakata, Aya Sakaguchi, Yoshiaki Yamakawa, Chihiro Miyamoto, Minako Kurisu, and Yoshio Takahashi
Atmos. Chem. Phys., 23, 9815–9836, https://doi.org/10.5194/acp-23-9815-2023, https://doi.org/10.5194/acp-23-9815-2023, 2023
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Anthropogenic iron is the dominant source of dissolved Fe in aerosol particles, but its contribution to dissolved Fe in aerosol particles has not been quantitatively evaluated. We established the molar concentration ratio of dissolved Fe to dissolved Al as a new indicator to evaluate the contribution of anthropogenic iron. As a result, about 10 % of dissolved Fe in aerosol particles was derived from anthropogenic iron when aerosol particles were transported from East Asia to the Pacific Ocean.
Li Li, Qiyuan Wang, Jie Tian, Huikun Liu, Yong Zhang, Steven Sai Hang Ho, Weikang Ran, and Junji Cao
Atmos. Chem. Phys., 23, 9597–9612, https://doi.org/10.5194/acp-23-9597-2023, https://doi.org/10.5194/acp-23-9597-2023, 2023
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The Tibetan Plateau has a unique geographical location, but there is a lack of detailed research on the real-time characteristics of full aerosol composition. This study elaborates the changes in chemical characteristics between transport and local fine particles during the pre-monsoon, reveals the size distribution and the mixing states of different individual particles, and highlights the contributions of photooxidation and aqueous reaction to the formation of the secondary species.
Erin K. Boedicker, Elisabeth Andrews, Patrick J. Sheridan, and Patricia K. Quinn
Atmos. Chem. Phys., 23, 9525–9547, https://doi.org/10.5194/acp-23-9525-2023, https://doi.org/10.5194/acp-23-9525-2023, 2023
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We present 15 years of measurements from a marine site on the northern California coast and characterize the seasonal trends of aerosol ion composition and optical properties at the site. We investigate the relationship between the chemical and optical properties and show that they both support similar seasonal variations in aerosol sources at the site. Additionally, we show through comparisons to other marine aerosol observations that the site is representative of a clean marine environment.
Qian Li, Dantong Liu, Xiaotong Jiang, Ping Tian, Yangzhou Wu, Siyuan Li, Kang Hu, Quan Liu, Mengyu Huang, Ruijie Li, Kai Bi, Shaofei Kong, Deping Ding, and Chenjie Yu
Atmos. Chem. Phys., 23, 9439–9453, https://doi.org/10.5194/acp-23-9439-2023, https://doi.org/10.5194/acp-23-9439-2023, 2023
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By attributing the shortwave absorption from black carbon, primary organic aerosol and secondary organic aerosol in a suburban environment, we firstly observed that the photochemically produced nitrogen-containing secondary organic aerosol may contribute to the enhancement of brown carbon absorption, partly compensating for some bleaching effect on the absorption of primary organic aerosol, hereby exerting radiative impacts.
Yong Zhang, Jie Tian, Qiyuan Wang, Lu Qi, Manousos Ioannis Manousakas, Yuemei Han, Weikang Ran, Yele Sun, Huikun Liu, Renjian Zhang, Yunfei Wu, Tianqu Cui, Kaspar Rudolf Daellenbach, Jay Gates Slowik, André S. H. Prévôt, and Junji Cao
Atmos. Chem. Phys., 23, 9455–9471, https://doi.org/10.5194/acp-23-9455-2023, https://doi.org/10.5194/acp-23-9455-2023, 2023
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PM2.5 pollution still frequently occurs in northern China during winter, and it is necessary to figure out the causes of air pollution based on intensive real-time measurement. The findings elaborate the chemical characteristics and source contributions of PM2.5 in three pilot cities, reveal potential formation mechanisms of secondary aerosols, and highlight the importance of controlling biomass burning and inhibiting generation of secondary aerosol for air quality improvement.
Qi Yuan, Yuanyuan Wang, Yixin Chen, Siyao Yue, Jian Zhang, Yinxiao Zhang, Liang Xu, Wei Hu, Dantong Liu, Pingqing Fu, Huiwang Gao, and Weijun Li
Atmos. Chem. Phys., 23, 9385–9399, https://doi.org/10.5194/acp-23-9385-2023, https://doi.org/10.5194/acp-23-9385-2023, 2023
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This study for the first time found large amounts of liquid–liquid phase separation particles with soot redistributing in organic coatings instead of sulfate cores in the eastern Tibetan Plateau atmosphere. The particle size and the ratio of the organic matter coating thickness to soot size are two of the major possible factors that likely affect the soot redistribution process. The soot redistribution process promoted the morphological compaction of soot particles.
Yuting Lyu, Yin Hau Lam, Yitao Li, Nadine Borduas-Dedekind, and Theodora Nah
Atmos. Chem. Phys., 23, 9245–9263, https://doi.org/10.5194/acp-23-9245-2023, https://doi.org/10.5194/acp-23-9245-2023, 2023
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We measured singlet oxygen (1O2*) and triplet excited states of organic matter (3C*) in illuminated aqueous extracts of PM2.5 collected in different seasons at different sites in Hong Kong SAR, South China. In contrast to the locations, seasonality had significant effects on 3C* and 1O2* production due to seasonal variations in long-range air mass transport. The steady-state concentrations of 3C* and 1O2* correlated with the concentration and absorbance of water-soluble organic carbon.
Karine Desboeufs, Paola Formenti, Raquel Torres-Sánchez, Kerstin Schepanski, Jean-Pierre Chaboureau, Hendrik Andersen, Jan Cermak, Stefanie Feuerstein, Benoit Laurent, Danitza Klopper, Andreas Namwoonde, Mathieu Cazaunau, Servanne Chevaillier, Anaïs Feron, Cecile Mirande-Bret, Sylvain Triquet, and Stuart J. Piketh
EGUsphere, https://doi.org/10.5194/egusphere-2023-1736, https://doi.org/10.5194/egusphere-2023-1736, 2023
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This study investigates the fractional solubility of iron (Fe) in dust particles along the coast of Namibia, a critical region for the atmospheric Fe supply of the Southern Atlantic Ocean. Our results suggest a possible two-way interplay whereby marine biogenic emissions from the coastal marine ecosystems to the atmosphere would increase the solubility of Fe-bearing dust by photo-reduction processes. The subsequent deposition of soluble Fe could act to further enhance marine biogenic emissions.
Sophie L. Haslett, David M. Bell, Varun Kumar, Jay G. Slowik, Dongyu S. Wang, Suneeti Mishra, Neeraj Rastogi, Atinderpal Singh, Dilip Ganguly, Joel Thornton, Feixue Zheng, Yuanyuan Li, Wei Nie, Yongchun Liu, Wei Ma, Chao Yan, Markku Kulmala, Kaspar R. Daellenbach, David Hadden, Urs Baltensperger, Andre S. H. Prevot, Sachchida N. Tripathi, and Claudia Mohr
Atmos. Chem. Phys., 23, 9023–9036, https://doi.org/10.5194/acp-23-9023-2023, https://doi.org/10.5194/acp-23-9023-2023, 2023
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In Delhi, some aspects of daytime and nighttime atmospheric chemistry are inverted, and parodoxically, vehicle emissions may be limiting other forms of particle production. This is because the nighttime emissions of nitrogen oxide (NO) by traffic and biomass burning prevent some chemical processes that would otherwise create even more particles and worsen the urban haze.
Rose Marie Miller, Robert M. Rauber, Larry Di Girolamo, Matthew Rilloraza, Dongwei Fu, Greg M. McFarquhar, Stephen W. Nesbitt, Luke D. Ziemba, Sarah Woods, and Kenneth Lee Thornhill
Atmos. Chem. Phys., 23, 8959–8977, https://doi.org/10.5194/acp-23-8959-2023, https://doi.org/10.5194/acp-23-8959-2023, 2023
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The influence of human-produced aerosols on clouds remains one of the uncertainties in radiative forcing of Earth’s climate. Measurements of aerosol chemistry from sources around the Philippines illustrate the linkage between aerosol chemical composition and cloud droplet characteristics. Differences in aerosol chemical composition in the marine layer from biomass burning, industrial, ship-produced, and marine aerosols are shown to impact cloud microphysical structure just above cloud base.
Yiyu Cai, Chenshuo Ye, Wei Chen, Weiwei Hu, Wei Song, Yuwen Peng, Shan Huang, Jipeng Qi, Sihang Wang, Chaomin Wang, Caihong Wu, Zelong Wang, Baolin Wang, Xiaofeng Huang, Lingyan He, Sasho Gligorovski, Bin Yuan, Min Shao, and Xinming Wang
Atmos. Chem. Phys., 23, 8855–8877, https://doi.org/10.5194/acp-23-8855-2023, https://doi.org/10.5194/acp-23-8855-2023, 2023
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We studied the variability and molecular composition of ambient oxidized organic nitrogen (OON) in both gas and particle phases using a state-of-the-art online mass spectrometer in urban air. Biomass burning and secondary formation were found to be the two major sources of OON. Daytime nitrate radical chemistry for OON formation was more important than previously thought. Our results improved the understanding of the sources and molecular composition of OON in the polluted urban atmosphere.
Frédéric Ledoux, Cloé Roche, Gilles Delmaire, Gilles Roussel, Olivier Favez, Marc Fadel, and Dominique Courcot
Atmos. Chem. Phys., 23, 8607–8622, https://doi.org/10.5194/acp-23-8607-2023, https://doi.org/10.5194/acp-23-8607-2023, 2023
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We quantify the emissions from the marine sector in northern France, whether from natural or human-made sources. Therefore, a 1-year PM10 sampling campaign was conducted at a French coastal site. Results showed that sea salts contributed 37 %, while secondary nitrate and sulfate contributed 42 %, biomass burning 8 %, and heavy-fuel-oil combustion from shipping emissions 5 %. Sources contributing more than 80 % of PM10 are of regional and/or long-range origin.
Sebastian Zeppenfeld, Manuela van Pinxteren, Markus Hartmann, Moritz Zeising, Astrid Bracher, and Hartmut Herrmann
EGUsphere, https://doi.org/10.5194/egusphere-2023-1607, https://doi.org/10.5194/egusphere-2023-1607, 2023
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Marine carbohydrates are produced in the surface of the ocean, enter the atmophere as part of sea spray aerosol particles and potentially contribute to the formation of clouds. Here, we present the results of a sea-air transfer study of marine carbohydrates conducted in the high Arctic. Besides a chemo-selective transfer, we observed a quick atmospheric aging of carbohydrates, possibly as a result of both biotic and abiotic processes.
Shuhui Zhu, Min Zhou, Liping Qiao, Dan Dan Huang, Qiongqiong Wang, Shan Wang, Yaqin Gao, Shengao Jing, Qian Wang, Hongli Wang, Changhong Chen, Cheng Huang, and Jian Zhen Yu
Atmos. Chem. Phys., 23, 7551–7568, https://doi.org/10.5194/acp-23-7551-2023, https://doi.org/10.5194/acp-23-7551-2023, 2023
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Organic aerosol (OA) is increasingly important in urban PM2.5 pollution as inorganic ions are becoming lower. We investigated the chemical characteristics of OA during nine episodes in Shanghai. The availability of bi-hourly measured molecular markers revealed that the control of local urban sources such as vehicular and cooking emissions lessened the severity of local episodes. Regional control of precursors and biomass burning would reduce PM2.5 episodes influenced by regional transport.
Karolina Siegel, Yvette Gramlich, Sophie L. Haslett, Gabriel Freitas, Radovan Krejci, Paul Zieger, and Claudia Mohr
Atmos. Chem. Phys., 23, 7569–7587, https://doi.org/10.5194/acp-23-7569-2023, https://doi.org/10.5194/acp-23-7569-2023, 2023
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Hydroperoxymethyl thioformate (HPMTF) is a recently discovered oxidation product of dimethyl sulfide (DMS). We present a full year of concurrent gas- and particle-phase observations of HPMTF and other DMS oxidation products from the Arctic. We did not observe significant amounts of HPMTF in the particle phase but a good agreement between gas-phase HMPTF and methanesulfonic acid in the summer. Our study provides information about the relationship between HPMTF and other DMS oxidation products.
Samira Atabakhsh, Laurent Poulain, Gang Chen, Francesco Canonaco, André S. H. Prévôt, Mira Pöhlker, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 6963–6988, https://doi.org/10.5194/acp-23-6963-2023, https://doi.org/10.5194/acp-23-6963-2023, 2023
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The study focuses on the aerosol chemical variations found in the rural-background station of Melpitz based on ACSM and MAAP measurements. Source apportionment on both organic aerosol (OA) and black carbon (eBC) was performed, and source seasonality was also linked to air mass trajectories. Overall, three anthropogenic sources were identified in OA and eBC plus two additional aged OA. Our results demonstrate the influence of transported coal-combustion-related OA even during summer time.
Yanqin Ren, Gehui Wang, Jie Wei, Jun Tao, Zhisheng Zhang, and Hong Li
Atmos. Chem. Phys., 23, 6835–6848, https://doi.org/10.5194/acp-23-6835-2023, https://doi.org/10.5194/acp-23-6835-2023, 2023
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Nine quantified nitrated aromatic compounds (NACs) in PM2.5 were examined at the peak of Mt. Wuyi. They manifested a significant rise in overall abundance in the winter and autumn. The transport of contaminants had a significant impact on NACs. Under low-NOx conditions, the formation of NACs was comparatively sensitive to NO2, suggesting that NACs would become significant in the aerosol characteristics when nitrate concentrations decreased as a result of emission reduction measures.
Yu Xu, Xin-Ni Dong, Chen He, Dai-She Wu, Hong-Wei Xiao, and Hua-Yun Xiao
Atmos. Chem. Phys., 23, 6775–6788, https://doi.org/10.5194/acp-23-6775-2023, https://doi.org/10.5194/acp-23-6775-2023, 2023
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The air pollution associated with fine particles and secondary organic aerosol is not weakened by the application of mist cannon trucks but rather is aggravated. Our results provide not only new insights into the formation processes of aerosol water-soluble organic compounds associated with the water mist sprayed by mist cannon trucks in the road atmospheric environment but also crucial information for the decision makers to regulate the operation of mist cannon trucks in many cities in China.
Manuela van Pinxteren, Sebastian Zeppenfeld, Khanneh Wadinga Fomba, Nadja Triesch, Sanja Frka, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 6571–6590, https://doi.org/10.5194/acp-23-6571-2023, https://doi.org/10.5194/acp-23-6571-2023, 2023
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Important marine organic carbon compounds were identified in the Atlantic Ocean and marine aerosol particles. These compounds were strongly enriched in the atmosphere. Their enrichment was, however, not solely explained via sea-to-air transfer but also via atmospheric in situ formation. The identified compounds constituted about 50 % of the organic carbon on the aerosol particles, and a pronounced coupling between ocean and atmosphere for this oligotrophic region could be concluded.
Aliki Christodoulou, Iasonas Stavroulas, Mihalis Vrekoussis, Maximillien Desservettaz, Michael Pikridas, Elie Bimenyimana, Jonilda Kushta, Matic Ivančič, Martin Rigler, Philippe Goloub, Konstantina Oikonomou, Roland Sarda-Estève, Chrysanthos Savvides, Charbel Afif, Nikos Mihalopoulos, Stéphane Sauvage, and Jean Sciare
Atmos. Chem. Phys., 23, 6431–6456, https://doi.org/10.5194/acp-23-6431-2023, https://doi.org/10.5194/acp-23-6431-2023, 2023
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Our study presents, for the first time, a detailed source identification of aerosols at an urban background site in Cyprus (eastern Mediterranean), a region strongly impacted by climate change and air pollution. Here, we identify an unexpected high contribution of long-range transported pollution from fossil fuel sources in the Middle East, highlighting an urgent need to further characterize these fast-growing emissions and their impacts on regional atmospheric composition, climate, and health.
Tingting Li, Jun Li, Zeyu Sun, Hongxing Jiang, Chongguo Tian, and Gan Zhang
Atmos. Chem. Phys., 23, 6395–6407, https://doi.org/10.5194/acp-23-6395-2023, https://doi.org/10.5194/acp-23-6395-2023, 2023
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N-NH4+ and N-NO3- were vital components in nitrogenous aerosols and contributed 69 % to total nitrogen in PM2.5. Coal combustion was still the most important source of urban atmospheric NO3-. However, the non-agriculture sources play an increasingly important role in NH4+ emissions.
Yuan Cheng, Xu-bing Cao, Jiu-meng Liu, Ying-jie Zhong, Qin-qin Yu, Qiang Zhang, and Ke-bin He
Atmos. Chem. Phys., 23, 6241–6253, https://doi.org/10.5194/acp-23-6241-2023, https://doi.org/10.5194/acp-23-6241-2023, 2023
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Brown carbon (BrC) aerosols were explored in the northernmost megacity in China during a frigid winter and an agricultural-fire-impacted spring. BrC was more light absorbing at night for both seasons, with more pronounced diurnal variations in spring, and the dominant drivers were identified as regulations on heavy-duty diesel trucks and open burning, respectively. Agricultural fires resulted in unique absorption spectra of BrC, which were characterized by a distinct peak at ∼365 nm.
Nansi Fakhri, Robin Stevens, Arnold Downey, Konstantina Oikonomou, Jean Sciare, Charbel Afif, and Patrick L. Hayes
EGUsphere, https://doi.org/10.5194/egusphere-2023-1039, https://doi.org/10.5194/egusphere-2023-1039, 2023
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The chemical composition of PM2.5 and emission sources as well as potential human health risk associated with trace elements are investigated for an urban site in Montréal over a 3-month period (August–November). To our knowledge, this study represents the first time that such extensive composition measurements were included in an urban source apportionment study in Canada and provides greater resolution of PM2.5 sources than has been previously achieved using PMF in similar Canadian studies.
Lisa Azzarello, Rebecca A. Washenfelder, Michael A. Robinson, Alessandro Franchin, Caroline C. Womack, Christopher D. Holmes, Steven S. Brown, Ann Middlebrook, Tim Newberger, Colm Sweeney, and Cora J. Young
EGUsphere, https://doi.org/10.5194/egusphere-2023-1128, https://doi.org/10.5194/egusphere-2023-1128, 2023
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We present a molecular size-resolved offline analysis of water-soluble brown carbon collected on an aircraft during FIREX-AQ. The smoke plumes were aged 0 to 5 h where absorption was dominated by small molecular weight molecules, brown carbon absorption downwind did not consistently decrease, and the measurements differed from online absorption measurements of the same samples. We show how differences between online and offline absorption could be related to different measurement conditions.
Eric Schneider, Hendryk Czech, Olga Popovicheva, Marina Chichaeva, Vasily Kobelev, Nikolay Kasimov, Tatiana Minkina, Christopher Paul Rüger, and Ralf Zimmermann
EGUsphere, https://doi.org/10.5194/egusphere-2023-769, https://doi.org/10.5194/egusphere-2023-769, 2023
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This study provides insights into the complex chemical composition of long-range transported wildfire plumes from Yakutia, which underwent different levels of atmospheric processing. With mass complementary mass spectrometric techniques, we improve our understanding of the chemical processes and atmospheric fate of wildfire plumes. Unprecedented high levels of carbonaceous aerosols crossed the polar circle with implications for the Arctic ecosystem and consequently climate.
Eka Dian Pusfitasari, Jose Ruiz-Jimenez, Aleksi Tiusanen, Markus Suuronen, Jesse Haataja, Yusheng Wu, Juha Kangasluoma, Krista Luoma, Tuukka Petäjä, Matti Jussila, Kari Hartonen, and Marja-Liisa Riekkola
Atmos. Chem. Phys., 23, 5885–5904, https://doi.org/10.5194/acp-23-5885-2023, https://doi.org/10.5194/acp-23-5885-2023, 2023
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A miniaturized air-sampling drone system was successfully applied for the collection of volatile organic compounds (VOCs) and for the measurement of black carbon (BC) and total particle number concentrations in atmospheric air. Here we report, for the first time, the vertical profiles of BC and aerosol number concentrations above the boreal forest in Hyytiälä (Finland) at high altitudes close to the boundary layer in autumn 2021. VOC composition with its distribution was studied as well.
Yifang Gu, Ru-Jin Huang, Jing Duan, Wei Xu, Chunshui Lin, Haobin Zhong, Ying Wang, Haiyan Ni, Quan Liu, Ruiguang Xu, Litao Wang, and Yong Jie Li
Atmos. Chem. Phys., 23, 5419–5433, https://doi.org/10.5194/acp-23-5419-2023, https://doi.org/10.5194/acp-23-5419-2023, 2023
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Secondary organic aerosol (SOA) can be produced by various pathways, but its formation mechanisms are unclear. Observations were conducted in the North China Plain during a highly oxidizing atmosphere in summer. We found that fast photochemistry dominated SOA formation during daytime. Two types of aqueous-phase chemistry (nocturnal and daytime processing) take place at high relative humidity. The potential transformation from primary organic aerosol (POA) to SOA was also an important pathway.
Miaomiao Zhai, Ye Kuang, Li Liu, Yao He, Biao Luo, Wanyun Xu, Jiangchuan Tao, Yu Zou, Fei Li, Changqin Yin, Chunhui Li, Hanbing Xu, and Xuejiao Deng
Atmos. Chem. Phys., 23, 5119–5133, https://doi.org/10.5194/acp-23-5119-2023, https://doi.org/10.5194/acp-23-5119-2023, 2023
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Using year-long aerosol mass spectrometer measurements, roles of secondary organic aerosols (SOA) during haze formations in an urban area of southern China were systematically analyzed. Almost all severe haze events were accompanied by continuous daytime and nighttime SOA formations, whereas coordinated gas-phase photochemistry and aqueous-phase reactions likely played significant roles in quick daytime SOA formations, and nitrate radicals played significant roles in nighttime SOA formations.
Jiyuan Yang, Guoyang Lei, Jinfeng Zhu, Yutong Wu, Chang Liu, Kai Hu, Junsong Bao, Zitong Zhang, Weili Lin, and Jun Jin
EGUsphere, https://doi.org/10.5194/egusphere-2023-700, https://doi.org/10.5194/egusphere-2023-700, 2023
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The atmospheric pollution and formation mechanisms of particulate-bound alkyl nitrate in Beijing were studied. Long-chain n-alkyl nitrates contributed more to the total n-alkyl nitrate in PM2.5. Long-chain n-alkyl nitrates negatively correlated with O3 but positively correlated with PM2.5 and NO2, so they may not be produced during photochemical reactions but form through reactions between alkanes and nitrates on PM surfaces. Particulate-bound n-alkyl nitrates strongly influence haze pollution.
Amie Dobracki, Paquita Zuidema, Steven G. Howell, Pablo Saide, Steffen Freitag, Allison C. Aiken, Sharon P. Burton, Arthur J. Sedlacek III, Jens Redemann, and Robert Wood
Atmos. Chem. Phys., 23, 4775–4799, https://doi.org/10.5194/acp-23-4775-2023, https://doi.org/10.5194/acp-23-4775-2023, 2023
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Southern Africa produces approximately one-third of the world’s carbon from fires. The thick smoke layer can flow westward, interacting with the southeastern Atlantic cloud deck. The net radiative impact can alter regional circulation patterns, impacting rainfall over Africa. We find that the smoke is highly absorbing of sunlight, mostly because it contains more black carbon than smoke over the Northern Hemisphere.
Rui Li, Yining Gao, Yubao Chen, Meng Peng, Weidong Zhao, Gehui Wang, and Jiming Hao
Atmos. Chem. Phys., 23, 4709–4726, https://doi.org/10.5194/acp-23-4709-2023, https://doi.org/10.5194/acp-23-4709-2023, 2023
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A random forest model was used to isolate the effects of emission and meteorology to trace elements in PM2.5 in Tangshan. The results suggested that control measures facilitated decreases of Ga, Co, Pb, Zn, and As, due to the strict implementation of coal-to-gas strategies and optimisation of industrial structure and layout. However, the deweathered levels of Ca, Cr, and Fe only displayed minor decreases, indicating that ferrous metal smelting and vehicle emission controls should be enhanced.
Jinyoung Jung, Yuzo Miyazaki, Jin Hur, Yun Kyung Lee, Mi Hae Jeon, Youngju Lee, Kyoung-Ho Cho, Hyun Young Chung, Kitae Kim, Jung-Ok Choi, Catherine Lalande, Joo-Hong Kim, Taejin Choi, Young Jun Yoon, Eun Jin Yang, and Sung-Ho Kang
Atmos. Chem. Phys., 23, 4663–4684, https://doi.org/10.5194/acp-23-4663-2023, https://doi.org/10.5194/acp-23-4663-2023, 2023
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This study examined the summertime fluorescence properties of water-soluble organic carbon (WSOC) in aerosols over the western Arctic Ocean. We found that the WSOC in fine-mode aerosols in coastal areas showed a higher polycondensation degree and aromaticity than in sea-ice-covered areas. The fluorescence properties of atmospheric WSOC in the summertime marine Arctic boundary can improve our understanding of the WSOC chemical and biological linkages at the ocean–sea-ice–atmosphere interface.
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Short summary
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.
We show that the ion balance and molar ratio methods are unsuitable for use as aerosol pH...
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