Articles | Volume 15, issue 20
Atmos. Chem. Phys., 15, 11667–11682, 2015
https://doi.org/10.5194/acp-15-11667-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 15, 11667–11682, 2015
https://doi.org/10.5194/acp-15-11667-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article 21 Oct 2015
Research article | 21 Oct 2015
PM2.5 water-soluble elements in the southeastern United States: automated analytical method development, spatiotemporal distributions, source apportionment, and implications for heath studies
T. Fang et al.
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Anusha Priyadarshani Silva Hettiyadura, Ibrahim M. Al-Naiema, Dagen D. Hughes, Ting Fang, and Elizabeth A. Stone
Atmos. Chem. Phys., 19, 3191–3206, https://doi.org/10.5194/acp-19-3191-2019, https://doi.org/10.5194/acp-19-3191-2019, 2019
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This study examines anthropogenic influences on secondary organic aerosol at an urban site in Atlanta, Georgia. Organosulfates accounted for 16.5 % of PM2.5 organic carbon and were mostly derived from isoprene. In contrast to a rural forested site, Atlanta's isoprene-derived organosulfate concentrations were 2–6 times higher and accounted for twice as much organic carbon. Insights are provided as to which organosulfates should be measured in future studies and targeted for standard development.
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.
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.
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.
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
Atmos. Chem. Phys., 21, 11079–11098, https://doi.org/10.5194/acp-21-11079-2021, https://doi.org/10.5194/acp-21-11079-2021, 2021
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This paper reports the vertical profiles of trace gas and aerosol properties over the eastern North Atlantic, a region of persistent but diverse subtropical marine boundary layer (MBL) clouds. We examined the key processes that drive the cloud condensation nuclei (CCN) population and how it varies with season and synoptic conditions. This study helps improve the model representation of the aerosol processes in the remote MBL, reducing the simulated aerosol indirect effects.
Sudheer Salana, Yixiang Wang, Joseph Puthussery, and Vishal Verma
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-188, https://doi.org/10.5194/amt-2021-188, 2021
Revised manuscript under review for AMT
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Oxidative Potential (OP) of particulate matter (PM) is an important indicator of PM toxicity. However, no automated instrument has ever been developed to provide a rapid high-throughput analysis of the cell-based OP measurements. Here, we developed a first-of-its kind semi-automated instrument for measuring oxidative potential using rat alveolar cells. We also developed a dataset on the intrinsic cellular OP of several compounds commonly known to be present in the ambient PM.
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.
Haoran Yu, Joseph Varghese Puthussery, Yixiang Wang, and Vishal Verma
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-376, https://doi.org/10.5194/acp-2021-376, 2021
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We assessed the oxidative potential (OP) of ambient PM2.5 collected from five sites in the Midwest US. Compared to the homogeneously distributed PM2.5 mass, OP showed high spatiotemporal variation. Weak correlations for the regression between mass and OP indicated a limited role of mass in determining the OP. Moreover, the intercorrelations among different OP endpoints were not strong, justifying the need for using multiple assays for determining the oxidative levels of the particles.
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
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-131, https://doi.org/10.5194/amt-2021-131, 2021
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Three online systems for measuring water-soluble brown carbon are compared. A mist chamber and two different particle-into-liquid samplers were deployed on separate research aircraft targeting wildfires and followed a similar detection method using a long path liquid waveguide with a spectrometer to measure the light absorption from 300 to 700 nm. Detection limits, signal hysteresis and other sampling issues are compared, and further improvements of these liquid-based systems are provided.
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.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-173, https://doi.org/10.5194/acp-2021-173, 2021
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere, and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
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
Revised manuscript under review for ACP
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Yunle Chen, Masayuki Takeuchi, Theodora Nah, Lu Xu, Manjula R. Canagaratna, Harald Stark, Karsten Baumann, Francesco Canonaco, André S. H. Prévôt, L. Gregory Huey, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 20, 8421–8440, https://doi.org/10.5194/acp-20-8421-2020, https://doi.org/10.5194/acp-20-8421-2020, 2020
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Two online mass spectrometry instruments, an aerosol mass spectrometer and a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols, were deployed at Yorkville, GA, for a comprehensive characterization of organic aerosol. We observed notable secondary organic aerosol formation from isoprene and monoterpenes via different pathways during both day and night, and a series of highly oxidized acid-like compounds was found to be closely related to aged SOA.
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.
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.
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 %.
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.
Anusha Priyadarshani Silva Hettiyadura, Ibrahim M. Al-Naiema, Dagen D. Hughes, Ting Fang, and Elizabeth A. Stone
Atmos. Chem. Phys., 19, 3191–3206, https://doi.org/10.5194/acp-19-3191-2019, https://doi.org/10.5194/acp-19-3191-2019, 2019
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This study examines anthropogenic influences on secondary organic aerosol at an urban site in Atlanta, Georgia. Organosulfates accounted for 16.5 % of PM2.5 organic carbon and were mostly derived from isoprene. In contrast to a rural forested site, Atlanta's isoprene-derived organosulfate concentrations were 2–6 times higher and accounted for twice as much organic carbon. Insights are provided as to which organosulfates should be measured in future studies and targeted for standard development.
Kate R. Smith, Peter M. Edwards, Peter D. Ivatt, James D. Lee, Freya Squires, Chengliang Dai, Richard E. Peltier, Mat J. Evans, Yele Sun, and Alastair C. Lewis
Atmos. Meas. Tech., 12, 1325–1336, https://doi.org/10.5194/amt-12-1325-2019, https://doi.org/10.5194/amt-12-1325-2019, 2019
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Clusters of low-cost, low-power atmospheric gas sensors were built into a sensor instrument to monitor NO2 and O3 in Beijing, alongside reference instruments, aiming to improve the reliability of sensor measurements. Clustering identical sensors and using the median sensor signal was used to minimize drift over short and medium timescales. Three different machine learning techniques were used for all the sensor data in an attempt to correct for cross-interferences, which worked to some degree.
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.
Joseph V. Puthussery, Chen Zhang, and Vishal Verma
Atmos. Meas. Tech., 11, 5767–5780, https://doi.org/10.5194/amt-11-5767-2018, https://doi.org/10.5194/amt-11-5767-2018, 2018
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The oxidative potential (OP) of ambient particulate matter (PM) has recently gained attention as an alternative metric for assessing the ambient PM toxicity. However, a major constraint in measuring the OP is its labor-intensive protocol. Here, we developed a new online instrument by coupling a mist chamber to an automated analytical system which can measure the real-time OP of ambient PM. We also report for the first time, the hourly averaged diurnal profile of ambient PM OP at an urban site.
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.
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.
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.
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.
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.
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.
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.
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.
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.
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.
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.
H. Guo, L. Xu, A. Bougiatioti, K. M. Cerully, S. L. Capps, J. R. Hite Jr., A. G. Carlton, S.-H. Lee, M. H. Bergin, N. L. Ng, A. Nenes, and R. J. Weber
Atmos. Chem. Phys., 15, 5211–5228, https://doi.org/10.5194/acp-15-5211-2015, https://doi.org/10.5194/acp-15-5211-2015, 2015
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Particle pH can affect many aerosol processes, including gas-particle partitioning, SOA formation, and mobilization of toxic redox metals. pH is challenging to directly measure and often improperly characterized by proxies like ion balances or molar ratios of measured aerosol ionic species. We present a detailed analysis predicting pH with a thermodynamic model, verify the prediction, and test pH sensitivity to model inputs based on data from the SOAS field campaign.
J. W. Taylor, J. D. Allan, D. Liu, M. Flynn, R. Weber, X. Zhang, B. L. Lefer, N. Grossberg, J. Flynn, and H. Coe
Atmos. Meas. Tech., 8, 1701–1718, https://doi.org/10.5194/amt-8-1701-2015, https://doi.org/10.5194/amt-8-1701-2015, 2015
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When using the SP2 to report black carbon core/shell coating thickness, the core density and refractive index must be estimated from literature values. We systematically vary the assumed parameters and the instrument calibration, and quantify the effects in the derived coatings. The technique is highly sensitive to the core refractive index but has only a minor sensitivity to the core density and coating refractive index. We identify the most appropriate values to use in future analysis.
C. J. Hennigan, J. Izumi, A. P. Sullivan, R. J. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 2775–2790, https://doi.org/10.5194/acp-15-2775-2015, https://doi.org/10.5194/acp-15-2775-2015, 2015
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We show that the ion balance and molar ratio methods are unsuitable for use as aerosol pH proxies. Our recommendation is that 1) thermodynamic equilibrium models constrained by both gas and aerosol inputs run in the forward (open) mode, and 2) the phase partitioning of ammonia provides the best predictions of aerosol pH. Given the significance of acidity for numerous chemical processes in the atmosphere, the implications of this study are important and far reaching.
B. Yuan, P. R. Veres, C. Warneke, J. M. Roberts, J. B. Gilman, A. Koss, P. M. Edwards, M. Graus, W. C. Kuster, S.-M. Li, R. J. Wild, S. S. Brown, W. P. Dubé, B. M. Lerner, E. J. Williams, J. E. Johnson, P. K. Quinn, T. S. Bates, B. Lefer, P. L. Hayes, J. L. Jimenez, R. J. Weber, R. Zamora, B. Ervens, D. B. Millet, B. Rappenglück, and J. A. de Gouw
Atmos. Chem. Phys., 15, 1975–1993, https://doi.org/10.5194/acp-15-1975-2015, https://doi.org/10.5194/acp-15-1975-2015, 2015
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In this work, secondary formation of formic acid at an urban site and a site in an oil and gas production region is studied. We investigated various gas phase formation pathways of formic acid, including those recently proposed, using a box model. The contributions from aerosol-related processes, fog events and air-snow exchange to formic acid are also quantified.
T. Fang, V. Verma, H. Guo, L. E. King, E. S. Edgerton, and R. J. Weber
Atmos. Meas. Tech., 8, 471–482, https://doi.org/10.5194/amt-8-471-2015, https://doi.org/10.5194/amt-8-471-2015, 2015
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This work summarizes a newly developed semi-automated system for quantifying the oxidative potential of aerosol aqueous extracts using the dithiothreitol (DTT) assay. 500 sample analyses indicate that DTT activity in the southeast US is likely not dominated by a unique local source, and sources change with season. The unique large data set generated with the technique described in this paper allows new studies on DTT sources and investigating linkages between reactive oxygen species and health.
V. Verma, T. Fang, H. Guo, L. King, J. T. Bates, R. E. Peltier, E. Edgerton, A. G. Russell, and R. J. Weber
Atmos. Chem. Phys., 14, 12915–12930, https://doi.org/10.5194/acp-14-12915-2014, https://doi.org/10.5194/acp-14-12915-2014, 2014
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The major emission sources of the reactive oxygen species (ROS) associated with ambient particulate matter in the southeastern United States were identified. The study shows biomass burning and secondary aerosol formation as the major sources contributing to the ROS-generating capability of ambient particles. The ubiquitous nature of these two sources suggests widespread population exposures to the toxic aerosol components.
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
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Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
T. K. V. Nguyen, M. D. Petters, S. R. Suda, H. Guo, R. J. Weber, and A. G. Carlton
Atmos. Chem. Phys., 14, 10911–10930, https://doi.org/10.5194/acp-14-10911-2014, https://doi.org/10.5194/acp-14-10911-2014, 2014
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
Y. Cheng, G. Engling, K.-B. He, F.-K. Duan, Y.-L. Ma, Z.-Y. Du, J.-M. Liu, M. Zheng, and R. J. Weber
Atmos. Chem. Phys., 13, 7765–7781, https://doi.org/10.5194/acp-13-7765-2013, https://doi.org/10.5194/acp-13-7765-2013, 2013
L. E. King and R. J. Weber
Atmos. Meas. Tech., 6, 1647–1658, https://doi.org/10.5194/amt-6-1647-2013, https://doi.org/10.5194/amt-6-1647-2013, 2013
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
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Measurement report: The chemical composition of and temporal variability in aerosol particles at Tuktoyaktuk, Canada, during the Year of Polar Prediction Second Special Observing Period
Ammonium nitrate promotes sulfate formation through uptake kinetic regime
Measurement report: Indirect evidence for the controlling influence of acidity on the speciation of iodine in Atlantic aerosols
Urban aerosol chemistry at a land–water transition site during summer – Part 1: Impact of agricultural and industrial ammonia emissions
Measurement report: Vertical distribution of biogenic and anthropogenic secondary organic aerosols in the urban boundary layer over Beijing during late summer
Source-specific light absorption by carbonaceous components in the complex aerosol matrix from yearly filter-based measurements
Variability in black carbon mass concentration in surface snow at Svalbard
Rapid mass growth and enhanced light extinction of atmospheric aerosols during the heating season haze episodes in Beijing revealed by aerosol–chemistry–radiation–boundary layer interaction
Measurement report: Saccharide composition in atmospheric fine particulate matter during spring at the remote sites of southwest China and estimates of source contributions
Gas–particle partitioning of polyol tracers at a suburban site in Nanjing, east China: increased partitioning to the particle phase
Measurement report: Source characteristics of water-soluble organic carbon in PM2.5 at two sites in Japan, as assessed by long-term observation and stable carbon isotope ratio
The importance of sesquiterpene oxidation products for secondary organic aerosol formation in a springtime hemiboreal forest
PM1 composition and source apportionment at two sites in Delhi, India, across multiple seasons
Increase of nitrooxy organosulfates in firework-related urban aerosols during Chinese New Year's Eve
Differentiation of coarse-mode anthropogenic, marine and dust particles in the High Arctic islands of Svalbard
Source apportionment of atmospheric PM10 oxidative potential: synthesis of 15 year-round urban datasets in France
Measurement report: Long-emission-wavelength chromophores dominate the light absorption of brown carbon in aerosols over Bangkok: impact from biomass burning
Secondary organic aerosols from anthropogenic volatile organic compounds contribute substantially to air pollution mortality
Dramatic changes in Harbin aerosol during 2018–2020: the roles of open burning policy and secondary aerosol formation
Mediterranean nascent sea spray organic aerosol and relationships with seawater biogeochemistry
Seasonal analysis of submicron aerosol in Old Delhi using high-resolution aerosol mass spectrometry: chemical characterisation, source apportionment and new marker identification
Eight years of sub-micrometre organic aerosol composition data from the boreal forest characterized using a machine-learning approach
Quantification of solid fuel combustion and aqueous chemistry contributions to secondary organic aerosol during wintertime haze events in Beijing
Large seasonal and interannual variations of biogenic sulfur compounds in the Arctic atmosphere (Svalbard; 78.9° N, 11.9° E)
Disparities in particulate matter (PM10) origins and oxidative potential at a city scale (Grenoble, France) – Part 2: Sources of PM10 oxidative potential using multiple linear regression analysis and the predictive applicability of multilayer perceptron neural network analysis
Inter-annual variations of wet deposition in Beijing from 2014–2017: implications of below-cloud scavenging of inorganic aerosols
Urban organic aerosol composition in eastern China differs from north to south: molecular insight from a liquid chromatography–mass spectrometry (Orbitrap) study
Cultivable halotolerant ice-nucleating bacteria and fungi in coastal precipitation
Determination of free amino acids, saccharides, and selected microbes in biogenic atmospheric aerosols – seasonal variations, particle size distribution, chemical and microbial relations
Physical and chemical properties of urban aerosols in São Paulo, Brazil: links between composition and size distribution of submicron particles
Substantial changes in gaseous pollutants and chemical compositions in fine particles in the North China Plain during the COVID-19 lockdown period: anthropogenic vs. meteorological influences
Measurement report: Spatiotemporal and policy-related variations of PM2.5 compositions and sources during 2015–2019 at multisite of a Chinese megacity
Measurement report: Molecular composition, optical properties, and radiative effects of water-soluble organic carbon in snowpack samples from northern Xinjiang, China
Reduced volatility of aerosols from surface emission to the top of planetary boundary layer
Spatiotemporal Variability in the Oxidative Potential of Ambient Fine Particulate Matter in Midwestern United States
Significant contrasts in aerosol acidity between China and the United States
Increase in secondary organic aerosol in an urban environment
Carbonaceous aerosol composition in air masses influenced by large-scale biomass burning: a case study in northwestern Vietnam
The role of coarse aerosol particles as a sink of HNO3 in wintertime pollution events in the Salt Lake Valley
Molecular characterization of gaseous and particulate oxygenated compounds at a remote site in Cape Corsica in the western Mediterranean Basin
Aircraft measurements of aerosol and trace gas chemistry in the eastern North Atlantic
Impacts of the COVID-19 lockdown on air pollution at regional and urban background sites in northern Italy
Measurement report: Fourteen months of real-time characterisation of the submicronic aerosol and its atmospheric dynamics at the Marseille–Longchamp supersite
Trends, composition, and sources of carbonaceous aerosol at the Birkenes Observatory, northern Europe, 2001–2018
Enhancement of nanoparticle formation and growth during the COVID-19 lockdown period in urban Beijing
Chemical composition and source attribution of sub-micrometre aerosol particles in the summertime Arctic lower troposphere
Sources of black carbon at residential and traffic environments
In-depth characterization of submicron particulate matter inter-annual variations at a street canyon site in northern Europe
Measurement report: Firework impacts on air quality in Metro Manila, Philippines, during the 2019 New Year revelry
Measurement report: Receptor modelling for source identification of urban fine and coarse particulate matter using hourly elemental composition
John MacInnis, Jai Prakash Chaubey, Crystal Weagle, David Atkinson, and Rachel Ying-Wen Chang
Atmos. Chem. Phys., 21, 14199–14213, https://doi.org/10.5194/acp-21-14199-2021, https://doi.org/10.5194/acp-21-14199-2021, 2021
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This study measured particulate matter in the western Canadian Arctic during 2018 as part of the Year of Polar Prediction. It was found that the particles were likely from the ocean, soil, road dust, and combustion. The concentrations of small aerosol particles, which can affect human health, were low, suggesting they had little impact on local air quality. These results can be used to understand future changes in local aerosol particle sources and concentrations.
Yongchun Liu, Zemin Feng, Feixue Zheng, Xiaolei Bao, Pengfei Liu, Yanli Ge, Yan Zhao, Tao Jiang, Yunwen Liao, Yusheng Zhang, Xiaolong Fan, Chao Yan, Biwu Chu, Yonghong Wang, Wei Du, Jing Cai, Federico Bianchi, Tuukka Petäjä, Yujing Mu, Hong He, and Markku Kulmala
Atmos. Chem. Phys., 21, 13269–13286, https://doi.org/10.5194/acp-21-13269-2021, https://doi.org/10.5194/acp-21-13269-2021, 2021
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The mechanisms and kinetics of particulate sulfate formation in the atmosphere are still open questions although they have been extensively discussed. We found that uptake of SO2 is the rate-determining step for the conversion of SO2 to particulate sulfate. NH4NO3 plays an important role in AWC, the phase state of aerosol particles, and subsequently the uptake kinetics of SO2 under high-RH conditions. This work is a good example of the feedback between aerosol physics and aerosol chemistry.
Alex R. Baker and Chan Yodle
Atmos. Chem. Phys., 21, 13067–13076, https://doi.org/10.5194/acp-21-13067-2021, https://doi.org/10.5194/acp-21-13067-2021, 2021
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Iodine is emitted from the ocean and helps to destroy ozone in the lower atmosphere before being taken up into aerosol particles. We measured the chemical forms of iodine in aerosols over the Atlantic Ocean, because some of these forms can return to the gas phase and destroy more ozone. Our results indicate that aerosol acidity exerts a strong control on iodine speciation and therefore on its recycling behaviour and impact on ozone concentrations.
Nicholas Balasus, Michael A. Battaglia Jr., Katherine Ball, Vanessa Caicedo, Ruben Delgado, Annmarie G. Carlton, and Christopher J. Hennigan
Atmos. Chem. Phys., 21, 13051–13065, https://doi.org/10.5194/acp-21-13051-2021, https://doi.org/10.5194/acp-21-13051-2021, 2021
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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.
Hong Ren, Wei Hu, Lianfang Wei, Siyao Yue, Jian Zhao, Linjie Li, Libin Wu, Wanyu Zhao, Lujie Ren, Mingjie Kang, Qiaorong Xie, Sihui Su, Xiaole Pan, Zifa Wang, Yele Sun, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 21, 12949–12963, https://doi.org/10.5194/acp-21-12949-2021, https://doi.org/10.5194/acp-21-12949-2021, 2021
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This study presents vertical profiles of biogenic and anthropogenic secondary organic aerosols (SOAs) in the urban boundary layer based on a 325 m tower in Beijing in late summer. The increases in the isoprene and toluene SOAs with height were found to be more related to regional transport, whereas the decrease in those from monoterpenes and sesquiterpene were more subject to local emissions. Such complicated vertical distributions of SOA should be considered in future modeling work.
Vaios Moschos, Martin Gysel-Beer, Robin L. Modini, Joel C. Corbin, Dario Massabò, Camilla Costa, Silvia G. Danelli, Athanasia Vlachou, Kaspar R. Daellenbach, Sönke Szidat, Paolo Prati, André S. H. Prévôt, Urs Baltensperger, and Imad El Haddad
Atmos. Chem. Phys., 21, 12809–12833, https://doi.org/10.5194/acp-21-12809-2021, https://doi.org/10.5194/acp-21-12809-2021, 2021
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This study provides a holistic approach to studying the spectrally resolved light absorption by atmospheric brown carbon (BrC) and black carbon using long time series of daily samples from filter-based measurements. The obtained results provide (1) a better understanding of the aerosol absorption profile and its dependence on BrC and on lensing from less absorbing coatings and (2) an estimation of the most important absorbers at typical European locations.
Michele Bertò, David Cappelletti, Elena Barbaro, Cristiano Varin, Jean-Charles Gallet, Krzysztof Markowicz, Anna Rozwadowska, Mauro Mazzola, Stefano Crocchianti, Luisa Poto, Paolo Laj, Carlo Barbante, and Andrea Spolaor
Atmos. Chem. Phys., 21, 12479–12493, https://doi.org/10.5194/acp-21-12479-2021, https://doi.org/10.5194/acp-21-12479-2021, 2021
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We present the daily and seasonal variability in black carbon (BC) in surface snow inferred from two specific experiments based on the hourly and daily time resolution sampling during the Arctic spring in Svalbard. These unique data sets give us, for the first time, the opportunity to evaluate the associations between the observed surface snow BC mass concentration and a set of predictors corresponding to the considered meteorological and snow physico-chemical parameters.
Zhuohui Lin, Yonghong Wang, Feixue Zheng, Ying Zhou, Yishuo Guo, Zemin Feng, Chang Li, Yusheng Zhang, Simo Hakala, Tommy Chan, Chao Yan, Kaspar R. Daellenbach, Biwu Chu, Lubna Dada, Juha Kangasluoma, Lei Yao, Xiaolong Fan, Wei Du, Jing Cai, Runlong Cai, Tom V. Kokkonen, Putian Zhou, Lili Wang, Tuukka Petäjä, Federico Bianchi, Veli-Matti Kerminen, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 12173–12187, https://doi.org/10.5194/acp-21-12173-2021, https://doi.org/10.5194/acp-21-12173-2021, 2021
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We find that ammonium nitrate and aerosol water content contributed most during low mixing layer height conditions; this may further trigger enhanced formation of sulfate and organic aerosol via heterogeneous reactions. The results of this study contribute towards a more detailed understanding of the aerosol–chemistry–radiation–boundary layer feedback that is likely to be responsible for explosive aerosol mass growth events in urban Beijing.
Zhenzhen Wang, Di Wu, Zhuoyu Li, Xiaona Shang, Qing Li, Xiang Li, Renjie Chen, Haidong Kan, Huiling Ouyang, Xu Tang, and Jianmin Chen
Atmos. Chem. Phys., 21, 12227–12241, https://doi.org/10.5194/acp-21-12227-2021, https://doi.org/10.5194/acp-21-12227-2021, 2021
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This study firstly investigates the composition of sugars in the fine fraction of aerosol over three sites in southwest China. The result suggested no significant reduction in biomass burning emissions in southwest Yunnan Province to some extent. The result shown sheds light on the contributions of biomass burning and the characteristics of biogenic saccharides in these regions, which could be further applied to regional source apportionment models and global climate models.
Chao Qin, Yafeng Gou, Yuhang Wang, Yuhao Mao, Hong Liao, Qin'geng Wang, and Mingjie Xie
Atmos. Chem. Phys., 21, 12141–12153, https://doi.org/10.5194/acp-21-12141-2021, https://doi.org/10.5194/acp-21-12141-2021, 2021
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In this study, we found that the aqueous solution in aerosols is an important absorbing phase for gaseous polyols in the atmosphere, indicating that the dissolution in aerosol liquid water should not be ignored when investigating gas–particle partitioning of water-soluble organics. The exponential increase in effective partitioning coefficients of polyol tracers with sulfate ion concentrations could be attributed to organic–inorganic interactions in the particle phase.
Nana Suto and Hiroto Kawashima
Atmos. Chem. Phys., 21, 11815–11828, https://doi.org/10.5194/acp-21-11815-2021, https://doi.org/10.5194/acp-21-11815-2021, 2021
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The sources and seasonal trends of water-soluble organic carbon (WSOC) in PM2.5 on long-term trends at two sites in Japan are investigated by carbon isotope ratio (δ13C) of WSOC. At the rural site, the δ13C of WSOC from autumn to spring was concluded to reflect mainly the biomass burning of rice straw. The heaviest δ13C of WSOC from February to April 2019 might reflect long-range transport of particles resulting from the overseas burning of C4 plants such as corn.
Luis M. F. Barreira, Arttu Ylisirniö, Iida Pullinen, Angela Buchholz, Zijun Li, Helina Lipp, Heikki Junninen, Urmas Hõrrak, Steffen M. Noe, Alisa Krasnova, Dmitrii Krasnov, Kaia Kask, Eero Talts, Ülo Niinemets, Jose Ruiz-Jimenez, and Siegfried Schobesberger
Atmos. Chem. Phys., 21, 11781–11800, https://doi.org/10.5194/acp-21-11781-2021, https://doi.org/10.5194/acp-21-11781-2021, 2021
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We present results from PM1 atmospheric composition and concentration measurements performed in a springtime hemiboreal forest. Sesquiterpene mixing ratios and particle-phase concentrations of corresponding oxidation products were rapidly increasing on some early mornings. The particle volatility suggested that condensable sesquiterpene oxidation products are rapidly formed in the atmosphere. The results revealed the importance of sesquiterpenes for secondary organic aerosol particulate mass.
Ernesto Reyes-Villegas, Upasana Panda, Eoghan Darbyshire, James M. Cash, Rutambhara Joshi, Ben Langford, Chiara F. Di Marco, Neil J. Mullinger, Mohammed S. Alam, Leigh R. Crilley, Daniel J. Rooney, W. Joe F. Acton, Will Drysdale, Eiko Nemitz, Michael Flynn, Aristeidis Voliotis, Gordon McFiggans, Hugh Coe, James Lee, C. Nicholas Hewitt, Mathew R. Heal, Sachin S. Gunthe, Tuhin K. Mandal, Bhola R. Gurjar, Shivani, Ranu Gadi, Siddhartha Singh, Vijay Soni, and James D. Allan
Atmos. Chem. Phys., 21, 11655–11667, https://doi.org/10.5194/acp-21-11655-2021, https://doi.org/10.5194/acp-21-11655-2021, 2021
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This paper shows the first multisite online measurements of PM1 in Delhi, India, with measurements over different seasons in Old Delhi and New Delhi in 2018. Organic aerosol (OA) source apportionment was performed using positive matrix factorisation (PMF). Traffic was the main primary aerosol source for both OAs and black carbon, seen with PMF and Aethalometer model analysis, indicating that control of primary traffic exhaust emissions would make a significant reduction to Delhi air pollution.
Qiaorong Xie, Sihui Su, Jing Chen, Yuqing Dai, Siyao Yue, Hang Su, Haijie Tong, Wanyu Zhao, Lujie Ren, Yisheng Xu, Dong Cao, Ying Li, Yele Sun, Zifa Wang, Cong-Qiang Liu, Kimitaka Kawamura, Guibin Jiang, Yafang Cheng, and Pingqing Fu
Atmos. Chem. Phys., 21, 11453–11465, https://doi.org/10.5194/acp-21-11453-2021, https://doi.org/10.5194/acp-21-11453-2021, 2021
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This study investigated the role of nighttime chemistry during Chinese New Year's Eve that enhances the formation of nitrooxy organosulfates in the aerosol phase. Results show that anthropogenic precursors, together with biogenic ones, considerably contribute to the formation of low-volatility nitrooxy OSs. Our study provides detailed molecular composition of firework-related aerosols, which gives new insights into the physicochemical properties and potential health effects of urban aerosols.
Congbo Song, Manuel Dall'Osto, Angelo Lupi, Mauro Mazzola, Rita Traversi, Silvia Becagli, Stefania Gilardoni, Stergios Vratolis, Karl Espen Yttri, David C. S. Beddows, Julia Schmale, James Brean, Agung Ghani Kramawijaya, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 11317–11335, https://doi.org/10.5194/acp-21-11317-2021, https://doi.org/10.5194/acp-21-11317-2021, 2021
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We present a cluster analysis of relatively long-term (2015–2019) aerosol aerodynamic volume size distributions up to 20 μm in the Arctic for the first time. The study found that anthropogenic and natural aerosols comprised 27 % and 73 % of the occurrence of the coarse-mode aerosols, respectively. Our study shows that about two-thirds of the coarse-mode aerosols are related to two sea-spray-related aerosol clusters, indicating that sea spray aerosol may more complex in the Arctic environment.
Samuël Weber, Gaëlle Uzu, Olivier Favez, Lucille Joanna S. Borlaza, Aude Calas, Dalia Salameh, Florie Chevrier, Julie Allard, Jean-Luc Besombes, Alexandre Albinet, Sabrina Pontet, Boualem Mesbah, Grégory Gille, Shouwen Zhang, Cyril Pallares, Eva Leoz-Garziandia, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 21, 11353–11378, https://doi.org/10.5194/acp-21-11353-2021, https://doi.org/10.5194/acp-21-11353-2021, 2021
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Oxidative potential (OP) of aerosols is apportioned to the main PM sources found in 15 sites over France. The sources present clear distinct intrinsic OPs at a large geographic scale, and a drastic redistribution between the mass concentration and OP measured by both ascorbic acid and dithiothreitol is highlighted. Moreover, the high discrepancy between the mean and median contributions of the sources to the given metrics raises some important questions when dealing with health endpoints.
Jiao Tang, Jiaqi Wang, Guangcai Zhong, Hongxing Jiang, Yangzhi Mo, Bolong Zhang, Xiaofei Geng, Yingjun Chen, Jianhui Tang, Congguo Tian, Surat Bualert, Jun Li, and Gan Zhang
Atmos. Chem. Phys., 21, 11337–11352, https://doi.org/10.5194/acp-21-11337-2021, https://doi.org/10.5194/acp-21-11337-2021, 2021
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This article provides a combined EEM–PARAFAC and statistical analysis method to explore how excitation–emission matrix (EEM) chromophores influence BrC light absorption in soluble organic matter. The application enables us to deduce that BrC absorption is mainly dependent on longer-emission-wavelength chromophores largely associated with biomass burning emissions. This method promotes the application of EEM spectroscopy and helps us understand the light absorption of BrC in the atmosphere.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Yuan Cheng, Qin-qin Yu, Jiu-meng Liu, Xu-bing Cao, Ying-jie Zhong, Zhen-yu Du, Lin-lin Liang, Guan-nan Geng, Wan-li Ma, Hong Qi, Qiang Zhang, and Ke-bin He
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-522, https://doi.org/10.5194/acp-2021-522, 2021
Revised manuscript accepted for ACP
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Open burning policies in Heilongjiang Province experienced a rapid transition during 2018 to 2020. This study evaluated the responses of PM2.5 pollution to this transition, and suggested neither of the policies could be considered successful. In addition, heterogeneous reactions were found to be at play in secondary aerosol formation, even in the frigid atmosphere in Heilongjiang. The unique haze in Northeast China deserves more attention.
Evelyn Freney, Karine Sellegri, Alessia Nicosia, Leah R. Williams, Matteo Rinaldi, Jonathan T. Trueblood, André S. H. Prévôt, Melilotus Thyssen, Gérald Grégori, Nils Haëntjens, Julie Dinasquet, Ingrid Obernosterer, France Van Wambeke, Anja Engel, Birthe Zäncker, Karine Desboeufs, Eija Asmi, Hilkka Timonen, and Cécile Guieu
Atmos. Chem. Phys., 21, 10625–10641, https://doi.org/10.5194/acp-21-10625-2021, https://doi.org/10.5194/acp-21-10625-2021, 2021
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In this work, we present observations of the organic aerosol content in primary sea spray aerosols (SSAs) continuously generated along a 5-week cruise in the Mediterranean. This information is combined with seawater biogeochemical properties also measured continuously along the ship track to develop a number of parametrizations that can be used in models to determine SSA organic content in oligotrophic waters that represent 60 % of the oceans from commonly measured seawater variables.
James M. Cash, Ben Langford, Chiara Di Marco, Neil J. Mullinger, James Allan, Ernesto Reyes-Villegas, Ruthambara Joshi, Mathew R. Heal, W. Joe F. Acton, C. Nicholas Hewitt, Pawel K. Misztal, Will Drysdale, Tuhin K. Mandal, Shivani, Ranu Gadi, Bhola Ram Gurjar, and Eiko Nemitz
Atmos. Chem. Phys., 21, 10133–10158, https://doi.org/10.5194/acp-21-10133-2021, https://doi.org/10.5194/acp-21-10133-2021, 2021
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We present the first real-time composition of submicron particulate matter (PM1) in Old Delhi using high-resolution aerosol mass spectrometry. Seasonal analysis shows peak concentrations occur during the post-monsoon, and novel-tracers reveal the largest sources are a combination of local open and regional crop residue burning. Strong links between increased chloride aerosol concentrations and burning sources of PM1 suggest burning sources are responsible for the post-monsoon chloride peak.
Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Gang Chen, Olga Garmash, Diego Aliaga, Frans Graeffe, Meri Räty, Krista Luoma, Pasi Aalto, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 21, 10081–10109, https://doi.org/10.5194/acp-21-10081-2021, https://doi.org/10.5194/acp-21-10081-2021, 2021
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In many locations worldwide aerosol particles have been shown to be made up of organic aerosol (OA). The boreal forest is a region where aerosol particles possess a high OA mass fraction. Here, we studied OA composition using the longest time series of OA composition ever obtained from a boreal environment. For this purpose, we tested a new analysis framework and discovered that most of the OA was highly oxidized, with strong seasonal behaviour reflecting different sources in summer and winter.
Yandong Tong, Veronika Pospisilova, Lu Qi, Jing Duan, Yifang Gu, Varun Kumar, Pragati Rai, Giulia Stefenelli, Liwei Wang, Ying Wang, Haobin Zhong, Urs Baltensperger, Junji Cao, Ru-Jin Huang, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 21, 9859–9886, https://doi.org/10.5194/acp-21-9859-2021, https://doi.org/10.5194/acp-21-9859-2021, 2021
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We investigate SOA sources and formation processes by a field deployment of the EESI-TOF-MS and L-TOF AMS in Beijing in late autumn and early winter. Our study shows that the sources and processes giving rise to haze events in Beijing are variable and seasonally dependent: (1) in the heating season, SOA formation is driven by oxidation of aromatics from solid fuel combustion; and (2) under high-NOx and RH conditions, aqueous-phase chemistry can be a major contributor to SOA formation.
Sehyun Jang, Ki-Tae Park, Kitack Lee, Young Jun Yoon, Kitae Kim, Hyun Young Chung, Eunho Jang, Silvia Becagli, Bang Yong Lee, Rita Traversi, Konstantinos Eleftheriadis, Radovan Krejci, and Ove Hermansen
Atmos. Chem. Phys., 21, 9761–9777, https://doi.org/10.5194/acp-21-9761-2021, https://doi.org/10.5194/acp-21-9761-2021, 2021
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This study provides comprehensive datasets encompassing seasonal and interannual variations in sulfate and MSA concentration in aerosol particles in the Arctic atmosphere. As oxidation products of DMS have important roles in new particle formation and growth, we focused on factors affecting their variability and the branching ratio of DMS oxidation. We found a strong correlation between the ratio and the light condition, chemical properties of particles, and biological activities near Svalbard.
Lucille Joanna S. Borlaza, Samuël Weber, Jean-Luc Jaffrezo, Stephan Houdier, Rémy Slama, Camille Rieux, Alexandre Albinet, Steve Micallef, Cécile Trébluchon, and Gaëlle Uzu
Atmos. Chem. Phys., 21, 9719–9739, https://doi.org/10.5194/acp-21-9719-2021, https://doi.org/10.5194/acp-21-9719-2021, 2021
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With an enhanced source apportionment obtained in a companion paper, this paper acquires more understanding of the spatiotemporal associations of the sources of PM to oxidative potential (OP), an emerging health-based metric. Multilayer perceptron neural network analysis was used to apportion OP from PM sources. Results showed that such a methodology is as robust as the linear classical inversion and permits an improvement in the OP prediction when local features or non-linear effects occur.
Baozhu Ge, Danhui Xu, Oliver Wild, Xuefeng Yao, Junhua Wang, Xueshun Chen, Qixin Tan, Xiaole Pan, and Zifa Wang
Atmos. Chem. Phys., 21, 9441–9454, https://doi.org/10.5194/acp-21-9441-2021, https://doi.org/10.5194/acp-21-9441-2021, 2021
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In this study, an improved sequential sampling method is developed and implemented to estimate the contribution of below-cloud and in-cloud wet deposition over four years of measurements in Beijing. We find that the contribution of below-cloud scavenging for Ca2+, SO4 2–, and NH4+ decreases from above 50 % in 2014 to below 40 % in 2017. This suggests that the Action Plan has mitigated particulate matter pollution in the surface layer and hence decreased scavenging due to the washout process.
Kai Wang, Ru-Jin Huang, Martin Brüggemann, Yun Zhang, Lu Yang, Haiyan Ni, Jie Guo, Meng Wang, Jiajun Han, Merete Bilde, Marianne Glasius, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 9089–9104, https://doi.org/10.5194/acp-21-9089-2021, https://doi.org/10.5194/acp-21-9089-2021, 2021
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Here we present the detailed molecular composition of the organic aerosol collected in three eastern Chinese cities from north to south, Changchun, Shanghai and Guangzhou, by applying LC–Orbitrap analysis. Accordingly, the aromaticity degree of chemical compounds decreases from north to south, while the oxidation degree increases from north to south, which can be explained by the different anthropogenic emissions and photochemical oxidation processes.
Charlotte M. Beall, Jennifer M. Michaud, Meredith A. Fish, Julie Dinasquet, Gavin C. Cornwell, M. Dale Stokes, Michael D. Burkart, Thomas C. Hill, Paul J. DeMott, and Kimberly A. Prather
Atmos. Chem. Phys., 21, 9031–9045, https://doi.org/10.5194/acp-21-9031-2021, https://doi.org/10.5194/acp-21-9031-2021, 2021
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Ice-nucleating particles (INPs) can influence multiple climate-relevant cloud properties by triggering droplet freezing at relative humidities below or temperatures above the freezing point of water. The ocean is a significant INP source; however, the specific identities of marine INPs remain largely unknown. Here, we identify 14 ice-nucleating microbes from aerosol and precipitation samples collected at a coastal site in southern California, two or more of which are likely marine.
Jose Ruiz-Jimenez, Magdalena Okuljar, Outi-Maaria Sietiö, Giorgia Demaria, Thanaporn Liangsupree, Elisa Zagatti, Juho Aalto, Kari Hartonen, Jussi Heinonsalo, Jaana Bäck, Tuukka Petäjä, and Marja-Liisa Riekkola
Atmos. Chem. Phys., 21, 8775–8790, https://doi.org/10.5194/acp-21-8775-2021, https://doi.org/10.5194/acp-21-8775-2021, 2021
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Altogether, 84 size-segregated aerosol samples from four particle size fractions were collected at the Station for Measuring Forest Ecosystem-Atmosphere Relations, Hyytiälä, Finland, in autumn 2017 for the clarification of the complex interrelationships between airborne and particulate chemical traces, amino acids and saccharides, gene copy numbers (16S and 18S for bacteria and fungi, respectively), gas-phase chemistry, and the particle size distribution.
Djacinto Monteiro dos Santos, Luciana Varanda Rizzo, Samara Carbone, Patrick Schlag, and Paulo Artaxo
Atmos. Chem. Phys., 21, 8761–8773, https://doi.org/10.5194/acp-21-8761-2021, https://doi.org/10.5194/acp-21-8761-2021, 2021
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The metropolitan area of São Paulo (MASP), with very extensive biofuel use, has unique atmospheric chemistry among world megacities. In this study, we examine the complex relationships between aerosol chemical composition and particle size distribution. Our findings provide a better understanding of the dynamics of the physicochemical properties of submicron particles and highlight the key role of secondary organic aerosol formation in the pollution levels in São Paulo.
Rui Li, Yilong Zhao, Hongbo Fu, Jianmin Chen, Meng Peng, and Chunying Wang
Atmos. Chem. Phys., 21, 8677–8692, https://doi.org/10.5194/acp-21-8677-2021, https://doi.org/10.5194/acp-21-8677-2021, 2021
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Based on a random forest model, the strict lockdown measures significantly decreased primary components such as Cr (−67 %) and Fe (−61 %) in PM2.5 (p < 0.01), whereas the higher relative humidity (RH) and NH3 level and the lower air temperature (T) remarkably enhanced the production of secondary aerosol including SO42− (29 %), NO3− (29 %), and NH4+ (21 %) (p < 0.05). The natural experiment suggested that the NH3 emission should be strictly controlled.
Xinyao Feng, Yingze Tian, Qianqian Xue, Danlin Song, Fengxia Huang, and Yinchang Feng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-311, https://doi.org/10.5194/acp-2021-311, 2021
Revised manuscript accepted for ACP
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This study focused on PM2.5 compositions and sources, and explored their spatiotemporal and policy-related variations based on observation at 19 sites during wintertime of 2015–2019 in a fast-developing megacity. We found that PM2.5 compositions for outer-most zone in 2019 were similar to that for core zone two or three years ago. Percentage contributions of coal and biomass combustion dramatically declined in core zone, while traffic source showed an increasing trend.
Yue Zhou, Christopher P. West, Anusha P. S. Hettiyadura, Xiaoying Niu, Hui Wen, Jiecan Cui, Tenglong Shi, Wei Pu, Xin Wang, and Alexander Laskin
Atmos. Chem. Phys., 21, 8531–8555, https://doi.org/10.5194/acp-21-8531-2021, https://doi.org/10.5194/acp-21-8531-2021, 2021
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We present a comprehensive characterization of water-soluble organic carbon (WSOC) in seasonal snow of northwestern China. We applied complementary multimodal analytical techniques to investigate bulk and molecular-level composition, optical properties, and sources of WSOC. For the first time, we estimated the extent of radiative forcing due to WSOC in snow using a model simulation and showed the profound influences of WSOC on the energy budget of midlatitude seasonal snowpack.
Quan Liu, Dantong Liu, Yangzhou Wu, Kai Bi, Wenkang Gao, Ping Tian, Delong Zhao, Siyuan Li, Chenjie Yu, Yunfei Wu, Kang Hu, Shuo Ding, Qian Gao, Fei Wang, Hui He, Mengyu Huang, and Deping Ding
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-362, https://doi.org/10.5194/acp-2021-362, 2021
Revised manuscript accepted for ACP
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Through simultaneous online measurements of detailed aerosol compositions at both surface and surface-influenced mountain sites, the evolution of aerosol composition during daytime vertical transport was investigated. The results show that from surface to the top of the PBL, the oxidation state of organic aerosol had been significantly enhanced due to evaporation and further oxidation on these evaporated gases.
Haoran Yu, Joseph Varghese Puthussery, Yixiang Wang, and Vishal Verma
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-376, https://doi.org/10.5194/acp-2021-376, 2021
Revised manuscript accepted for ACP
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We assessed the oxidative potential (OP) of ambient PM2.5 collected from five sites in the Midwest US. Compared to the homogeneously distributed PM2.5 mass, OP showed high spatiotemporal variation. Weak correlations for the regression between mass and OP indicated a limited role of mass in determining the OP. Moreover, the intercorrelations among different OP endpoints were not strong, justifying the need for using multiple assays for determining the oxidative levels of the particles.
Bingqing Zhang, Huizhong Shen, Pengfei Liu, Hongyu Guo, Yongtao Hu, Yilin Chen, Shaodong Xie, Ziyan Xi, T. Nash Skipper, and Armistead G. Russell
Atmos. Chem. Phys., 21, 8341–8356, https://doi.org/10.5194/acp-21-8341-2021, https://doi.org/10.5194/acp-21-8341-2021, 2021
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Extended ground-level measurements are coupled with model simulations to comprehensively compare the aerosol acidity in China and the United States. Aerosols in China are significantly less acidic than those in the United States, with pH values 1–2 units higher. Higher aerosol mass concentrations and the abundance of ammonia and ammonium in China, compared to the United States, are leading causes of the pH difference between these two countries.
Marta Via, María Cruz Minguillón, Cristina Reche, Xavier Querol, and Andrés Alastuey
Atmos. Chem. Phys., 21, 8323–8339, https://doi.org/10.5194/acp-21-8323-2021, https://doi.org/10.5194/acp-21-8323-2021, 2021
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Atmospheric pollutants have been measured in an urban environment by means of state-of-the-art techniques, allowing the origin and the sources of pollution to be identified. Recent years are shown to be increasingly dominated by non-directly emitted particulate matter. Knowledge about the sources of atmospheric pollutants is necessary to design effective mitigation policies.
Dac-Loc Nguyen, Hendryk Czech, Simone M. Pieber, Jürgen Schnelle-Kreis, Martin Steinbacher, Jürgen Orasche, Stephan Henne, Olga B. Popovicheva, Gülcin Abbaszade, Guenter Engling, Nicolas Bukowiecki, Nhat-Anh Nguyen, Xuan-Anh Nguyen, and Ralf Zimmermann
Atmos. Chem. Phys., 21, 8293–8312, https://doi.org/10.5194/acp-21-8293-2021, https://doi.org/10.5194/acp-21-8293-2021, 2021
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Southeast Asia is well-known for emission-intense and recurring wildfires and after-harvest crop residue burning during the pre-monsoon season from February to April. We describe a biomass burning (BB) plume arriving at remote Pha Din meteorological station, outline its carbonaceous particulate matter (PM) constituents based on more than 50 target compounds and discuss possible BB sources. This study adds valuable information on chemical PM composition for a region with scarce data availability.
Amy Hrdina, Jennifer G. Murphy, Anna Gannet Hallar, John C. Lin, Alexander Moravek, Ryan Bares, Ross C. Petersen, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Munkh Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 21, 8111–8126, https://doi.org/10.5194/acp-21-8111-2021, https://doi.org/10.5194/acp-21-8111-2021, 2021
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Wintertime air pollution in the Salt Lake Valley is primarily composed of ammonium nitrate, which is formed when gas-phase ammonia and nitric acid react. The major point in this work is that the chemical composition of snow tells a very different story to what we measured in the atmosphere. With the dust–sea salt cations observed in PM2.5 and particle sizing data, we can estimate how much nitric acid may be lost to dust–sea salt that is not accounted for and how much more PM2.5 this could form.
Vincent Michoud, Elise Hallemans, Laura Chiappini, Eva Leoz-Garziandia, Aurélie Colomb, Sébastien Dusanter, Isabelle Fronval, François Gheusi, Jean-Luc Jaffrezo, Thierry Léonardis, Nadine Locoge, Nicolas Marchand, Stéphane Sauvage, Jean Sciare, and Jean-François Doussin
Atmos. Chem. Phys., 21, 8067–8088, https://doi.org/10.5194/acp-21-8067-2021, https://doi.org/10.5194/acp-21-8067-2021, 2021
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A multiphasic molecular characterization of oxygenated compounds has been carried out during the ChArMEx field campaign using offline analysis. It leads to the identification of 97 different compounds in the gas and aerosol phases and reveals the important contribution of organic acids to organic aerosol. In addition, comparison between experimental and theoretical partitioning coefficients revealed in most cases a large underestimation by the theory reaching 1 to 7 orders of magnitude.
Maria A. Zawadowicz, Kaitlyn Suski, Jiumeng Liu, Mikhail Pekour, Jerome Fast, Fan Mei, Arthur J. Sedlacek, Stephen Springston, Yang Wang, Rahul A. Zaveri, Robert Wood, Jian Wang, and John E. Shilling
Atmos. Chem. Phys., 21, 7983–8002, https://doi.org/10.5194/acp-21-7983-2021, https://doi.org/10.5194/acp-21-7983-2021, 2021
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This paper describes the results of a recent field campaign in the eastern North Atlantic, where two mass spectrometers were deployed aboard a research aircraft to measure the chemistry of aerosols and trace gases. Very clean conditions were found, dominated by local sulfate-rich acidic aerosol and very aged organics. Evidence of
long-range transport of aerosols from the continents was also identified.
Jean-Philippe Putaud, Luca Pozzoli, Enrico Pisoni, Sebastiao Martins Dos Santos, Friedrich Lagler, Guido Lanzani, Umberto Dal Santo, and Augustin Colette
Atmos. Chem. Phys., 21, 7597–7609, https://doi.org/10.5194/acp-21-7597-2021, https://doi.org/10.5194/acp-21-7597-2021, 2021
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To determine the impact of the COVID lockdown on air quality in northern Italy, measurements of atmospheric pollutants (NO2, PM10, O3, NO, SO2 ) were compared to the output of a model ignoring the lockdown. We found that NO2 decreased on average by −30 % to −40 %. Unlike NO2, PM10 was not significantly affected due to the compensation of decreased emissions from traffic by increased emissions from domestic heating and/or by changes in atmospheric chemistry enhancing secondary aerosol formation.
Benjamin Chazeau, Brice Temime-Roussel, Grégory Gille, Boualem Mesbah, Barbara D'Anna, Henri Wortham, and Nicolas Marchand
Atmos. Chem. Phys., 21, 7293–7319, https://doi.org/10.5194/acp-21-7293-2021, https://doi.org/10.5194/acp-21-7293-2021, 2021
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The temporal trends in the chemical composition and particle number of the submicron aerosols in a Mediterranean city, Marseille, are investigated over 14 months. Fifteen days were found to exceed the WHO PM2.5 daily limit (25 µg m−3) only during the cold period, with two distinct origins: local pollution events with an increased fraction of the carbonaceous fraction due to domestic wood burning and long-range pollution events with a high level of oxygenated organic aerosol and ammonium nitrate.
Karl Espen Yttri, Francesco Canonaco, Sabine Eckhardt, Nikolaos Evangeliou, Markus Fiebig, Hans Gundersen, Anne-Gunn Hjellbrekke, Cathrine Lund Myhre, Stephen Matthew Platt, André S. H. Prévôt, David Simpson, Sverre Solberg, Jason Surratt, Kjetil Tørseth, Hilde Uggerud, Marit Vadset, Xin Wan, and Wenche Aas
Atmos. Chem. Phys., 21, 7149–7170, https://doi.org/10.5194/acp-21-7149-2021, https://doi.org/10.5194/acp-21-7149-2021, 2021
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Carbonaceous aerosol sources and trends were studied at the Birkenes Observatory. A large decrease in elemental carbon (EC; 2001–2018) and a smaller decline in levoglucosan (2008–2018) suggest that organic carbon (OC)/EC from traffic/industry is decreasing, whereas the abatement of OC/EC from biomass burning has been less successful. Positive matrix factorization apportioned 72 % of EC to fossil fuel sources and 53 % (PM2.5) and 78 % (PM10–2.5) of OC to biogenic sources.
Xiaojing Shen, Junying Sun, Fangqun Yu, Ying Wang, Junting Zhong, Yangmei Zhang, Xinyao Hu, Can Xia, Sinan Zhang, and Xiaoye Zhang
Atmos. Chem. Phys., 21, 7039–7052, https://doi.org/10.5194/acp-21-7039-2021, https://doi.org/10.5194/acp-21-7039-2021, 2021
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In this work, we revealed the changes of PNSD and NPF events during the COVID-19 lockdown period in Beijing, China, to illustrate the impact of reduced primary emission and elavated atmospheric oxidized capicity on the nucleation and growth processes. The subsequent growth of nucleated particles and their contribution to the aerosol pollution formation were also explored, to highlight the necessity of controlling the nanoparticles in the future air quality management.
Franziska Köllner, Johannes Schneider, Megan D. Willis, Hannes Schulz, Daniel Kunkel, Heiko Bozem, Peter Hoor, Thomas Klimach, Frank Helleis, Julia Burkart, W. Richard Leaitch, Amir A. Aliabadi, Jonathan P. D. Abbatt, Andreas B. Herber, and Stephan Borrmann
Atmos. Chem. Phys., 21, 6509–6539, https://doi.org/10.5194/acp-21-6509-2021, https://doi.org/10.5194/acp-21-6509-2021, 2021
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We present in situ observations of vertically resolved particle chemical composition in the summertime Arctic lower troposphere. Our analysis demonstrates the strong vertical contrast between particle properties within the boundary layer and aloft. Emissions from vegetation fires and anthropogenic sources in northern Canada, Europe, and East Asia influenced particle composition in the free troposphere. Organics detected in Arctic aerosol particles can partly be identified as dicarboxylic acids.
Sanna Saarikoski, Jarkko V. Niemi, Minna Aurela, Liisa Pirjola, Anu Kousa, Topi Rönkkö, and Hilkka Timonen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-231, https://doi.org/10.5194/acp-2021-231, 2021
Revised manuscript accepted for ACP
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This study presents the main sources of black carbon (BC) at two urban environments. The largest fraction of BC originated from biomass burning at the residential site (38 %) and from vehicular emissions (57 %) at the street canyon. Also, a significant fraction of BC was associated with urban background or long-range transport. The data are needed by modelers and authorities when assessing climate and air quality impact of BC as well as directing the emission legislation and mitigation actions.
Luis M. F. Barreira, Aku Helin, Minna Aurela, Kimmo Teinilä, Milla Friman, Leena Kangas, Jarkko V. Niemi, Harri Portin, Anu Kousa, Liisa Pirjola, Topi Rönkkö, Sanna Saarikoski, and Hilkka Timonen
Atmos. Chem. Phys., 21, 6297–6314, https://doi.org/10.5194/acp-21-6297-2021, https://doi.org/10.5194/acp-21-6297-2021, 2021
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We present results from the long-term measurements (5 years) of highly time-resolved atmospheric PM1 composition at an urban street canyon site. Overall, the results increased knowledge of the variability of PM1 concentration, composition, and sources in a traffic site and the implications for urban air quality. The investigation of pollution episodes showed that both local and long-range-transported pollutants can still cause elevated PM1 and PM2.5 concentrations in northern Europe.
Genevieve Rose Lorenzo, Paola Angela Bañaga, Maria Obiminda Cambaliza, Melliza Templonuevo Cruz, Mojtaba AzadiAghdam, Avelino Arellano, Grace Betito, Rachel Braun, Andrea F. Corral, Hossein Dadashazar, Eva-Lou Edwards, Edwin Eloranta, Robert Holz, Gabrielle Leung, Lin Ma, Alexander B. MacDonald, Jeffrey S. Reid, James Bernard Simpas, Connor Stahl, Shane Marie Visaga, and Armin Sorooshian
Atmos. Chem. Phys., 21, 6155–6173, https://doi.org/10.5194/acp-21-6155-2021, https://doi.org/10.5194/acp-21-6155-2021, 2021
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Firework emissions change the physicochemical and optical properties of water-soluble particles, which subsequently alters the background aerosol’s respirability, influence on surroundings, ability to uptake gases, and viability as cloud condensation nuclei (CCN). There was heavy aerosol loading due to fireworks in the boundary layer. The aerosol constituents were largely water-soluble and submicrometer in size due to both inorganic salts in firework materials and gas-to-particle conversion.
Magdalena Reizer, Giulia Calzolai, Katarzyna Maciejewska, José A. G. Orza, Luca Carraresi, Franco Lucarelli, and Katarzyna Juda-Rezler
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-253, https://doi.org/10.5194/acp-2021-253, 2021
Revised manuscript accepted for ACP
Short summary
Short summary
Elemental composition of atmospheric PM2.5 and PM2.5-10 was measured during wintertime with 1-hour resolution by the use of “streaker” sampler for the first time at Central European urban background site. A set of multivariate, wind- and trajectory-based receptor models identified main sources of ambient aerosol. Fine PM fraction was mainly comprised of regionally transported aged secondary sulfate from solid fuel combustion in residential sector, while coarse mode showed traffic-related origin.
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Short summary
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.
This work presented a new method of quantifying water-soluble elements in PM2.5 aqueous extracts...
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