Articles | Volume 15, issue 20
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.
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.
PM2.5 water-soluble elements in the southeastern United States: automated analytical method development, spatiotemporal distributions, source apportionment, and implications for heath studies
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
H. Guo
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
V. Verma
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
now at: Department of Civil and Environmental Engineering, University of Illinois Urbana-Champaign, Champaign, IL, USA
R. E. Peltier
School of Public Health and Health Sciences, University of Massachusetts, Amherst, MA, USA
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
Related authors
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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.
Linghan Zeng, Jack Dibb, Eric Scheuer, Joseph M. Katich, Joshua P. Schwarz, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Carsten Warneke, Anne E. Perring, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Richard H. Moore, Elizabeth B. Wiggins, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Lu Xu, and Rodney J. Weber
Atmos. Chem. Phys., 22, 8009–8036, https://doi.org/10.5194/acp-22-8009-2022, https://doi.org/10.5194/acp-22-8009-2022, 2022
Short summary
Short summary
Wildfires emit aerosol particles containing brown carbon material that affects visibility and global climate and is toxic. Brown carbon is poorly characterized due to measurement limitations, and its evolution in the atmosphere is not well known. We report on aircraft measurements of brown carbon from large wildfires in the western United States. We compare two methods for measuring brown carbon and study the evolution of brown carbon in the smoke as it moved away from the burning regions.
Varun Kumar, Stamatios Giannoukos, Sophie L. Haslett, Yandong Tong, Atinderpal Singh, Amelie Bertrand, Chuan Ping Lee, Dongyu S. Wang, Deepika Bhattu, Giulia Stefenelli, Jay S. Dave, Joseph V. Puthussery, Lu Qi, Pawan Vats, Pragati Rai, Roberto Casotto, Rangu Satish, Suneeti Mishra, Veronika Pospisilova, Claudia Mohr, David M. Bell, Dilip Ganguly, Vishal Verma, Neeraj Rastogi, Urs Baltensperger, Sachchida N. Tripathi, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 22, 7739–7761, https://doi.org/10.5194/acp-22-7739-2022, https://doi.org/10.5194/acp-22-7739-2022, 2022
Short summary
Short summary
Here we present source apportionment results from the first field deployment in Delhi of an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF). The EESI-TOF is a recently developed instrument capable of providing uniquely detailed online chemical characterization of organic aerosol (OA), in particular the secondary OA (SOA) fraction. Here, we are able to apportion not only primary OA but also SOA to specific sources, which is performed for the first time in Delhi.
Sudheer Salana, Yixiang Wang, Joseph V. Puthussery, and Vishal Verma
Atmos. Meas. Tech., 14, 7579–7593, https://doi.org/10.5194/amt-14-7579-2021, https://doi.org/10.5194/amt-14-7579-2021, 2021
Short summary
Short summary
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 cell-based OP measurements. Here, we developed a semi-automated instrument, the first of its kind, 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 ambient PM.
Haoran Yu, Joseph Varghese Puthussery, Yixiang Wang, and Vishal Verma
Atmos. Chem. Phys., 21, 16363–16386, https://doi.org/10.5194/acp-21-16363-2021, https://doi.org/10.5194/acp-21-16363-2021, 2021
Short summary
Short summary
We assessed the oxidative potential (OP) of ambient PM2.5 collected from many sites in the US Midwest through multiple acellular endpoints. Compared to homogeneously distributed PM2.5, OP showed higher spatiotemporal variation. Poor correlations for the regression between mass and OP indicated a limited role of mass in determining the OP. Moreover, weak correlations among different OP endpoints justify the need for using multiple assays to determine oxidative levels of particles.
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, Siyuan Wang, 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., 21, 15023–15063, https://doi.org/10.5194/acp-21-15023-2021, https://doi.org/10.5194/acp-21-15023-2021, 2021
Short summary
Short summary
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 a 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.
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., 14, 6357–6378, https://doi.org/10.5194/amt-14-6357-2021, https://doi.org/10.5194/amt-14-6357-2021, 2021
Short summary
Short summary
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.
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
Short summary
Short summary
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.
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
Short summary
Short summary
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
Short summary
Short summary
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.
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
Overprediction of fine-particle ammonium-sulfate molar ratios (R) by thermodynamic models is suggested as evidence for organic aerosol limiting the condensation of ammonia onto particles, with significant impacts on aerosol chemistry. We find that the effects of small amounts of salt and dust, combined with measurement artifacts, explain the discrepancy in R. These results are highly insensitive to mixing state. This means that aerosol predictions are much more robust than thought before.
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
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.
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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)
Chemical properties and single-particle mixing state of soot aerosol in Houston during the TRACER campaign
Measurement report: Evaluation of the TOF-ACSM-CV for PM1.0 and PM2.5 measurements during the RITA-2021 field campaign
Sea salt reactivity over the northwest Atlantic: an in-depth look using the airborne ACTIVATE dataset
Measurement report: Atmospheric ice nuclei in the Changbai Mountains (2623 m a.s.l.) in northeastern Asia
Morphological and optical properties of carbonaceous aerosol particles from ship emissions and biomass burning during a summer cruise measurement in the South China Sea
Tropical tropospheric aerosol sources and chemical composition observed at high altitude in the Bolivian Andes
Chemical composition, sources and formation mechanism of urban PM2.5 in Southwest China: a case study at the beginning of 2023
Chemical characterization of atmospheric aerosols at a high-altitude mountain site: a study of source apportionment
Composition and sources of carbonaceous aerosol in the European Arctic at Zeppelin Observatory, Svalbard (2017 to 2020)
Variation in chemical composition and volatility of oxygenated organic aerosol in different rural, urban, and mountain environments
Elucidating the mechanisms of atmospheric new particle formation in the highly polluted Po Valley, Italy
Roles of marine biota in the formation of atmospheric bioaerosols, cloud condensation nuclei, and ice-nucleating particles over the North Pacific Ocean, Bering Sea, and Arctic Ocean
Evolution of nucleophilic high molecular-weight organic compounds in ambient aerosols: a case study
Fractional solubility of iron in mineral dust aerosols over coastal Namibia: a link to marine biogenic emissions?
Real-world observations of reduced nitrogen and ultrafine particles in commercial cooking organic aerosol emissions
Source apportionment of PM2.5 in Montréal, Canada, and health risk assessment for potentially toxic elements
Physicochemical and temporal characteristics of individual atmospheric aerosol particles in urban Seoul during KORUS-AQ campaign: insights from single-particle analysis
Mass spectrometric analysis of unprecedented high levels of carbonaceous aerosol particles long-range transported from wildfires in the Siberian Arctic
Short-term source apportionment of fine particulate matter with time-dependent profiles using SoFi Pro: exploring the reliability of rolling positive matrix factorization (PMF) applied to bihourly molecular and elemental tracer data
Particulate-bound alkyl nitrate pollution and formation mechanisms in Beijing, China
Measurement report: Characteristics of nitrogen-containing organics in PM2.5 in Urumqi, northwest China: differential impacts of combustion of fresh and old-age biomass materials
Characterization of water-soluble brown carbon chromophores from wildfire plumes in the western USA using size-exclusion chromatography
Marine carbohydrates in Arctic aerosol particles and fog – diversity of oceanic sources and atmospheric transformations
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying preexisting particles – Part 1: Observational data analysis
Measurement report: Brown carbon aerosol in polluted urban air of the North China Plain – day–night differences in the chromophores and optical properties
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
Bayesian Inference-Based Estimation of Hourly Primary and Secondary Organic Carbon at Suburban Hong Kong: Multi-temporal Scale Variations and Evolution Characteristics during PM2.5 episodes
Simultaneous organic aerosol source apportionment at two Antarctic sites reveals large-scale and eco-region specific components
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
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
Ryan N. Farley, James E. Lee, Laura-Hélèna Rivellini, Alex K. Y. Lee, Rachael Dal Porto, Christopher D. Cappa, Kyle Gorkowski, Abu Sayeed Md Shawon, Katherine B. Benedict, Allison C. Aiken, Manvendra K. Dubey, and Qi Zhang
Atmos. Chem. Phys., 24, 3953–3971, https://doi.org/10.5194/acp-24-3953-2024, https://doi.org/10.5194/acp-24-3953-2024, 2024
Short summary
Short summary
The black carbon aerosol composition and mixing state were characterized using a soot particle aerosol mass spectrometer. Single-particle measurements revealed the major role of atmospheric processing in modulating the black carbon mixing state. A significant fraction of soot particles were internally mixed with oxidized organic aerosol and sulfate, with implications for activation as cloud nuclei.
Xinya Liu, Bas Henzing, Arjan Hensen, Jan Mulder, Peng Yao, Danielle van Dinther, Jerry van Bronckhorst, Rujin Huang, and Ulrike Dusek
Atmos. Chem. Phys., 24, 3405–3420, https://doi.org/10.5194/acp-24-3405-2024, https://doi.org/10.5194/acp-24-3405-2024, 2024
Short summary
Short summary
We evaluated the time-of-flight aerosol chemical speciation monitor (TOF-ACSM) following the implementation of the PM2.5 aerodynamic lens and a capture vaporizer (CV). The results showed that it significantly improved the accuracy and precision of ACSM in the field observations. The paper elucidates the measurement outcomes of various instruments and provides an analysis of their biases. This comprehensive evaluation is expected to benefit the ACSM community and other aerosol field measurements.
Eva-Lou Edwards, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Claire E. Robinson, Michael A. Shook, Edward L. Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 24, 3349–3378, https://doi.org/10.5194/acp-24-3349-2024, https://doi.org/10.5194/acp-24-3349-2024, 2024
Short summary
Short summary
We investigate Cl− depletion in sea salt particles over the northwest Atlantic from December 2021 to June 2022 using an airborne dataset. Losses of Cl− are greatest in May and least in December–February and March. Inorganic acidic species can account for all depletion observed for December–February, March, and June near Bermuda but none in May. Quantifying Cl− depletion as a percentage captures seasonal trends in depletion but fails to convey the effects it may have on atmospheric oxidation.
Yue Sun, Yujiao Zhu, Yanbin Qi, Lanxiadi Chen, Jiangshan Mu, Ye Shan, Yu Yang, Yanqiu Nie, Ping Liu, Can Cui, Ji Zhang, Mingxuan Liu, Lingli Zhang, Yufei Wang, Xinfeng Wang, Mingjin Tang, Wenxing Wang, and Likun Xue
Atmos. Chem. Phys., 24, 3241–3256, https://doi.org/10.5194/acp-24-3241-2024, https://doi.org/10.5194/acp-24-3241-2024, 2024
Short summary
Short summary
Field observations were conducted at the summit of Changbai Mountain in northeast Asia. The cumulative number concentration of ice-nucleating particles (INPs) varied from 1.6 × 10−3 to 78.3 L−1 over the temperature range of −5.5 to −29.0 ℃. Biological INPs (bio-INPs) accounted for the majority of INPs, and the proportion exceeded 90% above −13.0 ℃. Planetary boundary layer height, valley breezes, and long-distance transport of air mass influence the abundance of bio-INPs.
Cuizhi Sun, Yongyun Zhang, Baoling Liang, Min Gao, Xi Sun, Fei Li, Xue Ni, Qibin Sun, Hengjia Ou, Dexian Chen, Shengzhen Zhou, and Jun Zhao
Atmos. Chem. Phys., 24, 3043–3063, https://doi.org/10.5194/acp-24-3043-2024, https://doi.org/10.5194/acp-24-3043-2024, 2024
Short summary
Short summary
In a May–June 2021 expedition in the South China Sea, we analyzed black and brown carbon in marine aerosols, key to light absorption and climate impact. Using advanced in situ and microscope techniques, we observed particle size, structure, and tar balls mixed with various elements. Results showed biomass burning and fossil fuels majorly influence light absorption, especially during significant burning events. This research aids the understanding of carbonaceous aerosols' role in marine climate.
C. Isabel Moreno, Radovan Krejci, Jean-Luc Jaffrezo, Gaëlle Uzu, Andrés Alastuey, Marcos F. Andrade, Valeria Mardóñez, Alkuin Maximilian Koenig, Diego Aliaga, Claudia Mohr, Laura Ticona, Fernando Velarde, Luis Blacutt, Ricardo Forno, David N. Whiteman, Alfred Wiedensohler, Patrick Ginot, and Paolo Laj
Atmos. Chem. Phys., 24, 2837–2860, https://doi.org/10.5194/acp-24-2837-2024, https://doi.org/10.5194/acp-24-2837-2024, 2024
Short summary
Short summary
Aerosol chemical composition (ions, sugars, carbonaceous matter) from 2011 to 2020 was studied at Mt. Chacaltaya (5380 m a.s.l., Bolivian Andes). Minimum concentrations occur in the rainy season with maxima in the dry and transition seasons. The origins of the aerosol are located in a radius of hundreds of kilometers: nearby urban and rural areas, natural biogenic emissions, vegetation burning from Amazonia and Chaco, Pacific Ocean emissions, soil dust, and Peruvian volcanism.
Junke Zhang, Yunfei Su, Chunying Chen, Wenkai Guo, Qinwen Tan, Miao Feng, Danlin Song, Tao Jiang, Qiang Chen, Yuan Li, Wei Li, Yizhi Wang, Xiaojuan Huang, Lin Han, Wanqing Wu, and Gehui Wang
Atmos. Chem. Phys., 24, 2803–2820, https://doi.org/10.5194/acp-24-2803-2024, https://doi.org/10.5194/acp-24-2803-2024, 2024
Short summary
Short summary
Typical haze events in Chengdu at the beginning of 2023 were investigated with bulk-chemical and single-particle analyses along with numerical model simulations. By integrating the obtained chemical composition, source, mixing state and numerical simulation results, we infer that Haze-1 was mainly caused by pollutants related to fossil fuel combustion, especially local mobile sources, while Haze-2 was triggered by the secondary pollutants, which mainly came from regional transmission.
Elena Barbaro, Matteo Feltracco, Fabrizio De Blasi, Clara Turetta, Marta Radaelli, Warren Cairns, Giulio Cozzi, Giovanna Mazzi, Marco Casula, Jacopo Gabrieli, Carlo Barbante, and Andrea Gambaro
Atmos. Chem. Phys., 24, 2821–2835, https://doi.org/10.5194/acp-24-2821-2024, https://doi.org/10.5194/acp-24-2821-2024, 2024
Short summary
Short summary
The study analyzed a year of atmospheric aerosol composition at Col Margherita in the Italian Alps. Over 100 chemical markers were identified, including major ions, organic compounds, and trace elements. It revealed sources of aerosol, highlighted impacts of Saharan dust events, and showed anthropogenic pollution's influence despite the site's remoteness. Enrichment factors emphasized non-natural sources of trace elements. Source apportionment identified four key factors affecting the area.
Karl Espen Yttri, Are Bäcklund, Franz Conen, Sabine Eckhardt, Nikolaos Evangeliou, Markus Fiebig, Anne Kasper-Giebl, Avram Gold, Hans Gundersen, Cathrine Lund Myhre, Stephen Matthew Platt, David Simpson, Jason D. Surratt, Sönke Szidat, Martin Rauber, Kjetil Tørseth, Martin Album Ytre-Eide, Zhenfa Zhang, and Wenche Aas
Atmos. Chem. Phys., 24, 2731–2758, https://doi.org/10.5194/acp-24-2731-2024, https://doi.org/10.5194/acp-24-2731-2024, 2024
Short summary
Short summary
We discuss carbonaceous aerosol (CA) observed at the high Arctic Zeppelin Observatory (2017 to 2020). We find that organic aerosol is a significant fraction of the Arctic aerosol, though less than sea salt aerosol and mineral dust, as well as non-sea-salt sulfate, originating mainly from anthropogenic sources in winter and from natural sources in summer, emphasizing the importance of wildfires for biogenic secondary organic aerosol and primary biological aerosol particles observed in the Arctic.
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr
Atmos. Chem. Phys., 24, 2607–2624, https://doi.org/10.5194/acp-24-2607-2024, https://doi.org/10.5194/acp-24-2607-2024, 2024
Short summary
Short summary
We present distinct molecular composition and volatility of oxygenated organic aerosol particles in different rural, urban, and mountain environments. We do a comprehensive investigation of the relationship between the chemical composition and volatility of oxygenated organic aerosol particles across different systems and environments. This study provides implications for volatility descriptions of oxygenated organic aerosol particles in different model frameworks.
Jing Cai, Juha Sulo, Yifang Gu, Sebastian Holm, Runlong Cai, Steven Thomas, Almuth Neuberger, Fredrik Mattsson, Marco Paglione, Stefano Decesari, Matteo Rinaldi, Rujing Yin, Diego Aliaga, Wei Huang, Yuanyuan Li, Yvette Gramlich, Giancarlo Ciarelli, Lauriane Quéléver, Nina Sarnela, Katrianne Lehtipalo, Nora Zannoni, Cheng Wu, Wei Nie, Juha Kangasluoma, Claudia Mohr, Markku Kulmala, Qiaozhi Zha, Dominik Stolzenburg, and Federico Bianchi
Atmos. Chem. Phys., 24, 2423–2441, https://doi.org/10.5194/acp-24-2423-2024, https://doi.org/10.5194/acp-24-2423-2024, 2024
Short summary
Short summary
By combining field measurements, simulations and recent chamber experiments, we investigate new particle formation (NPF) and growth in the Po Valley, where both haze and frequent NPF occur. Our results show that sulfuric acid, ammonia and amines are the dominant NPF precursors there. A high NPF rate and a lower condensation sink lead to a greater survival probability for newly formed particles, highlighting the importance of gas-to-particle conversion for aerosol concentrations.
Kaori Kawana, Fumikazu Taketani, Kazuhiko Matsumoto, Yutaka Tobo, Yoko Iwamoto, Takuma Miyakawa, Akinori Ito, and Yugo Kanaya
Atmos. Chem. Phys., 24, 1777–1799, https://doi.org/10.5194/acp-24-1777-2024, https://doi.org/10.5194/acp-24-1777-2024, 2024
Short summary
Short summary
Based on comprehensive shipborne observations, we found strong links between sea-surface biological materials and the formation of atmospheric fluorescent bioaerosols, cloud condensation nuclei, and ice-nucleating particles over the Arctic Ocean and Bering Sea during autumn 2019. Taking the wind-speed effect into account, we propose equations to approximate the links for this cruise, which can be used as a guide for modeling as well as for systematic comparisons with other observations.
Chen He, Hanxiong Che, Zier Bao, Yiliang Liu, Qing Li, Miao Hu, Jiawei Zhou, Shumin Zhang, Xiaojiang Yao, Quan Shi, Chunmao Chen, Yan Han, Lingshuo Meng, Xin Long, Fumo Yang, and Yang Chen
Atmos. Chem. Phys., 24, 1627–1639, https://doi.org/10.5194/acp-24-1627-2024, https://doi.org/10.5194/acp-24-1627-2024, 2024
Short summary
Short summary
We examined the daily evolution of high molecular-weight organic compounds with a molecular weight of up to 1000 Da in order to comprehend their behaviors in the atmosphere under actual conditions. These compounds were proven to undergo multi-generation oxidation, carboxylation, and nitrification via both day- and nighttime chemistry.
Karine Desboeufs, Paola Formenti, Raquel Torres-Sánchez, Kerstin Schepanski, Jean-Pierre Chaboureau, Hendrik Andersen, Jan Cermak, Stefanie Feuerstein, Benoit Laurent, Danitza Klopper, Andreas Namwoonde, Mathieu Cazaunau, Servanne Chevaillier, Anaïs Feron, Cécile Mirande-Bret, Sylvain Triquet, and Stuart J. Piketh
Atmos. Chem. Phys., 24, 1525–1541, https://doi.org/10.5194/acp-24-1525-2024, https://doi.org/10.5194/acp-24-1525-2024, 2024
Short summary
Short summary
This study investigates the fractional solubility of iron (Fe) in dust particles along the coast of Namibia, a critical region for the atmospheric Fe supply of the South Atlantic Ocean. Our results suggest a possible two-way interplay whereby marine biogenic emissions from the coastal marine ecosystems into the atmosphere would increase the solubility of Fe-bearing dust by photo-reduction processes. The subsequent deposition of soluble Fe could act to further enhance marine biogenic emissions.
Sunhye Kim, Jo Machesky, Drew R. Gentner, and Albert A. Presto
Atmos. Chem. Phys., 24, 1281–1298, https://doi.org/10.5194/acp-24-1281-2024, https://doi.org/10.5194/acp-24-1281-2024, 2024
Short summary
Short summary
Cooking emissions are often an overlooked source of air pollution. We used a mobile lab to measure the characteristics of particles emitted from cooking sites in two cities. Our findings showed that cooking releases a substantial number of fine particles. While most emissions were similar, a bakery site showed distinctive chemical compositions with higher nitrogen compound levels. Thus, understanding the particle emissions from different cooking activities is crucial.
Nansi Fakhri, Robin Stevens, Arnold Downey, Konstantina Oikonomou, Jean Sciare, Charbel Afif, and Patrick L. Hayes
Atmos. Chem. Phys., 24, 1193–1212, https://doi.org/10.5194/acp-24-1193-2024, https://doi.org/10.5194/acp-24-1193-2024, 2024
Short summary
Short summary
We investigated the chemical composition of atmospheric fine particles, their emission sources, and the potential human health risk associated with trace elements in particles for an urban site in Montréal over a 3-month period (August–November). This study represents the first time that such extensive composition measurements were included in an urban source apportionment study in Canada, and it provides greater resolution of fine-particle sources than has been previously achieved in Canada.
Hanjin Yoo, Li Wu, Hong Geng, and Chul-Un Ro
Atmos. Chem. Phys., 24, 853–867, https://doi.org/10.5194/acp-24-853-2024, https://doi.org/10.5194/acp-24-853-2024, 2024
Short summary
Short summary
We conducted an investigation of atmospheric aerosols collected in Seoul, South Korea, during the KORUS-AQ campaign on a single-particle basis. We were able to identify their sources, the atmospheric fate, and the impacts of local emissions and long-range transport on aerosol composition. Additionally, we traced potential sources of non-exhaust heavy-metal particles. This comprehensive analysis provides valuable insights into the complex dynamics of urban aerosols.
Eric Schneider, Hendryk Czech, Olga Popovicheva, Marina Chichaeva, Vasily Kobelev, Nikolay Kasimov, Tatiana Minkina, Christopher Paul Rüger, and Ralf Zimmermann
Atmos. Chem. Phys., 24, 553–576, https://doi.org/10.5194/acp-24-553-2024, https://doi.org/10.5194/acp-24-553-2024, 2024
Short summary
Short summary
This study provides insights into the complex chemical composition of long-range-transported wildfire plumes from Yakutia, which underwent different levels of atmospheric processing. With complementary mass spectrometric techniques, we improve our understanding of the chemical processes and atmospheric fate of wildfire plumes. Unprecedented high levels of carbonaceous aerosols crossed the polar circle with implications for the Arctic ecosystem and consequently climate.
Qiongqiong Wang, Shuhui Zhu, Shan Wang, Cheng Huang, Yusen Duan, and Jian Zhen Yu
Atmos. Chem. Phys., 24, 475–486, https://doi.org/10.5194/acp-24-475-2024, https://doi.org/10.5194/acp-24-475-2024, 2024
Short summary
Short summary
We investigated short-term source apportionment of PM2.5 utilizing rolling positive matrix factorization (PMF) and online PM chemical speciation data, which included source-specific organic tracers collected over a period of 37 d during the winter of 2019–2020 in suburban Shanghai, China. The findings highlight that by imposing constraints on the primary source profiles, short-term PMF analysis successfully replicated both the individual primary sources and the total secondary sources.
Jiyuan Yang, Guoyang Lei, Jinfeng Zhu, Yutong Wu, Chang Liu, Kai Hu, Junsong Bao, Zitong Zhang, Weili Lin, and Jun Jin
Atmos. Chem. Phys., 24, 123–136, https://doi.org/10.5194/acp-24-123-2024, https://doi.org/10.5194/acp-24-123-2024, 2024
Short summary
Short summary
The atmospheric pollution and formation mechanisms of particulate-bound alkyl nitrate in Beijing were studied. C9–C16 long-chain n-alkyl nitrates negatively correlated with O3 but positively correlated with PM2.5 and NO2, so they may not be produced during gas-phase homogeneous reactions in the photochemical process but form through reactions between alkanes and nitrates on PM surfaces. Particulate-bound n-alkyl nitrates strongly affect both haze pollution and atmospheric visibility.
Yi-Jia Ma, Yu Xu, Ting Yang, Hong-Wei Xiao, and Hua-Yun Xiao
EGUsphere, https://doi.org/10.5194/egusphere-2023-2514, https://doi.org/10.5194/egusphere-2023-2514, 2024
Short summary
Short summary
This study provides the field evidence on the differential impacts of combustion of fresh and old-age biomass materials on aerosol NOCs, bridging the linkages between the observations and previous laboratory studies showing the formation mechanisms of NOCs.
Lisa Azzarello, Rebecca A. Washenfelder, Michael A. Robinson, Alessandro Franchin, Caroline C. Womack, Christopher D. Holmes, Steven S. Brown, Ann Middlebrook, Tim Newberger, Colm Sweeney, and Cora J. Young
Atmos. Chem. Phys., 23, 15643–15654, https://doi.org/10.5194/acp-23-15643-2023, https://doi.org/10.5194/acp-23-15643-2023, 2023
Short summary
Short summary
We present a molecular size-resolved offline analysis of water-soluble brown carbon collected on an aircraft during FIREX-AQ. The smoke plumes were aged 0 to 5 h, where absorption was dominated by small molecular weight molecules, brown carbon absorption downwind did not consistently decrease, and the measurements differed from online absorption measurements of the same samples. We show how differences between online and offline absorption could be related to different measurement conditions.
Sebastian Zeppenfeld, Manuela van Pinxteren, Markus Hartmann, Moritz Zeising, Astrid Bracher, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 15561–15587, https://doi.org/10.5194/acp-23-15561-2023, https://doi.org/10.5194/acp-23-15561-2023, 2023
Short summary
Short summary
Marine carbohydrates are produced in the surface of the ocean, enter the atmophere as part of sea spray aerosol particles, and potentially contribute to the formation of fog and clouds. Here, we present the results of a sea–air transfer study of marine carbohydrates conducted in the high Arctic. Besides a chemo-selective transfer, we observed a quick atmospheric aging of carbohydrates, possibly as a result of both biotic and abiotic processes.
Xing Wei, Yanjie Shen, Xiao-Ying Yu, Yang Gao, Huiwang Gao, Ming Chu, Yujiao Zhu, and Xiaohong Yao
Atmos. Chem. Phys., 23, 15325–15350, https://doi.org/10.5194/acp-23-15325-2023, https://doi.org/10.5194/acp-23-15325-2023, 2023
Short summary
Short summary
We investigate the contribution of grown new particles to Nccn at a rural mountain site in the North China Plain. The total particle number concentrations (Ncn) observed on 8 new particle formation (NPF) days were higher compared to non-NPF days. The Nccn at 0.2 % supersaturation (SS) and 0.4 % SS on the NPF days was significantly lower than on non-NPF days. Only one of eight NPF events had detectable net contributions to Nccn at 0.4 % SS and 1.0 % SS with increased κ values.
Yuquan Gong, Ru-Jin Huang, Lu Yang, Ting Wang, Wei Yuan, Wei Xu, Wenjuan Cao, Yang Wang, and Yongjie Li
Atmos. Chem. Phys., 23, 15197–15207, https://doi.org/10.5194/acp-23-15197-2023, https://doi.org/10.5194/acp-23-15197-2023, 2023
Short summary
Short summary
This study reveals the large day–night differences in brown carbon (BrC) chromophore composition, which was not known previously. The results provide insights into the effects of atmospheric processes and emissions on BrC composition.
Ryan N. Farley, Sonya Collier, Christopher D. Cappa, Leah R. Williams, Timothy B. Onasch, Lynn M. Russell, Hwajin Kim, and Qi Zhang
Atmos. Chem. Phys., 23, 15039–15056, https://doi.org/10.5194/acp-23-15039-2023, https://doi.org/10.5194/acp-23-15039-2023, 2023
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
In this study, 130 OS species were quantified in ambient fine particulate matter (PM2.5) collected in urban and suburban Shanghai (East China) in the summer of 2021. The daytime OS formation was concretized based on the interactions among OSs, ultraviolet (UV), ozone (O3), and sulfate. Our finding provides field evidence for the influence of photochemical process and anthropogenic sulfate on OS formation and has important implications for the mitigation of organic particulate pollution.
Shan Wang, Kezheng Liao, Zijing Zhang, Yuk Ying Cheng, Qiongqiong Wang, Hanzhe Chen, and Jian Zhen Yu
EGUsphere, https://doi.org/10.5194/egusphere-2023-2286, https://doi.org/10.5194/egusphere-2023-2286, 2023
Short summary
Short summary
In this work, hourly primary and secondary organic carbon were estimated by a novel Bayesian inference approach in suburban Hong Kong. Their multi-temporal scale variations and evolution characteristics during PM2.5 episodes were examined. The methodology could serve as a guide for other locations with similar monitoring capabilities. The observation-based results are helpful for understanding the evolving nature of secondary organic aerosols and refining the accuracy of model simulations.
Marco Paglione, David C. S. Beddows, Anna Jones, Thomas Lachlan-Cope, Matteo Rinaldi, Stefano Decesari, Francesco Manarini, Mara Russo, Karam Mansour, Roy M. Harrison, Andrea Mazzanti, Emilio Tagliavini, and Manuel Dall'Osto
EGUsphere, https://doi.org/10.5194/egusphere-2023-2275, https://doi.org/10.5194/egusphere-2023-2275, 2023
Short summary
Short summary
Applying factor analysis techniques to H-NMR spectra, we present the Organic Aerosol (OA) source apportionment of PM1 samples collected in parallel at two peri-Antarctic stations, namely Signy and Halley, important to investigate aerosol-climate interactions in an unperturbed atmosphere. Our results show remarkable differences between pelagic (open ocean) and sympagic (sea-ice influenced) air masses and indicate that various sources and processes are controlling Antarctic aerosols.
Miao Zhong, Jianzhong Xu, Huiqin Wang, Li Gao, Haixia Zhu, Lixiang Zhai, Xinghua Zhang, and Wenhui Zhao
Atmos. Chem. Phys., 23, 12609–12630, https://doi.org/10.5194/acp-23-12609-2023, https://doi.org/10.5194/acp-23-12609-2023, 2023
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
We examine iron in atmospheric fine aerosol particles collected over the Indian Ocean during shipborne observations in November 2018. Transmission electron microscopy analysis with water dialysis shows that various types of iron (fly ash, iron oxide, and mineral dust) co-exist with ammonium sulfate and that their solubility differs depending on the iron type. Using PM2.5 bulk samples and global model simulations, we elucidate their origins, aging, and implications for present iron simulations.
Farhan R. Nursanto, Roy Meinen, Rupert Holzinger, Maarten C. Krol, Xinya Liu, Ulrike Dusek, Bas Henzing, and Juliane L. Fry
Atmos. Chem. Phys., 23, 10015–10034, https://doi.org/10.5194/acp-23-10015-2023, https://doi.org/10.5194/acp-23-10015-2023, 2023
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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.
Cited articles
Adachi, K. and Tainosho, Y.: Characterization of heavy metal particles embedded in tire dust, Environ. Int., 30, 1009–1017, https://doi.org/10.1016/j.envint.2004.04.004, 2004.
Akhtar, U. S., McWhinney, R. D., Rastogi, N., Abbatt, J. P. D., Evans, G. J., and Scott, J. A.: Cytotoxic and proinflammatory effects of ambient and source-related particulate matter (PM) in relation to the production of reactive oxygen species (ROS) and cytokine adsorption by particles, Inhalation Toxic., 22, 37–47, https://doi.org/10.3109/08958378.2010.518377, 2010.
Atkinson, R. W., Fuller, G. W., Anderson, H. R., Harrison, R. M., and Armstrong, B.: Urban ambient particle metrics and health: a time-series analysis, Epidemiology, 21, 501–511, https://doi.org/10.1097/EDE.0b013e3181debc88, 2010.
Bae, M.-S., Schauer, J. J., and Turner, J. R.: Estimation of the monthly average ratios of organic mass to organic carbon for fine particulate matter at an urban site, Aerosol Sci. Technol., 40, 1123–1139, https://doi.org/10.1080/02786820601004085, 2006.
Bates, J. T., Weber, R. J., Abrams, J., Verma, V., Fang, T., Klein, M., Strickland, M. J., Sarnat, S. E., Chang, H. H., Mulholland, J. A., Tolbert, P. E., and Russell, A. G.: Reactive Oxygen Species Generation Linked to Soures of Atmospheric Particulate Matter and Cardiorespiratory Effects, Environ. Sci. Technol., accepted, https://doi.org/10.1021/acs.est.5b02967, 2015.
Bell, M. L., Dominici, F., Ebisu, K., Zeger, S. L., and Samet, J. M.: Spatial and temporal variation in PM(2.5) chemical composition in the United States for health effects studies, Environ. Health Perspect., 115, 989–995, https://doi.org/10.1289/ehp.9621, 2007.
Birmili, W., Allen, A. G., Bary, F., and Harrison, R. M.: Trace Metal Concentrations and Water Solubility in Size-Fractionated Atmospheric Particles and Influence of Road Traffic, Environ. Sci. Techno., 40, 1144–1153, https://doi.org/10.1021/es0486925, 2006.
Brunekreef, B., Janssen, N. A., de Hartog, J., Harssema, H., Knape, M., and van Vliet, P.: Air pollution from truck traffic and lung function in children living near motorways, Epidemiology, 8, 298–303, https://doi.org/10.1097/00001648-199705000-00012, 1997.
Burchiel, S. W., Lauer, F. T., Dunaway, S. L., Zawadzki, J., McDonald, J. D., and Reed, M. D.: Hardwood smoke alters murine splenic T cell responses to mitogens following a 6-month whole body inhalation exposure, Toxicol. Appl. Pharmacol., 202, 229–236, https://doi.org/10.1016/j.taap.2004.06.024, 2005.
Burnett, R. T., Brook, J., Dann, T., Delocla, C., Philips, O., Cakmak, S., Vincent, R., Goldberg, M. S., and Krewski, D.: Association between particulate- and gas-phase components of urban air pollution and daily mortality in eight Canadian cities, Inhal. Toxicol., 12, 15–39, https://doi.org/10.1080/08958370050164851, 2000.
Chang-Graham, A. L., Profeta, L. T. M., Johnson, T. J., Yokelson, R. J., Laskin, A., and Laskin, J.: Case study of water-soluble metal containing organic constituents of biomass burning aerosol, Environ. Sci. Technol., 45, 1257–1263, https://doi.org/10.1021/es103010j, 2011.
Charrier, J. G. and Anastasio, C.: On dithiothreitol (DTT) as a measure of oxidative potential for ambient particles: evidence for the importance of soluble transition metals, Atmos. Chem. Phys., 12, 9321–9333, https://doi.org/10.5194/acp-12-9321-2012, 2012.
Cheung, K., Shafer, M. M., Schauer, J. J., and Sioutas, C.: Diurnal trends in oxidative potential of coarse particulate matter in the Los Angeles basin and their relation to sources and chemical composition, Environ. Sci. Technol., 46, 3779–3787, https://doi.org/10.1021/es204211v, 2012.
Cheung, K. L., Ntziachristos, L., Tzamkiozis, T., Schauer, J. J., Samaras, Z., Moore, K. F., and Sioutas, C.: Emissions of particulate trace elements, metals and organic species from gasoline, diesel, and biodiesel passenger vehicles and their relation to oxidative potential, Aerosol Sci. Technol., 44, 500–513, https://doi.org/10.1080/02786821003758294, 2010.
Chevion, M.: A site-specific mechanism for free radical induced biological damage: The essential role of redox-active transition metals, Free Radical Biol. Medicine, 5, 27–37, https://doi.org/10.1016/0891-5849(88)90059-7, 1988.
Cho, W.-S., Duffin, R., Poland, C. A., Duschl, A., Oostingh, G. J., MacNee, W., Bradley, M., Megson, I. L., and Donaldson, K.: Differential pro-inflammatory effects of metal oxide nanoparticles and their soluble ions in vitro and in vivo; zinc and copper nanoparticles, but not their ions, recruit eosinophils to the lungs, Nanotoxicology, 6, 22–35, https://doi.org/10.3109/17435390.2011.552810, 2011.
Darrow, L. A., Klein, M., Flanders, W. D., Waller, L. A., Correa, A., Marcus, M., Mulholland, J. A., Russell, A. G., and Tolbert, P. E.: Ambient air pollution and preterm birth: a time-series analysis, Epidemiology, 20, 689–698, https://doi.org/10.1097/EDE.0b013e3181a7128f, 2009.
Darrow, L. A., Klein, M., Strickland, M. J., Mulholland, J. A., and Tolbert, P. E.: Ambient air pollution and birth weight in full-term infants in Atlanta, 1994–2004, Environ. Health Perspect., 119, 731–737, https://doi.org/10.1289/ehp.1002785, 2011.
Dockery, D. W., Cunningham, J., Damokosh, A. I., Neas, L. M., Spengler, J. D., Koutrakis, P., Ware, J. H., Raizenne, M., and Speizer, F. E.: Health effects of acid aerosols on North American children: respiratory symptoms, Environ. Health Perspect., 104, 500–505, 1996.
Espinosa, A. J. F., Rodríguez, M. T., de la Rosa, F. J. B., and Sánchez, J. C. J.: A chemical speciation of trace metals for fine urban particles, Atmos. Environ., 36, 773–780, https://doi.org/10.1016/S1352-2310(01)00534-9, 2002.
Fang, T., Verma, V., Guo, H., King, L. E., Edgerton, E. S., and Weber, R. J.: A semi-automated system for quantifying the oxidative potential of ambient particles in aqueous extracts using the dithiothreitol (DTT) assay: results from the Southeastern Center for Air Pollution and Epidemiology (SCAPE), Atmos. Meas. Tech., 8, 471–482, https://doi.org/10.5194/amt-8-471-2015, 2015a.
Fang, T., Verma, V., Bates, J. T., Abrams, J., Klein, M., Strickland, M. J., Sarnat, S. E., Chang, H. H., Mulholland, J. A., Tolbert, P. E., Russell, A. G., and Weber, R. J.: Oxidative Potential of Ambient Water-Soluble PM2.5 Measured by Dithiothreitol (DTT) and Ascorbic Acid (AA) Assays in the Southeastern United States: Contrasts in Sources and Health Associations, Atmos. Chem. Phys., in preparation, 2015b.
Garg, B. D., Cadle, S. H., Mulawa, P. A., Groblicki, P. J., Laroo, C., and Parr, G. A.: Brake wear particulate matter emissions, Environ. Sci. Technol., 34, 4463–4469, https://doi.org/10.1021/es001108h, 2000.
Gasser, M., Riediker, M., Mueller, L., Perrenoud, A., Blank, F., Gehr, P., and Rothen-Rutishauser, B.: Toxic effects of brake wear particles on epithelial lung cells in vitro, Particle Fibre Toxicol., 6, 30, https://doi.org/10.1186/1743-8977-6-30, 2009.
Gietl, J. K., Lawrence, R., Thorpe, A. J., and Harrison, R. M.: Identification of brake wear particles and derivation of a quantitative tracer for brake dust at a major road, Atmos. Environ., 44, 141–146, https://doi.org/10.1016/j.atmosenv.2009.10.016, 2010.
Gwynn, R. C., Burnett, R. T., and Thurston, G. D.: A time-series analysis of acidic particulate matter and daily mortality and morbidity in the Buffalo, New York, region, Environ. Health Perspect., 108, 125–133, 2000.
Hansen, D. A., Edgerton, E. S., Hartsell, B. E., Jansen, J. J., Kandasamy, N., Hidy, G. M., and Blanchard, C. L.: The Southeastern aerosol research and characterization study: Part 1 – Overview, J. Air Waste Manag. Assoc., 53, 1460–1471, https://doi.org/10.1080/10473289.2003.10466318, 2003.
Harrison, R. M., Jones, A. M., Gietl, J., Yin, J., and Green, D. C.: Estimation of the contributions of brake dust, tire wear, and resuspension to nonexhaust traffic particles derived from atmospheric measurements, Environ. Sci. Technol., 46, 6523–6529, https://doi.org/10.1021/es300894r, 2012.
He, K., Yang, F., Ma, Y., Zhang, Q., Yao, X., Chan, C. K., Cadle, S., Chan, T., and Mulawa, P.: The characteristics of PM2.5 in Beijing, China, Atmos. Environ., 35, 4959–4970, https://doi.org/10.1016/S1352-2310(01)00301-6, 2001.
Heal, M. R., Hibbs, L. R., Agius, R. M., and Beverland, I. J.: Total and water-soluble trace metal content of urban background PM10, PM2.5 and black smoke in Edinburgh, UK, Atmos. Environ., 39, 1417–1430, https://doi.org/10.1016/j.atmosenv.2004.11.026, 2005.
Hidy, G. M., Blanchard, C. L., Baumann, K., Edgerton, E., Tanenbaum, S., Shaw, S., Knipping, E., Tombach, I., Jansen, J., and Walters, J.: Chemical climatology of the southeastern United States, 1999–2013, Atmos. Chem. Phys., 14, 11893–11914, https://doi.org/10.5194/acp-14-11893-2014, 2014.
Hopke, P. K., Lamb, R. E., and Natusch, D. F. S.: Multielemental characterization of urban roadway dust, Environ. Sci. Technol., 14, 164–172, https://doi.org/10.1021/es60162a006, 1980.
Huang, Y. C., Ghio, A. J., Stonehuerner, J., McGee, J., Carter, J. D., Grambow, S. C., and Devlin, R. B.: The role of soluble components in ambient fine particles-induced changes in human lungs and blood, Inhal. Toxicol., 15, 327–342, https://doi.org/10.1080/08958370304460, 2003.
Hueglin, C., Gehrig, R., Baltensperger, U., Gysel, M., Monn, C., and Vonmont, H.: Chemical characterisation of PM2.5, PM10 and coarse particles at urban, near-city and rural sites in Switzerland, Atmos. Environ., 39, 637–651, https://doi.org/10.1016/j.atmosenv.2004.10.027, 2005.
Kam, W., Ning, Z., Shafer, M. M., Schauer, J. J., and Sioutas, C.: Chemical characterization and redox potential of coarse and fine particulate matter (PM) in underground and ground-level rail systems of the Los Angeles metro, Environ. Sci. Technol., 45, 6769–6776, https://doi.org/10.1021/es201195e, 2011.
Kleinman, M. T., Sioutas, C., Froines, J. R., Fanning, E., Hamade, A., Mendez, L., Meacher, D., and Oldham, M.: Inhalation of concentrated ambient particulate matter near a heavily trafficked road stimulates antigen-induced airway responses in mice, Inhal. Toxicol., 19, 117–126, https://doi.org/10.1080/08958370701495345, 2007.
Kodavanti, U. P., Schladweiler, M. C., Ledbetter, A. D., McGee, J. K., Walsh, L., Gilmour, P. S., Highfill, J. W., Davies, D., Pinkerton, K. E., Richards, J. H., Crissman, K., Andrews, D., and Costa, D. L.: Consistent pulmonary and systemic responses from inhalation of fine concentrated ambient particles: roles of rat strains used and physicochemical properties, Environ. Health Perspect., 113, 1561–1568, https://doi.org/10.1289/ehp.7868, 2005.
Laden, F., Neas, L. M., Dockery, D. W., and Schwartz, J.: Association of fine particulate matter from different sources with daily mortality in six U.S. cities, Environ. Health Perspect., 108, 941–947, https://doi.org/10.2307/3435052, 2000.
Landreman, A. P., Shafer, M. M., Hemming, J. C., Hannigan, M. P., and Schauer, J. J.: A macrophage-based method for the assessment of the Reactive Oxygen Species (ROS) activity of atmospheric particulate matter (PM) and application to routine (daily-24 h) aerosol monitoring studies, Aerosol Sci. Technol., 42, 946–957, https://doi.org/10.1080/02786820802363819, 2008.
Li, Q. F., Wyatt, A., and Kamens, R. M.: Oxidant generation and toxicity enhancement of aged-diesel exhaust, Atmos. Environ., 43, 1037–1042, https://doi.org/10.1016/j.atmosenv.2008.11.018, 2009.
Li, R., Ning, Z., Majumdar, R., Cui, J., Takabe, W., Jen, N., Sioutas, C., and Hsiai, T.: Ultrafine particles from diesel vehicle emissions at different driving cycles induce differential vascular pro-inflammatory responses: Implication of chemical components and NF-kappaB signaling, Particle Fibre Toxicol., 7, 6, https://doi.org/10.1186/1743-8977-7-6, 2010.
Liochev, S. I. and Fridovich, I.: The Haber-Weiss cycle – 70 years later: an alternative view, Redox report: communications in free radical research, 7, 55–57, https://doi.org/10.1179/135100002125000190, 2002.
Lundstedt, S., White, P. A., Lemieux, C. L., Lynes, K. D., Lambert, I. B., Öberg, L., Haglund, P., and Tysklind, M.: Sources, fate, and toxic hazards of oxygenated polycyclic aromatic hydrocarbons (PAHs) at PAH- contaminated sites, AMBIO: A Journal of the Human Environment, 36, 475–485, https://doi.org/10.1579/0044-7447(2007)36[475:sfatho]2.0.co;2, 2007.
Maynard, D., Coull, B. A., Gryparis, A., and Schwartz, J.: Mortality risk associated with short-term exposure to traffic particles and sulfates, Environ. Health Perspect., 115, 751–755, https://doi.org/10.1289/ehp.9537, 2007.
Metzger, K. B., Tolbert, P. E., Klein, M., Peel, J. L., Flanders, W. D., Todd, K., Mulholland, J. A., Ryan, P. B., and Frumkin, H.: Ambient air pollution and cardiovascular emergency department visits, Epidemiology, 15, 46–56, https://doi.org/10.1097/01.EDE.0000101748.28283.97, 2004.
Minguillón, M. C., Cirach, M., Hoek, G., Brunekreef, B., Tsai, M., de Hoogh, K., Jedynska, A., Kooter, I. M., Nieuwenhuijsen, M., and Querol, X.: Spatial variability of trace elements and sources for improved exposure assessment in Barcelona, Atmos. Environ., 89, 268–281, https://doi.org/10.1016/j.atmosenv.2014.02.047, 2014.
Nel, A. E., Diaz-Sanchez, D., and Li, N.: The role of particulate pollutants in pulmonary inflammation and asthma: evidence for the involvement of organic chemicals and oxidative stress, Current Opin. Pulm. Med., 7, 20–26, https://doi.org/10.1097/00063198-200101000-00004, 2001.
Oakes, M., Ingall, E. D., Lai, B., Shafer, M. M., Hays, M. D., Liu, Z. G., Russell, A. G., and Weber, R. J.: Iron solubility related to particle sulfur content in source emission and ambient fine particles, Environ. Sci. Technol., 46, 6637–6644, https://doi.org/10.1021/es300701c, 2012.
Paatero, P. and Tapper, U.: Positive matrix factorization: A non-negative factor model with optimal utilization of error estimates of data values, Environmetrics, 5, 111–126, https://doi.org/10.1002/env.3170050203, 1994.
Peel, J. L., Tolbert, P. E., Klein, M., Metzger, K. B., Flanders, W. D., Todd, K., Mulholland, J. A., Ryan, P. B., and Frumkin, H.: Ambient air pollution and respiratory emergency department visits, Epidemiology, 16, 164–174, https://doi.org/10.1097/01.ede.0000152905.42113.db, 2005.
Polissar, A. V., Hopke, P. K., Paatero, P., Malm, W. C., and Sisler, J. F.: Atmospheric aerosol over Alaska: 2. Elemental composition and sources, J. Geophys. Res.-Atmos., 103, 19045–19057, https://doi.org/10.1029/98JD01212, 1998.
Pope, C. A., Burnett, R. T., Thun, M. J., Calle, E. E., Krewski, D., Ito, K., and Thurston, G. D.: Lung cancer, cardiopulmonary mortality, and long-term exposure to fine particulate air pollution, J. Am. Med. Assoc., 287, 1132–1141, https://doi.org/10.1001/jama.287.9.1132, 2002.
Pope, C. A., Burnett, R. T., Thurston, G. D., Thun, M. J., Calle, E. E., Krewski, D., and Godleski, J. J.: Cardiovascular mortality and long-term exposure to particulate air pollution: epidemiological evidence of general pathophysiological pathways of disease, Circulation, 109, 71–77, https://doi.org/10.1161/01.CIR.0000108927.80044.7F, 2004.
Raizenne, M., Neas, L. M., Damokosh, A. I., Dockery, D. W., Spengler, J. D., Koutrakis, P., Ware, J. H., and Speizer, F. E.: Health effects of acid aerosols on North American children: pulmonary function, Environ. Health Perspect., 104, 506–514, https://doi.org/10.2307/3432991, 1996.
Richard, A., Gianini, M. F. D., Mohr, C., Furger, M., Bukowiecki, N., Minguillón, M. C., Lienemann, P., Flechsig, U., Appel, K., DeCarlo, P. F., Heringa, M. F., Chirico, R., Baltensperger, U., and Prévôt, A. S. H.: Source apportionment of size and time resolved trace elements and organic aerosols from an urban courtyard site in Switzerland, Atmos. Chem. Phys., 11, 8945–8963, https://doi.org/10.5194/acp-11-8945-2011, 2011.
Riediker, M., Devlin, R., Griggs, T., Herbst, M., Bromberg, P., Williams, R., and Cascio, W.: Cardiovascular effects in patrol officers are associated with fine particulate matter from brake wear and engine emissions, Particle Fibre Toxicol., 1, 2, https://doi.org/10.1186/1743-8977-1-2, 2004.
Saffari, A., Daher, N., Shafer, M. M., Schauer, J. J., and Sioutas, C.: Global perspective on the oxidative potential of airborne particulate matter: a synthesis of research findings, Environ. Sci. Technol., 48, 7576–7583, https://doi.org/10.1021/es500937x, 2014.
Sarnat, J. A., Marmur, A., Klein, M., Kim, E., Russell, A. G., Sarnat, S. E., Mulholland, J. A., Hopke, P. K., and Tolbert, P. E.: Fine particle sources and cardiorespiratory morbidity: an application of chemical mass balance and factor analytical source-apportionment methods, Environ. Health Perspect., 116, 459–466, https://doi.org/10.1289/ehp.10873, 2008.
Sauvain, J.-J., Deslarzes, S., and Riediker, M.: Nanoparticle reactivity toward dithiothreitol, Nanotoxicology, 2, 121–129, https://doi.org/10.1080/17435390802245716, 2008.
Seagrave, J., McDonald, J. D., Gigliotti, A. P., Nikula, K. J., Seilkop, S. K., Gurevich, M., and Mauderly, J. L.: Mutagenicity and in vivo toxicity of combined particulate and semivolatile organic fractions of gasoline and diesel engine emissions, Toxicol. Sci., 70, 212–226, https://doi.org/10.1093/toxsci/70.2.212, 2002.
Seagrave, J., Gigliotti, A., McDonald, J. D., Seilkop, S. K., Whitney, K. A., Zielinska, B., and Mauderly, J. L.: Composition, toxicity, and mutagenicity of particulate and semivolatile emissions from heavy-duty compressed natural gas-powered vehicles, Toxicological Sci., 87, 232–241, https://doi.org/10.1093/toxsci/kfi230, 2005.
Shakya, K. M. and Peltier, R. E.: Non-sulfate sulfur in fine aerosols across the United States: Insight for organosulfate prevalence, Atmos. Environ., 100, 159–166, https://doi.org/10.1016/j.atmosenv.2014.10.058, 2015.
Shen, H. and Anastasio, C.: Formation of hydroxyl radical from San Joaquin Valley particles extracted in a cell-free surrogate lung fluid, Atmos. Chem. Phys., 11, 9671–9682, https://doi.org/10.5194/acp-11-9671-2011, 2011.
Shi, T., Schins, R. P., Knaapen, A. M., Kuhlbusch, T., Pitz, M., Heinrich, J., and Borm, P. J.: Hydroxyl radical generation by electron paramagnetic resonance as a new method to monitor ambient particulate matter composition, J. Environ. Monitor., 5, 550–556, https://doi.org/10.1039/B303928P, 2003.
Sternbeck, J., Sjödin, Å., and Andréasson, K.: Metal emissions from road traffic and the influence of resuspension – results from two tunnel studies, Atmos. Environ., 36, 4735–4744, https://doi.org/10.1016/S1352-2310(02)00561-7, 2002.
Stohs, S. J. and Bagchi, D.: Oxidative mechanisms in the toxicity of metal ions, Free Radical Bio. Med., 18, 321–336, https://doi.org/10.1016/0891-5849(94)00159-H, 1995.
Strak, M., Janssen, N. A., Godri, K. J., Gosens, I., Mudway, I. S., Cassee, F. R., Lebret, E., Kelly, F. J., Harrison, R. M., Brunekreef, B., Steenhof, M., and Hoek, G.: Respiratory health effects of airborne particulate matter: the role of particle size, composition, and oxidative potential-the RAPTES project, Environ. Health Perspect., 120, 1183–1189, https://doi.org/10.1289/ehp.1104389, 2012.
Sullivan, A. P., Peltier, R. E., Brock, C. A., de Gouw, J. A., Holloway, J. S., Warneke, C., Wollny, A. G., and Weber, R. J.: Airborne measurements of carbonaceous aerosol soluble in water over northeastern United States: Method development and an investigation into water-soluble organic carbon sources, J. Geophys. Res.-Atmos., 111, D23S46, https://doi.org/10.1029/2006JD007072, 2006.
Tolocka, M. P. and Turpin, B.: Contribution of organosulfur compounds to organic aerosol mass, Environ. Sci. Technol., 46, 7978–7983, https://doi.org/10.1021/es300651v, 2012.
Torre, C., Mattutino, G., Vasino, V., and Robino, C.: Brake linings: a source of non-GSR particles containing lead, barium, and antimony, J. Forensic Sci., 47, 494–504, 2002.
Turn, S. Q., Jenkins, B. M., Chow, J. C., Pritchett, L. C., Campbell, D., Cahill, T., and Whalen, S. A.: Elemental characterization of particulate matter emitted from biomass burning: Wind tunnel derived source profiles for herbaceous and wood fuels, J. Geophys. Res.-Atmos., 102, 3683–3699, https://doi.org/10.1029/96jd02979, 1997.
Valko, M., Morris, H., and Cronin, M. T.: Metals, toxicity and oxidative stress, Curr. Med. Chem., 12, 1161–1208, https://doi.org/10.2174/0929867053764635, 2005.
Verma, V., Shafer, M. M., Schauer, J. J., and Sioutas, C.: Contribution of transition metals in the reactive oxygen species activity of PM emissions from retrofitted heavy-duty vehicles, Atmos. Environ., 44, 5165–5173, https://doi.org/10.1016/j.atmosenv.2010.08.052, 2010.
Verma, V., Rico-Martinez, R., Kotra, N., King, L. E., Liu, J., Snell, T. W., and Weber, R. J.: Contribution of water-soluble and insoluble components and their hydrophobic/hydrophilic subfractions to the reactive oxygen species-generating ootential of fine ambient aerosols, Environ. Sci. Technol., 46, 11384–11392, https://doi.org/10.1021/es302484r, 2012.
Verma, V., Fang, T., Guo, H., King, L., Bates, J. T., Peltier, R. E., Edgerton, E., Russell, A. G., and Weber, R. J.: Reactive oxygen species associated with water-soluble PM2.5 in the southeastern United States: spatiotemporal trends and source apportionment, Atmos. Chem. Phys., 14, 12915–12930, https://doi.org/10.5194/acp-14-12915-2014, 2014.
Verma, V., Fang, T., Xu, L., Peltier, R. E., Russell, A. G., Ng, N. L., and Weber, R. J.: Organic aerosols associated with the generation of Reactive Oxygen Species (ROS) by water-soluble PM2.5, Environ. Sci. Technol., 49, 4646–4656, https://doi.org/10.1021/es505577w, 2015.
Wilson, J. G., Kingham, S., Pearce, J., and Sturman, A. P.: A review of intraurban variations in particulate air pollution: Implications for epidemiological research, Atmos. Environ., 39, 6444–6462, https://doi.org/10.1016/j.atmosenv.2005.07.030, 2005.
Zhang, X., Hecobian, A., Zheng, M., Frank, N. H., and Weber, R. J.: Biomass burning impact on PM2.5 over the southeastern US during 2007: integrating chemically speciated FRM filter measurements, MODIS fire counts and PMF analysis, Atmos. Chem. Phys., 10, 6839–6853, https://doi.org/10.5194/acp-10-6839-2010, 2010.
Zhang, Y., Schauer, J. J., Shafer, M. M., Hannigan, M. P., and Dutton, S. J.: Source apportionment of in vitro Reactive Oxygen Species bioassay activity from atmospheric particulate matter, Environ. Sci. Technol., 42, 7502–7509, https://doi.org/10.1021/es800126y, 2008.
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...
Altmetrics
Final-revised paper
Preprint