Articles | Volume 20, issue 6
https://doi.org/10.5194/acp-20-3793-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-3793-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
31 Mar 2020
Research article |
| 31 Mar 2020
| 31 Mar 2020
Summertime and wintertime atmospheric processes of secondary aerosol in Beijing
Jing Duan
State Key Laboratory of Loess and Quaternary Geology, Key
Laboratory of Aerosol Chemistry and Physics, Institute of Earth
Environment, Chinese Academy of Sciences, Xi'an 710061, China
CAS Center for Excellence in Quaternary Science and Global Change,
Chinese Academy of Sciences, Xi'an 710061, China
University of Chinese Academy of Sciences, Beijing 100049, China
Ru-Jin Huang
CORRESPONDING AUTHOR
State Key Laboratory of Loess and Quaternary Geology, Key
Laboratory of Aerosol Chemistry and Physics, Institute of Earth
Environment, Chinese Academy of Sciences, Xi'an 710061, China
CAS Center for Excellence in Quaternary Science and Global Change,
Chinese Academy of Sciences, Xi'an 710061, China
Yongjie Li
Department of Civil and Environmental Engineering, Faculty of Science
and Technology, University of Macau, Taipa, Macau 999078, China
State Key Joint Laboratory of Environmental Simulation and Pollution
Control, College of Environmental Sciences and Engineering, Peking
University, Beijing 100871, China
Yan Zheng
State Key Joint Laboratory of Environmental Simulation and Pollution
Control, College of Environmental Sciences and Engineering, Peking
University, Beijing 100871, China
Yang Chen
Chongqing Institute of Green and Intelligent Technology, Chinese
Academy of Sciences, Chongqing 400714, China
Chunshui Lin
State Key Laboratory of Loess and Quaternary Geology, Key
Laboratory of Aerosol Chemistry and Physics, Institute of Earth
Environment, Chinese Academy of Sciences, Xi'an 710061, China
CAS Center for Excellence in Quaternary Science and Global Change,
Chinese Academy of Sciences, Xi'an 710061, China
Haiyan Ni
State Key Laboratory of Loess and Quaternary Geology, Key
Laboratory of Aerosol Chemistry and Physics, Institute of Earth
Environment, Chinese Academy of Sciences, Xi'an 710061, China
CAS Center for Excellence in Quaternary Science and Global Change,
Chinese Academy of Sciences, Xi'an 710061, China
Meng Wang
State Key Laboratory of Loess and Quaternary Geology, Key
Laboratory of Aerosol Chemistry and Physics, Institute of Earth
Environment, Chinese Academy of Sciences, Xi'an 710061, China
CAS Center for Excellence in Quaternary Science and Global Change,
Chinese Academy of Sciences, Xi'an 710061, China
Jurgita Ovadnevaite
School of Physics and Centre for Climate and Air Pollution Studies,
Ryan Institute, National University of Ireland Galway, University Road,
Galway, H91CF50, Ireland
Darius Ceburnis
School of Physics and Centre for Climate and Air Pollution Studies,
Ryan Institute, National University of Ireland Galway, University Road,
Galway, H91CF50, Ireland
Chunying Chen
CAS Key Laboratory for Biological Effects of Nanomaterials and
Nanosafety, National Centre for Nanoscience and Technology, Beijing 100191,
China
Douglas R. Worsnop
Aerodyne Research, Inc., Billerica, MA, USA
Thorsten Hoffmann
Institute of Inorganic and Analytical Chemistry, Johannes Gutenberg
University Mainz, Duesbergweg 10–14, 55128 Mainz, Germany
Colin O'Dowd
School of Physics and Centre for Climate and Air Pollution Studies,
Ryan Institute, National University of Ireland Galway, University Road,
Galway, H91CF50, Ireland
Junji Cao
State Key Laboratory of Loess and Quaternary Geology, Key
Laboratory of Aerosol Chemistry and Physics, Institute of Earth
Environment, Chinese Academy of Sciences, Xi'an 710061, China
CAS Center for Excellence in Quaternary Science and Global Change,
Chinese Academy of Sciences, Xi'an 710061, China
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We analyse a southern Siberian stalagmite to reconstruct soil respiration, wildfire, and vegetation trends during the Last Interglacial (LIG) (124.1–118.8 ka) and the Holocene (10–0 ka). Wildfires were more prevalent during the LIG than the Holocene and were supported by fire-prone species, low soil respiration, and a greater difference between summer and winter temperature. We show that vegetation type and summer/winter temperature contrast are strong drivers of Siberian wildfires.
Tiantian Wang, Jun Zhang, Houssni Lamkaddam, Kun Li, Ka Yuen Cheung, Lisa Kattner, Erlend Gammelsæter, Michael Bauer, Zachary C. J. Decker, Deepika Bhattu, Rujin Huang, Rob L. Modini, Jay G. Slowik, Imad El Haddad, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 25, 2707–2724, https://doi.org/10.5194/acp-25-2707-2025, https://doi.org/10.5194/acp-25-2707-2025, 2025
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Our study analyzes real-time emissions of organic vapors from solid fuel combustion. Using the mass spectrometer, we tested various fuels, finding higher emission factors for organic vapors from wood burning. Intermediate-volatility organic compounds constituted a significant fraction of emissions in solid fuel combustion. Statistical tests identified unique potential markers. Our insights benefit air quality, climate, and health, aiding accurate emission assessments.
Denis Leppla, Stefanie Hildmann, Nora Zannoni, Leslie Kremper, Bruna Hollanda, Jonathan Williams, Christopher Pöhlker, Stefan Wolff, Marta Sà, Maria Cristina Solci, Ulrich Pöschl, and Thorsten Hoffmann
EGUsphere, https://doi.org/10.5194/egusphere-2025-141, https://doi.org/10.5194/egusphere-2025-141, 2025
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The chemical composition of organic particles in the Amazon rainforest was investigated to understand how biogenic and human emissions influence the atmosphere in this unique ecosystem. Seasonal patterns were found where wet seasons were dominated by biogenic compounds from natural sources while dry seasons showed increased fire-related pollutants. These findings reveal how emissions, fires and long-range transport affect atmospheric chemistry, with implications for climate models.
Lang Liu, Xin Long, Yi Li, Zengliang Zang, Fengwen Wang, Yan Han, Zhier Bao, Yang Chen, Tian Feng, and Jinxin Yang
Atmos. Chem. Phys., 25, 1569–1585, https://doi.org/10.5194/acp-25-1569-2025, https://doi.org/10.5194/acp-25-1569-2025, 2025
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This study uses WRF-Chem to assess how meteorological conditions and emission reductions affected fine particulate matter (PM2.5) in the North China Plain (NCP). It highlights regional disparities: in the northern NCP, adverse weather negated emission reduction effects. In contrast, the southern NCP featured a PM2.5 decrease due to favorable weather and emission reductions. The research highlighted the interaction between emissions, meteorology, and PM2.5.
Yiliang Liu, Arttu Yli-Kujala, Fabian Schmidt-Ott, Sebastian Holm, Lauri Ahonen, Tommy Chan, Joonas Enroth, Joonas Vanhanen, Runlong Cai, Tuukka Petäjä, Markku Kulmala, Yang Chen, and Juha Kangasluoma
Atmos. Meas. Tech., 18, 431–442, https://doi.org/10.5194/amt-18-431-2025, https://doi.org/10.5194/amt-18-431-2025, 2025
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Accurate measurement of nanoparticles is crucial for understanding their impact on new particle formation and climate change. In this study, we calibrated the Particle Size Magnifier version 2.0 (PSM 2.0), using both laboratory-generated and atmospheric particles. Some differences were observed in the calibration results, with direct calibration using atmospheric particles enhancing measurement accuracy.
Johanna Schäfer, Anja Beschnitt, François Burgay, Thomas Singer, Margit Schwikowski, and Thorsten Hoffmann
Atmos. Meas. Tech., 18, 421–430, https://doi.org/10.5194/amt-18-421-2025, https://doi.org/10.5194/amt-18-421-2025, 2025
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Glaciers preserve organic compounds from atmospheric aerosols, which can serve as markers for emission sources. Most studies overlook the enantiomers of chiral compounds. We developed a two-dimensional liquid chromatography method to determine the chiral ratios of the monoterpene oxidation products cis-pinic acid and cis-pinonic acid in ice-core samples. Applied to samples from the Belukha Glacier (1870–1970 CE), the method revealed fluctuating chiral ratios for the analytes.
Christine Borchers, Lasse Moormann, Bastien Geil, Niklas Karbach, and Thorsten Hoffmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-4015, https://doi.org/10.5194/egusphere-2024-4015, 2025
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A three-dimensionally printed filter holder is connected to a lightweight, high-performance pump. This sampling system allows for easy and cost-effective measurements of organic aerosols at different heights and locations. By elucidating the chemical composition of organic aerosol, sources and processing of the compounds can be identified. Measurements at different altitudes and times of the day provide insight into the chemical aging and daytime trends of the aerosol particles.
Diego Aliaga, Victoria A. Sinclair, Radovan Krejci, Marcos Andrade, Paulo Artaxo, Luis Blacutt, Runlong Cai, Samara Carbone, Yvette Gramlich, Liine Heikkinen, Dominic Heslin-Rees, Wei Huang, Veli-Matti Kerminen, Alkuin Maximilian Koenig, Markku Kulmala, Paolo Laj, Valeria Mardoñez-Balderrama, Claudia Mohr, Isabel Moreno, Pauli Paasonen, Wiebke Scholz, Karine Sellegri, Laura Ticona, Gaëlle Uzu, Fernando Velarde, Alfred Wiedensohler, Doug Worsnop, Cheng Wu, Chen Xuemeng, Qiaozhi Zha, and Federico Bianchi
Aerosol Research, 3, 15–44, https://doi.org/10.5194/ar-3-15-2025, https://doi.org/10.5194/ar-3-15-2025, 2025
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This study examines new particle formation (NPF) in the Bolivian Andes at Chacaltaya mountain (CHC) and the urban El Alto–La Paz area (EAC). Days are clustered into four categories based on NPF intensity. Differences in particle size, precursor gases, and pollution levels are found. High NPF intensities increased Aitken mode particle concentrations at both sites, while volcanic influence selectively diminished NPF intensity at CHC but not EAC. This study highlights NPF dynamics in the Andes.
Christine Borchers, Jackson Seymore, Martanda Gautam, Konstantin Dörholt, Yannik Müller, Andreas Arndt, Laura Gömmer, Florian Ungeheuer, Miklós Szakáll, Stephan Borrmann, Alexander Theis, Alexander L. Vogel, and Thorsten Hoffmann
Atmos. Chem. Phys., 24, 13961–13974, https://doi.org/10.5194/acp-24-13961-2024, https://doi.org/10.5194/acp-24-13961-2024, 2024
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Riming, a crucial process in cloud dynamics, influences the vertical distribution of compounds in the atmosphere. Experiments in Mainz's wind tunnel investigated retention coefficients of organic compounds under varying conditions. Findings suggest a correlation between the Henry's law constant and retention, applicable even to complex organic molecules.
Zhaojin An, Rujing Yin, Xinyan Zhao, Xiaoxiao Li, Yuyang Li, Yi Yuan, Junchen Guo, Yiqi Zhao, Xue Li, Dandan Li, Yaowei Li, Dongbin Wang, Chao Yan, Kebin He, Douglas R. Worsnop, Frank N. Keutsch, and Jingkun Jiang
Atmos. Chem. Phys., 24, 13793–13810, https://doi.org/10.5194/acp-24-13793-2024, https://doi.org/10.5194/acp-24-13793-2024, 2024
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Online Vocus-PTR measurements show the compositions and seasonal variations in organic vapors in urban Beijing. With enhanced sensitivity and mass resolution, various species at a level of sub-parts per trillion (ppt) and organics with multiple oxygens (≥ 3) were observed. The fast photooxidation process in summer leads to an increase in both concentration and proportion of organics with multiple oxygens, while, in other seasons, the variations in them could be influenced by mixed sources.
Wei Yuan, Ru-Jin Huang, Chao Luo, Lu Yang, Wenjuan Cao, Jie Guo, and Huinan Yang
Atmos. Chem. Phys., 24, 13219–13230, https://doi.org/10.5194/acp-24-13219-2024, https://doi.org/10.5194/acp-24-13219-2024, 2024
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We characterized water-soluble oxidative potential (OP) levels in wintertime PM2.5 in the south and north of Beijing. Our results show that the volume-normalized dithiothreitol (DTTv) in the north was comparable to that in the south, while the mass-normalized dithiothreitol (DTTm) in the north was almost twice that in the south. Traffic-related emissions and biomass burning were the main sources of DTTv in the south, and traffic-related emissions contributed the most to DTTv in the north.
Meng Wang, Qiyuan Wang, Steven Sai Hang Ho, Jie Tian, Yong Zhang, Shun-cheng Lee, and Junji Cao
Atmos. Chem. Phys., 24, 11175–11189, https://doi.org/10.5194/acp-24-11175-2024, https://doi.org/10.5194/acp-24-11175-2024, 2024
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We studied nitrogen-containing organic compounds (NOCs) in particulate matter <2.5 µm particles on the southeastern Tibetan Plateau. We found that biomass burning and transboundary transport are the main sources of NOCs in the high-altitude area. Understanding these aerosol sources informs how they add to regional and potentially global climate changes. Our findings could help shape effective environmental policies to enhance air quality and address climate impacts in this sensitive region.
Kirsten N. Fossum, Chunshui Lin, Niall O'Sullivan, Lu Lei, Stig Hellebust, Darius Ceburnis, Aqeel Afzal, Anja Tremper, David Green, Srishti Jain, Steigvilė Byčenkienė, Colin O'Dowd, John Wenger, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 24, 10815–10831, https://doi.org/10.5194/acp-24-10815-2024, https://doi.org/10.5194/acp-24-10815-2024, 2024
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The chemical composition and sources of submicron aerosol in the Dublin Port area were investigated over a month-long campaign. Two distinct types of ship emissions were identified and characterised: sulfate-rich plumes from the use of heavy fuel oil with scrubbers and organic-rich plumes from the use of low-sulfur fuels. The latter were more frequent, emitting double the particle number and having a typical V / Ni ratio for ship emission.
Xinya Liu, Diego Alves Gouveia, Bas Henzing, Arnoud Apituley, Arjan Hensen, Danielle van Dinther, Rujin Huang, and Ulrike Dusek
Atmos. Chem. Phys., 24, 9597–9614, https://doi.org/10.5194/acp-24-9597-2024, https://doi.org/10.5194/acp-24-9597-2024, 2024
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The vertical distribution of aerosol optical properties is important for their effect on climate. This is usually measured by lidar, which has limitations, most notably the assumption of a lidar ratio. Our study shows that routine surface-level aerosol measurements are able to predict this lidar ratio reasonably well within the lower layers of the atmosphere and thus provide a relatively simple and cost-effective method to improve lidar measurements.
Tianle Pan, Andrew T. Lambe, Weiwei Hu, Yicong He, Minghao Hu, Huaishan Zhou, Xinming Wang, Qingqing Hu, Hui Chen, Yue Zhao, Yuanlong Huang, Doug R. Worsnop, Zhe Peng, Melissa A. Morris, Douglas A. Day, Pedro Campuzano-Jost, Jose-Luis Jimenez, and Shantanu H. Jathar
Atmos. Meas. Tech., 17, 4915–4939, https://doi.org/10.5194/amt-17-4915-2024, https://doi.org/10.5194/amt-17-4915-2024, 2024
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This study systematically characterizes the temperature enhancement in the lamp-enclosed oxidation flow reactor (OFR). The enhancement varied multiple dimensional factors, emphasizing the complexity of temperature inside of OFR. The effects of temperature on the flow field and gas- or particle-phase reaction inside OFR were also evaluated with experiments and model simulations. Finally, multiple mitigation strategies were demonstrated to minimize this temperature increase.
Zijun Zhang, Weiqi Xu, Yi Zhang, Wei Zhou, Xiangyu Xu, Aodong Du, Yinzhou Zhang, Hongqin Qiao, Ye Kuang, Xiaole Pan, Zifa Wang, Xueling Cheng, Lanzhong Liu, Qingyan Fu, Douglas R. Worsnop, Jie Li, and Yele Sun
Atmos. Chem. Phys., 24, 8473–8488, https://doi.org/10.5194/acp-24-8473-2024, https://doi.org/10.5194/acp-24-8473-2024, 2024
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We investigated aerosol composition and sources and the interaction between secondary organic aerosol (SOA) and clouds at a regional mountain site in southeastern China. Clouds efficiently scavenge more oxidized SOA; however, cloud evaporation leads to the production of less oxidized SOA. The unexpectedly high presence of nitrate in aerosol particles indicates that nitrate formed in polluted areas has undergone interactions with clouds, significantly influencing the regional background site.
Muhammed Irfan, Thomas Kühn, Taina Yli-Juuti, Anton Laakso, Eemeli Holopainen, Douglas R. Worsnop, Annele Virtanen, and Harri Kokkola
Atmos. Chem. Phys., 24, 8489–8506, https://doi.org/10.5194/acp-24-8489-2024, https://doi.org/10.5194/acp-24-8489-2024, 2024
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The study examines how the volatility of semi-volatile organic compounds affects secondary organic aerosol (SOA) formation and climate. Our simulations show that uncertainties in these volatilities influence aerosol mass and climate impacts. Accurate representation of these compounds in climate models is crucial for predicting global climate patterns.
Niklas Karbach, Lisa Höhler, Peter Hoor, Heiko Bozem, Nicole Bobrowski, and Thorsten Hoffmann
Atmos. Meas. Tech., 17, 4081–4086, https://doi.org/10.5194/amt-17-4081-2024, https://doi.org/10.5194/amt-17-4081-2024, 2024
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The system presented here can accurately generate and reproduce a stable flow of gas mixtures of known concentrations over several days using ambient air as a dilution medium. In combination with the small size and low weight of the system, this enables the calibration of hydrogen sensors in the field, reducing the influence of matrix effects on the accuracy of the sensor. The system is inexpensive to assemble and easy to maintain, which is the key to reliable measurement results.
Jing Duan, Ru-Jin Huang, Ying Wang, Wei Xu, Haobin Zhong, Chunshui Lin, Wei Huang, Yifang Gu, Jurgita Ovadnevaite, Darius Ceburnis, and Colin O'Dowd
Atmos. Chem. Phys., 24, 7687–7698, https://doi.org/10.5194/acp-24-7687-2024, https://doi.org/10.5194/acp-24-7687-2024, 2024
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The chemical composition of atmospheric particles has shown significant changes in recent years. We investigated the potential effects of changes in inorganics on aerosol water uptake and, thus, secondary organic aerosol formation in wintertime haze based on the size-resolved measurements of non-refractory fine particulate matter (NR-PM2.5) in Xi’an, northwestern China. We highlight the key role of aerosol water as a medium to link inorganics and organics in their multiphase processes.
Karam Mansour, Stefano Decesari, Darius Ceburnis, Jurgita Ovadnevaite, Lynn M. Russell, Marco Paglione, Laurent Poulain, Shan Huang, Colin O'Dowd, and Matteo Rinaldi
Earth Syst. Sci. Data, 16, 2717–2740, https://doi.org/10.5194/essd-16-2717-2024, https://doi.org/10.5194/essd-16-2717-2024, 2024
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We propose and evaluate machine learning predictive algorithms to model freshly formed biogenic methanesulfonic acid and sulfate concentrations. The long-term constructed dataset covers the North Atlantic at an unprecedented resolution. The improved parameterization of biogenic sulfur aerosols at regional scales is essential for determining their radiative forcing, which could help further understand marine-aerosol–cloud interactions and reduce uncertainties in climate models
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
Atmos. Chem. Phys., 24, 5625–5636, https://doi.org/10.5194/acp-24-5625-2024, https://doi.org/10.5194/acp-24-5625-2024, 2024
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Cooking is a major source of particles in urban areas. Previous studies demonstrated that the chemical lifetimes of cooking organic aerosols (COAs) were much shorter (~minutes) than the values reported by field observations (~hours). We conducted laboratory experiments to resolve the discrepancy by considering suppressed reactivity under low temperature. The parameterized k2–T relationships and observed surface temperature data were used to estimate the chemical lifetimes of COA particles.
Fangbing Li, Dan Dan Huang, Linhui Tian, Bin Yuan, Wen Tan, Liang Zhu, Penglin Ye, Douglas Worsnop, Ka In Hoi, Kai Meng Mok, and Yong Jie Li
Atmos. Meas. Tech., 17, 2415–2427, https://doi.org/10.5194/amt-17-2415-2024, https://doi.org/10.5194/amt-17-2415-2024, 2024
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The responses of protonated, adduct, and fragmented ions of 21 volatile organic compounds (VOCs) were investigated with varying instrument settings and relative humidity (RH) in a Vocus proton-transfer-reaction mass spectrometer (PTR-MS). The protonated ions of most VOCs studied show < 15 % variation in sensitivity, except for some long-chain aldehydes. The relationship between sensitivity and PTR rate constant is complicated by the influences from ion transmission and protonated ion fraction.
Mahen Konwar, Benjamin Werden, Edward C. Fortner, Sudarsan Bera, Mercy Varghese, Subharthi Chowdhuri, Kurt Hibert, Philip Croteau, John Jayne, Manjula Canagaratna, Neelam Malap, Sandeep Jayakumar, Shivsai A. Dixit, Palani Murugavel, Duncan Axisa, Darrel Baumgardner, Peter F. DeCarlo, Doug R. Worsnop, and Thara Prabhakaran
Atmos. Meas. Tech., 17, 2387–2400, https://doi.org/10.5194/amt-17-2387-2024, https://doi.org/10.5194/amt-17-2387-2024, 2024
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In a warm cloud seeding experiment hygroscopic particles are released to alter cloud processes to induce early raindrops. During the Cloud–Aerosol Interaction and Precipitation Enhancement Experiment, airborne mini aerosol mass spectrometers analyse the particles on which clouds form. The seeded clouds showed higher concentrations of chlorine and potassium, the oxidizing agents of flares. Small cloud droplet concentrations increased, and seeding particles were detected in deep cloud depths.
Markku Kulmala, Diego Aliaga, Santeri Tuovinen, Runlong Cai, Heikki Junninen, Chao Yan, Federico Bianchi, Yafang Cheng, Aijun Ding, Douglas R. Worsnop, Tuukka Petäjä, Katrianne Lehtipalo, Pauli Paasonen, and Veli-Matti Kerminen
Aerosol Research, 2, 49–58, https://doi.org/10.5194/ar-2-49-2024, https://doi.org/10.5194/ar-2-49-2024, 2024
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Atmospheric new particle formation (NPF), together with secondary production of particulate matter in the atmosphere, dominates aerosol particle number concentrations and submicron particle mass loads in many environments globally. In this opinion paper, we describe the paradigm shift to understand NPF in a continuous way instead of using traditional binary event–non-event analysis.
Xinya Liu, Bas Henzing, Arjan Hensen, Jan Mulder, Peng Yao, Danielle van Dinther, Jerry van Bronckhorst, Rujin Huang, and Ulrike Dusek
Atmos. Chem. Phys., 24, 3405–3420, https://doi.org/10.5194/acp-24-3405-2024, https://doi.org/10.5194/acp-24-3405-2024, 2024
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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.
Jian Zhao, Valter Mickwitz, Yuanyuan Luo, Ella Häkkinen, Frans Graeffe, Jiangyi Zhang, Hilkka Timonen, Manjula Canagaratna, Jordan E. Krechmer, Qi Zhang, Markku Kulmala, Juha Kangasluoma, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 17, 1527–1543, https://doi.org/10.5194/amt-17-1527-2024, https://doi.org/10.5194/amt-17-1527-2024, 2024
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Organic aerosol constitutes a significant portion of atmospheric fine particles but is less characterized due to its vast number of constituents. Recently, we developed a system for online measurements of particle-phase highly oxygenated organic molecules (HOMs). In this work, we systematically characterized the system, developed a new unit to enhance its performance, and demonstrated the essential role of thermograms in inferring volatility and quantifying HOMs in organic aerosols.
Jiangyi Zhang, Jian Zhao, Yuanyuan Luo, Valter Mickwitz, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 24, 2885–2911, https://doi.org/10.5194/acp-24-2885-2024, https://doi.org/10.5194/acp-24-2885-2024, 2024
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Due to the intrinsic connection between the formation pathways of O3 and HOMs, the ratio of HOM dimers or non-nitrate monomers to HOM organic nitrates could be used to determine O3 formation regimes. Owing to the fast formation and short lifetimes of HOMs, HOM-based indicating ratios can describe O3 formation in real time. Despite the success of our approach in this simple laboratory system, applicability to the much more complex atmosphere remains to be determined.
Feifan Yan, Hang Su, Yafang Cheng, Rujin Huang, Hong Liao, Ting Yang, Yuanyuan Zhu, Shaoqing Zhang, Lifang Sheng, Wenbin Kou, Xinran Zeng, Shengnan Xiang, Xiaohong Yao, Huiwang Gao, and Yang Gao
Atmos. Chem. Phys., 24, 2365–2376, https://doi.org/10.5194/acp-24-2365-2024, https://doi.org/10.5194/acp-24-2365-2024, 2024
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PM2.5 pollution is a major air quality issue deteriorating human health, and previous studies mostly focus on regions like the North China Plain and Yangtze River Delta. However, the characteristics of PM2.5 concentrations between these two regions are studied less often. Focusing on the transport corridor region, we identify an interesting seesaw transport phenomenon with stagnant weather conditions, conducive to PM2.5 accumulation over this region, resulting in large health effects.
Xi Cheng, Yong Jie Li, Yan Zheng, Keren Liao, Theodore K. Koenig, Yanli Ge, Tong Zhu, Chunxiang Ye, Xinghua Qiu, and Qi Chen
Atmos. Chem. Phys., 24, 2099–2112, https://doi.org/10.5194/acp-24-2099-2024, https://doi.org/10.5194/acp-24-2099-2024, 2024
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In this study we conducted laboratory measurements to investigate the formation of gas-phase oxygenated organic molecules (OOMs) from six aromatic volatile organic compounds (VOCs). We provide a thorough analysis on the effects of precursor structure (substituents and ring numbers) on product distribution and highlight from a laboratory perspective that heavy (e.g., double-ring) aromatic VOCs are important in initial particle growth during secondary organic aerosol formation.
Shuzheng Guo, Chunxiang Ye, Weili Lin, Yi Chen, Limin Zeng, Xuena Yu, Jinhui Cui, Chong Zhang, Jing Duan, Haobin Zhong, Rujin Huang, Xuguang Chi, Wei Nie, and Aijun Ding
EGUsphere, https://doi.org/10.5194/egusphere-2024-262, https://doi.org/10.5194/egusphere-2024-262, 2024
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@Tibet field campaigns 2021 discovered surprisingly high levels and activity contributions of oxygenated volatile organic compounds on the southeast of the Tibetan Plateau, which suggests that OVOCs may play a larger role in the chemical reactions that occur in high-altitude regions than previously thought.
Chen He, Hanxiong Che, Zier Bao, Yiliang Liu, Qing Li, Miao Hu, Jiawei Zhou, Shumin Zhang, Xiaojiang Yao, Quan Shi, Chunmao Chen, Yan Han, Lingshuo Meng, Xin Long, Fumo Yang, and Yang Chen
Atmos. Chem. Phys., 24, 1627–1639, https://doi.org/10.5194/acp-24-1627-2024, https://doi.org/10.5194/acp-24-1627-2024, 2024
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We examined the daily evolution of high molecular-weight organic compounds with a molecular weight of up to 1000 Da in order to comprehend their behaviors in the atmosphere under actual conditions. These compounds were proven to undergo multi-generation oxidation, carboxylation, and nitrification via both day- and nighttime chemistry.
Diego Aliaga, Santeri Tuovinen, Tinghan Zhang, Janne Lampilahti, Xinyang Li, Lauri Ahonen, Tom Kokkonen, Tuomo Nieminen, Simo Hakala, Pauli Paasonen, Federico Bianchi, Doug Worsnop, Veli-Matti Kerminen, and Markku Kulmala
Aerosol Research, 1, 81–92, https://doi.org/10.5194/ar-1-81-2023, https://doi.org/10.5194/ar-1-81-2023, 2023
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We introduce a novel method for evaluating days when small particles are formed in the atmosphere. Instead of the traditional binary division between event and non-event days, our method, known as "nano ranking analysis", provides a continuous, non-categorical metric for each day. By utilizing data from Hyytiälä, Finland, we show that our approach effectively quantifies these events. This innovative method paves the way for a deeper understanding of the factors influencing particle formation.
Yuquan Gong, Ru-Jin Huang, Lu Yang, Ting Wang, Wei Yuan, Wei Xu, Wenjuan Cao, Yang Wang, and Yongjie Li
Atmos. Chem. Phys., 23, 15197–15207, https://doi.org/10.5194/acp-23-15197-2023, https://doi.org/10.5194/acp-23-15197-2023, 2023
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This study reveals the large day–night differences in brown carbon (BrC) chromophore composition, which was not known previously. The results provide insights into the effects of atmospheric processes and emissions on BrC composition.
Zhongwei Luo, Yan Han, Kun Hua, Yufen Zhang, Jianhui Wu, Xiaohui Bi, Qili Dai, Baoshuang Liu, Yang Chen, Xin Long, and Yinchang Feng
Geosci. Model Dev., 16, 6757–6771, https://doi.org/10.5194/gmd-16-6757-2023, https://doi.org/10.5194/gmd-16-6757-2023, 2023
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This study explores how the variation in the source profiles adopted in chemical transport models (CTMs) impacts the simulated results of chemical components in PM2.5 based on sensitivity analysis. The impact on PM2.5 components cannot be ignored, and its influence can be transmitted and linked between components. The representativeness and timeliness of the source profile should be paid adequate attention in air quality simulation.
Shasha Tian, Kexin Zu, Huabin Dong, Limin Zeng, Keding Lu, and Qi Chen
Atmos. Meas. Tech., 16, 5525–5535, https://doi.org/10.5194/amt-16-5525-2023, https://doi.org/10.5194/amt-16-5525-2023, 2023
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We developed an online NH3 monitoring system based on a selective colorimetric reaction and a long-path absorption photometer (SAC-LOPAP), which can run statically for a long time and be applied to the continuous online measurement of low concentrations of ambient air by optimizing the reaction conditions, adding a constant-temperature module and liquid flow controller. It is well suited for the investigation of the NH3 budget for urban to rural conditions in China.
Andrew T. Lambe, Bin Bai, Masayuki Takeuchi, Nicole Orwat, Paul M. Zimmerman, Mitchell W. Alton, Nga L. Ng, Andrew Freedman, Megan S. Claflin, Drew R. Gentner, Douglas R. Worsnop, and Pengfei Liu
Atmos. Chem. Phys., 23, 13869–13882, https://doi.org/10.5194/acp-23-13869-2023, https://doi.org/10.5194/acp-23-13869-2023, 2023
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We developed a new method to generate nitrate radicals (NO3) for atmospheric chemistry applications that works by irradiating mixtures containing ceric ammonium nitrate with a UV light at room temperature. It has several advantages over traditional NO3 sources. We characterized its performance over a range of mixture and reactor conditions as well as other irradiation products. Proof of concept was demonstrated by generating and characterizing oxidation products of the β-pinene + NO3 reaction.
Jiyeon Park, Hyojin Kang, Yeontae Gim, Eunho Jang, Ki-Tae Park, Sangjong Park, Chang Hoon Jung, Darius Ceburnis, Colin O'Dowd, and Young Jun Yoon
Atmos. Chem. Phys., 23, 13625–13646, https://doi.org/10.5194/acp-23-13625-2023, https://doi.org/10.5194/acp-23-13625-2023, 2023
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We measured the number size distribution of 2.5–300 nm particles and cloud condensation nuclei (CCN) number concentrations at King Sejong Station on the Antarctic Peninsula continuously from 1 January to 31 December 2018. During the pristine and clean periods, 97 new particle formation (NPF) events were detected. For 83 of these, CCN concentrations increased by 2 %–268 % (median 44 %) following 1 to 36 h (median 8 h) after NPF events.
Xu-Cheng He, Jiali Shen, Siddharth Iyer, Paxton Juuti, Jiangyi Zhang, Mrisha Koirala, Mikko M. Kytökari, Douglas R. Worsnop, Matti Rissanen, Markku Kulmala, Norbert M. Maier, Jyri Mikkilä, Mikko Sipilä, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 4461–4487, https://doi.org/10.5194/amt-16-4461-2023, https://doi.org/10.5194/amt-16-4461-2023, 2023
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In this study, the upgraded multi-scheme chemical ionisation inlet 2 is presented. Sulfuric acid, hypoiodous acid, iodine, sulfur dioxide, and hydroperoxyl radicals are calibrated, and the improved ion optics allow us to detect sulfuric acid and iodine-containing molecules at as low as a few parts per quadrillion by volume. Additionally, we confirm the reliable detection of iodic acid using both the nitrate and bromide chemical ionisation methods under atmospherically relevant conditions.
Meng Wang, Yusen Duan, Zhuozhi Zhang, Qi Yuan, Xinwei Li, Shuwen Han, Juntao Huo, Jia Chen, Yanfen Lin, Qingyan Fu, Tao Wang, Junji Cao, and Shun-cheng Lee
Atmos. Chem. Phys., 23, 10313–10324, https://doi.org/10.5194/acp-23-10313-2023, https://doi.org/10.5194/acp-23-10313-2023, 2023
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Hourly elemental carbon (EC) and NOx were continuously measured for 5 years (2016–2020) at a sampling site near a highway in western Shanghai. We use a machine learning model to rebuild the measured EC and NOx, and a business-as-usual (BAU) scenario was assumed in 2020 and compared with the measured EC and NOx.
Taomou Zong, Zhijun Wu, Junrui Wang, Kai Bi, Wenxu Fang, Yanrong Yang, Xuena Yu, Zhier Bao, Xiangxinyue Meng, Yuheng Zhang, Song Guo, Yang Chen, Chunshan Liu, Yue Zhang, Shao-Meng Li, and Min Hu
Atmos. Meas. Tech., 16, 3679–3692, https://doi.org/10.5194/amt-16-3679-2023, https://doi.org/10.5194/amt-16-3679-2023, 2023
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This study developed and characterized an indoor chamber system (AIR) to simulate atmospheric multiphase chemistry processes. The AIR chamber can accurately control temperature and relative humidity (RH) over a broad range and simulate diurnal variation of ambient atmospheric RH. The aerosol generation unit can generate organic-coating seed particles with different phase states. The AIR chamber demonstrates high-quality performance in simulating secondary aerosol formation.
Julia Homann, Niklas Karbach, Stacy A. Carolin, Daniel H. James, David Hodell, Sebastian F. M. Breitenbach, Ola Kwiecien, Mark Brenner, Carlos Peraza Lope, and Thorsten Hoffmann
Biogeosciences, 20, 3249–3260, https://doi.org/10.5194/bg-20-3249-2023, https://doi.org/10.5194/bg-20-3249-2023, 2023
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Cave stalagmites contain substances that can be used to reconstruct past changes in local and regional environmental conditions. We used two classes of biomarkers (polycyclic aromatic hydrocarbons and monosaccharide anhydrides) to detect the presence of fire and to also explore changes in fire regime (e.g. fire frequency, intensity, and fuel source). We tested our new method on a stalagmite from Mayapan, a large Maya city on the Yucatán Peninsula.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Daniel John Katz, Aroob Abdelhamid, Harald Stark, Manjula R. Canagaratna, Douglas R. Worsnop, and Eleanor C. Browne
Atmos. Chem. Phys., 23, 5567–5585, https://doi.org/10.5194/acp-23-5567-2023, https://doi.org/10.5194/acp-23-5567-2023, 2023
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Ambient ion chemical composition measurements provide insight into trace gases that are precursors for the formation and growth of new aerosol particles. We use a new data analysis approach to increase the chemical information from these measurements. We analyze results from an agricultural region, a little studied land use type that is ~41 % of global land use, and find that the composition of gases important for aerosol formation and growth differs significantly from that in other ecosystems.
Yifang Gu, Ru-Jin Huang, Jing Duan, Wei Xu, Chunshui Lin, Haobin Zhong, Ying Wang, Haiyan Ni, Quan Liu, Ruiguang Xu, Litao Wang, and Yong Jie Li
Atmos. Chem. Phys., 23, 5419–5433, https://doi.org/10.5194/acp-23-5419-2023, https://doi.org/10.5194/acp-23-5419-2023, 2023
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Secondary organic aerosol (SOA) can be produced by various pathways, but its formation mechanisms are unclear. Observations were conducted in the North China Plain during a highly oxidizing atmosphere in summer. We found that fast photochemistry dominated SOA formation during daytime. Two types of aqueous-phase chemistry (nocturnal and daytime processing) take place at high relative humidity. The potential transformation from primary organic aerosol (POA) to SOA was also an important pathway.
Qiaozhi Zha, Wei Huang, Diego Aliaga, Otso Peräkylä, Liine Heikkinen, Alkuin Maximilian Koenig, Cheng Wu, Joonas Enroth, Yvette Gramlich, Jing Cai, Samara Carbone, Armin Hansel, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, Victoria Sinclair, Radovan Krejci, Marcos Andrade, Claudia Mohr, and Federico Bianchi
Atmos. Chem. Phys., 23, 4559–4576, https://doi.org/10.5194/acp-23-4559-2023, https://doi.org/10.5194/acp-23-4559-2023, 2023
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We investigate the chemical composition of atmospheric cluster ions from January to May 2018 at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes. With state-of-the-art mass spectrometers and air mass history analysis, the measured cluster ions exhibited distinct diurnal and seasonal patterns, some of which contributed to new particle formation. Our study will improve the understanding of atmospheric ions and their role in high-altitude new particle formation.
Ella Häkkinen, Jian Zhao, Frans Graeffe, Nicolas Fauré, Jordan E. Krechmer, Douglas Worsnop, Hilkka Timonen, Mikael Ehn, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 1705–1721, https://doi.org/10.5194/amt-16-1705-2023, https://doi.org/10.5194/amt-16-1705-2023, 2023
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Highly oxygenated compounds contribute to the formation and growth of atmospheric organic aerosol and thus impact the global climate. Knowledge of their transformations and fate after condensing into the particle phase has been limited by the lack of suitable detection techniques. Here, we present an online method for measuring highly oxygenated compounds from organic aerosol. We evaluate the performance of the method and demonstrate that the method is applicable to different organic species.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
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Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Chunshui Lin, Ru-Jin Huang, Haobin Zhong, Jing Duan, Zixi Wang, Wei Huang, and Wei Xu
Atmos. Chem. Phys., 23, 3595–3607, https://doi.org/10.5194/acp-23-3595-2023, https://doi.org/10.5194/acp-23-3595-2023, 2023
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The complex interaction between O3 and PM2.5, coupled with the topology of the Fenwei Plain and the evolution of the boundary layer height, highlights the challenges in further reducing particulate pollution in winter despite years of efforts to reduce emissions. Through scenario analysis in a chemical box model constrained by observation, we show the co-benefits of reducing NOx and VOCs simultaneously in reducing ozone and SOA.
Huanhuan Zhang, Rui Li, Chengpeng Huang, Xiaofei Li, Shuwei Dong, Fu Wang, Tingting Li, Yizhu Chen, Guohua Zhang, Yan Ren, Qingcai Chen, Ru-jin Huang, Siyu Chen, Tao Xue, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 23, 3543–3559, https://doi.org/10.5194/acp-23-3543-2023, https://doi.org/10.5194/acp-23-3543-2023, 2023
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This work investigated the seasonal variation of aerosol Fe solubility for coarse and fine particles in Xi’an, a megacity in northwestern China severely affected by anthropogenic emission and desert dust aerosol. In addition, we discussed in depth what controlled aerosol Fe solubility at different seasons for coarse and fine particles.
Jing Cai, Kaspar R. Daellenbach, Cheng Wu, Yan Zheng, Feixue Zheng, Wei Du, Sophie L. Haslett, Qi Chen, Markku Kulmala, and Claudia Mohr
Atmos. Meas. Tech., 16, 1147–1165, https://doi.org/10.5194/amt-16-1147-2023, https://doi.org/10.5194/amt-16-1147-2023, 2023
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We introduce the offline application of FIGAERO-CIMS by analyzing Teflon and quartz filter samples that were collected at a typical urban site in Beijing with the deposition time varying from 30 min to 24 h. This method provides a feasible, simple, and quantitative way to investigate the molecular composition and volatility of OA compounds by using FIGAERO-CIMS to analyze offline samples.
Zhier Bao, Xinyi Zhang, Qing Li, Jiawei Zhou, Guangming Shi, Li Zhou, Fumo Yang, Shaodong Xie, Dan Zhang, Chongzhi Zhai, Zhenliang Li, Chao Peng, and Yang Chen
Atmos. Chem. Phys., 23, 1147–1167, https://doi.org/10.5194/acp-23-1147-2023, https://doi.org/10.5194/acp-23-1147-2023, 2023
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We characterised non-refractory fine particulate matter (PM2.5) during winter in the Sichuan Basin (SCB), Southwest China. The factors driving severe aerosol pollution were revealed, highlighting the importance of rapid nitrate formation and intensive biomass burning. Nitrate was primarily formed through gas-phase oxidation during daytime and aqueous-phase oxidation during nighttime. Controlling nitrate and biomass burning will benefit the mitigation of haze formation in the SCB.
Denis Leppla, Nora Zannoni, Leslie Kremper, Jonathan Williams, Christopher Pöhlker, Marta Sá, Maria Christina Solci, and Thorsten Hoffmann
Atmos. Chem. Phys., 23, 809–820, https://doi.org/10.5194/acp-23-809-2023, https://doi.org/10.5194/acp-23-809-2023, 2023
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Chiral chemodiversity plays a critical role in biochemical processes such as insect and plant communication. Here we report on the measurement of chiral-specified secondary organic aerosol in the Amazon rainforest. The results show that the chiral ratio is mainly determined by large-scale emission processes. Characteristic emissions of chiral aerosol precursors from different forest ecosystems can thus provide large-scale information on different biogenic sources via chiral particle analysis.
Yunfan Liu, Hang Su, Siwen Wang, Chao Wei, Wei Tao, Mira L. Pöhlker, Christopher Pöhlker, Bruna A. Holanda, Ovid O. Krüger, Thorsten Hoffmann, Manfred Wendisch, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Yafang Cheng
Atmos. Chem. Phys., 23, 251–272, https://doi.org/10.5194/acp-23-251-2023, https://doi.org/10.5194/acp-23-251-2023, 2023
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The origins of the abundant cloud condensation nuclei (CCN) in the upper troposphere (UT) of the Amazon remain unclear. With model developments of new secondary organic aerosol schemes and constrained by observation, we show that strong aerosol nucleation and condensation in the UT is triggered by biogenic organics, and organic condensation is key for UT CCN production. This UT CCN-producing mechanism may prevail over broader vegetation canopies and deserves emphasis in aerosol–climate feedback.
Qian Zhang, Yujie Zhang, Zhichun Wu, Bin Zhang, Yaling Zeng, Jian Sun, Hongmei Xu, Qiyuan Wang, Zhihua Li, Junji Cao, and Zhenxing Shen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-801, https://doi.org/10.5194/acp-2022-801, 2022
Revised manuscript not accepted
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We identified the brown carbon (BrC) molecules and their absorbing abilities on a molecular level from animal dung fuel combustion over the Tibetan Plateau region in China. The ultra-high performance liquid chromatography quadrupole time-of-flight mass spectrometer coupled with the partial least squares regression were precisely applied to characterize the molecular absorptions, key molecular markers, and radiative effects of BrC from household combustion scenarios at the high-altitude area.
Diwei Wang, Zhenxing Shen, Qian Zhang, Yali Lei, Tian Zhang, Shasha Huang, Jian Sun, Hongmei Xu, and Junji Cao
Atmos. Chem. Phys., 22, 14893–14904, https://doi.org/10.5194/acp-22-14893-2022, https://doi.org/10.5194/acp-22-14893-2022, 2022
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The optical properties and molecular structure of atmospheric brown carbon (BrC) in winter of several megacities in China were analyzed, and the source contribution of brown carbon was improved by using positive matrix factorization coupled with a multilayer perceptron neural network. These results can provide a basis for the more effective control of BrC to reduce its impacts on regional climates and human health.
Ville Leinonen, Harri Kokkola, Taina Yli-Juuti, Tero Mielonen, Thomas Kühn, Tuomo Nieminen, Simo Heikkinen, Tuuli Miinalainen, Tommi Bergman, Ken Carslaw, Stefano Decesari, Markus Fiebig, Tareq Hussein, Niku Kivekäs, Radovan Krejci, Markku Kulmala, Ari Leskinen, Andreas Massling, Nikos Mihalopoulos, Jane P. Mulcahy, Steffen M. Noe, Twan van Noije, Fiona M. O'Connor, Colin O'Dowd, Dirk Olivie, Jakob B. Pernov, Tuukka Petäjä, Øyvind Seland, Michael Schulz, Catherine E. Scott, Henrik Skov, Erik Swietlicki, Thomas Tuch, Alfred Wiedensohler, Annele Virtanen, and Santtu Mikkonen
Atmos. Chem. Phys., 22, 12873–12905, https://doi.org/10.5194/acp-22-12873-2022, https://doi.org/10.5194/acp-22-12873-2022, 2022
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We provide the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five different earth system models. We investigated aerosol modes (nucleation, Aitken, and accumulation) separately and were able to show the differences between measured and modeled trends and especially their seasonal patterns. The differences in model results are likely due to complex effects of several processes instead of certain specific model features.
Meng Wang, Yusen Duan, Wei Xu, Qiyuan Wang, Zhuozhi Zhang, Qi Yuan, Xinwei Li, Shuwen Han, Haijie Tong, Juntao Huo, Jia Chen, Shan Gao, Zhongbiao Wu, Long Cui, Yu Huang, Guangli Xiu, Junji Cao, Qingyan Fu, and Shun-cheng Lee
Atmos. Chem. Phys., 22, 12789–12802, https://doi.org/10.5194/acp-22-12789-2022, https://doi.org/10.5194/acp-22-12789-2022, 2022
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In this study, we report the long-term measurement of organic carbon (OC) and elementary carbon (EC) in PM2.5 with hourly time resolution conducted at a regional site in Shanghai from 2016 to 2020. The results from this study provide critical information about the long-term trend of carbonaceous aerosol, in particular secondary OC, in one of the largest megacities in the world and are helpful for developing pollution control measures from a long-term planning perspective.
Marta Via, Gang Chen, Francesco Canonaco, Kaspar R. Daellenbach, Benjamin Chazeau, Hasna Chebaicheb, Jianhui Jiang, Hannes Keernik, Chunshui Lin, Nicolas Marchand, Cristina Marin, Colin O'Dowd, Jurgita Ovadnevaite, Jean-Eudes Petit, Michael Pikridas, Véronique Riffault, Jean Sciare, Jay G. Slowik, Leïla Simon, Jeni Vasilescu, Yunjiang Zhang, Olivier Favez, André S. H. Prévôt, Andrés Alastuey, and María Cruz Minguillón
Atmos. Meas. Tech., 15, 5479–5495, https://doi.org/10.5194/amt-15-5479-2022, https://doi.org/10.5194/amt-15-5479-2022, 2022
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This work presents the differences resulting from two techniques (rolling and seasonal) of the positive matrix factorisation model that can be run for organic aerosol source apportionment. The current state of the art suggests that the rolling technique is more accurate, but no proof of its effectiveness has been provided yet. This paper tackles this issue in the context of a synthetic dataset and a multi-site real-world comparison.
Chao Yan, Yicheng Shen, Dominik Stolzenburg, Lubna Dada, Ximeng Qi, Simo Hakala, Anu-Maija Sundström, Yishuo Guo, Antti Lipponen, Tom V. Kokkonen, Jenni Kontkanen, Runlong Cai, Jing Cai, Tommy Chan, Liangduo Chen, Biwu Chu, Chenjuan Deng, Wei Du, Xiaolong Fan, Xu-Cheng He, Juha Kangasluoma, Joni Kujansuu, Mona Kurppa, Chang Li, Yiran Li, Zhuohui Lin, Yiliang Liu, Yuliang Liu, Yiqun Lu, Wei Nie, Jouni Pulliainen, Xiaohui Qiao, Yonghong Wang, Yifan Wen, Ye Wu, Gan Yang, Lei Yao, Rujing Yin, Gen Zhang, Shaojun Zhang, Feixue Zheng, Ying Zhou, Antti Arola, Johanna Tamminen, Pauli Paasonen, Yele Sun, Lin Wang, Neil M. Donahue, Yongchun Liu, Federico Bianchi, Kaspar R. Daellenbach, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Aijun Ding, Jingkun Jiang, and Markku Kulmala
Atmos. Chem. Phys., 22, 12207–12220, https://doi.org/10.5194/acp-22-12207-2022, https://doi.org/10.5194/acp-22-12207-2022, 2022
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Atmospheric new particle formation (NPF) is a dominant source of atmospheric ultrafine particles. In urban environments, traffic emissions are a major source of primary pollutants, but their contribution to NPF remains under debate. During the COVID-19 lockdown, traffic emissions were significantly reduced, providing a unique chance to examine their relevance to NPF. Based on our comprehensive measurements, we demonstrate that traffic emissions alone are not able to explain the NPF in Beijing.
Jing Duan, Ru-Jin Huang, Yifang Gu, Chunshui Lin, Haobin Zhong, Wei Xu, Quan Liu, Yan You, Jurgita Ovadnevaite, Darius Ceburnis, Thorsten Hoffmann, and Colin O'Dowd
Atmos. Chem. Phys., 22, 10139–10153, https://doi.org/10.5194/acp-22-10139-2022, https://doi.org/10.5194/acp-22-10139-2022, 2022
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Biomass-burning-influenced oxygenated organic aerosol (OOA-BB), formed from the photochemical oxidation and aging of biomass burning OA (BBOA), was resolved in urban Xi’an. The aqueous-phase processed oxygenated OA (aq-OOA) concentration was more dependent on secondary inorganic aerosol (SIA) content and aerosol liquid water content (ALWC). The increased aq-OOA contribution during SIA-enhanced periods likely reflects OA evolution due to the addition of alcohol or peroxide groups
Haobin Zhong, Ru-Jin Huang, Chunshui Lin, Wei Xu, Jing Duan, Yifang Gu, Wei Huang, Haiyan Ni, Chongshu Zhu, Yan You, Yunfei Wu, Renjian Zhang, Jurgita Ovadnevaite, Darius Ceburnis, and Colin D. O'Dowd
Atmos. Chem. Phys., 22, 9513–9524, https://doi.org/10.5194/acp-22-9513-2022, https://doi.org/10.5194/acp-22-9513-2022, 2022
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To investigate the physico-chemical properties of aerosol transported from major pollution regions in China, observations were conducted ~200 m above the ground at the junction location of the two key pollution areas. We found that the formation efficiency, oxidation state and production rate of secondary aerosol were different in the transport sectors from different pollution regions, and they were largely enhanced by the regional long-distance transport.
Lisa J. Beck, Siegfried Schobesberger, Heikki Junninen, Janne Lampilahti, Antti Manninen, Lubna Dada, Katri Leino, Xu-Cheng He, Iida Pullinen, Lauriane L. J. Quéléver, Anna Franck, Pyry Poutanen, Daniela Wimmer, Frans Korhonen, Mikko Sipilä, Mikael Ehn, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Jonathan Duplissy
Atmos. Chem. Phys., 22, 8547–8577, https://doi.org/10.5194/acp-22-8547-2022, https://doi.org/10.5194/acp-22-8547-2022, 2022
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The presented article introduces an overview of atmospheric ions and their composition above the boreal forest. We provide the results of an extensive airborne measurement campaign with an air ion mass spectrometer and particle measurements, showing their diurnal evolution within the boundary layer and free troposphere. In addition, we compare the airborne dataset with the co-located data from the ground at SMEAR II station, Finland.
Lauriane L. J. Quéléver, Lubna Dada, Eija Asmi, Janne Lampilahti, Tommy Chan, Jonathan E. Ferrara, Gustavo E. Copes, German Pérez-Fogwill, Luis Barreira, Minna Aurela, Douglas R. Worsnop, Tuija Jokinen, and Mikko Sipilä
Atmos. Chem. Phys., 22, 8417–8437, https://doi.org/10.5194/acp-22-8417-2022, https://doi.org/10.5194/acp-22-8417-2022, 2022
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Understanding how aerosols form is crucial for correctly modeling the climate and improving future predictions. This work provides extensive analysis of aerosol particles and their precursors at Marambio Station, Antarctic Peninsula. We show that sulfuric acid, ammonia, and dimethylamine are key contributors to the frequent new particle formation events observed at the site. We discuss nucleation mechanisms and highlight the need for targeted measurement to fully understand these processes.
Youwei Hong, Xinbei Xu, Dan Liao, Taotao Liu, Xiaoting Ji, Ke Xu, Chunyang Liao, Ting Wang, Chunshui Lin, and Jinsheng Chen
Atmos. Chem. Phys., 22, 7827–7841, https://doi.org/10.5194/acp-22-7827-2022, https://doi.org/10.5194/acp-22-7827-2022, 2022
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Secondary organic aerosol (SOA) simulation remains uncertain, due to the unknown SOA formation mechanisms. Aerosol samples with a 4 h time resolution were collected, along with online measurements of aerosol chemical compositions and meteorological parameters. We found that anthropogenic emissions, atmospheric oxidation capacity and halogen chemistry have significant effects on the formation of biogenic SOA (BSOA). The findings of this study are helpful to better explore the missed SOA sources.
Minxia Shen, Kin Fai Ho, Wenting Dai, Suixin Liu, Ting Zhang, Qiyuan Wang, Jingjing Meng, Judith C. Chow, John G. Watson, Junji Cao, and Jianjun Li
Atmos. Chem. Phys., 22, 7489–7504, https://doi.org/10.5194/acp-22-7489-2022, https://doi.org/10.5194/acp-22-7489-2022, 2022
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Looking at characteristics and δ13C compositions of dicarboxylic acids and related compounds in BB aerosols, we used a combined combustion and aging system to generate fresh and aged aerosols from burning straw. The results showed the emission factors (EFaged) of total diacids of aging experiments were around an order of magnitude higher than EFfresh. This meant that dicarboxylic acids are involved with secondary photochemical processes in the atmosphere rather than primary emissions from BB.
Reza Bashiri Khuzestani, Keren Liao, Ying Liu, Ruqian Miao, Yan Zheng, Xi Cheng, Tianjiao Jia, Xin Li, Shiyi Chen, Guancong Huang, and Qi Chen
Atmos. Chem. Phys., 22, 7389–7404, https://doi.org/10.5194/acp-22-7389-2022, https://doi.org/10.5194/acp-22-7389-2022, 2022
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This work characterized the spatial variabilities of air pollutants in a megacity by advanced mobile measurements. The results show a large spatial heterogeneity in the distributions of PM2.5 composition and volatile organic compounds under non-haze conditions, and relatively uniform spatial distributions under haze conditions that may indicate a chemical homogeneity on an intracity scale. The findings improve our understanding of urban air pollution.
Mikko Sipilä, Nina Sarnela, Kimmo Neitola, Totti Laitinen, Deniz Kemppainen, Lisa Beck, Ella-Maria Duplissy, Salla Kuittinen, Tuuli Lehmusjärvi, Janne Lampilahti, Veli-Matti Kerminen, Katrianne Lehtipalo, Pasi P. Aalto, Petri Keronen, Erkki Siivola, Pekka A. Rantala, Douglas R. Worsnop, Markku Kulmala, Tuija Jokinen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 17559–17576, https://doi.org/10.5194/acp-21-17559-2021, https://doi.org/10.5194/acp-21-17559-2021, 2021
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Metallurgical industry in Kola peninsula is a large source of air pollution in the (sub-)Arctic domain. Sulfur dioxide emissions from the ore smelters are transported across large areas. We investigated sulfur dioxide and its transformation to sulfuric acid aerosol particles during winter months in Finnish Lapland, close to Kola industrial areas. We observed intense formation of new aerosol particles despite the low solar radiation intensity, often required for new particle formation elsewhere.
Ruqian Miao, Qi Chen, Manish Shrivastava, Youfan Chen, Lin Zhang, Jianlin Hu, Yan Zheng, and Keren Liao
Atmos. Chem. Phys., 21, 16183–16201, https://doi.org/10.5194/acp-21-16183-2021, https://doi.org/10.5194/acp-21-16183-2021, 2021
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We apply process-based and observation-constrained schemes to simulate organic aerosol in China and conduct comprehensive model–observation comparisons. The results show that anthropogenic semivolatile and intermediate-volatility organic compounds (SVOCs and IVOCs) are the main sources of secondary organic aerosol (SOA) in polluted regions, for which the residential sector is perhaps the predominant contributor. The hydroxyl radical level is also important for SOA modeling in polluted regions.
Chunshui Lin, Darius Ceburnis, Anna Trubetskaya, Wei Xu, William Smith, Stig Hellebust, John Wenger, Colin O'Dowd, and Jurgita Ovadnevaite
Atmos. Meas. Tech., 14, 6905–6916, https://doi.org/10.5194/amt-14-6905-2021, https://doi.org/10.5194/amt-14-6905-2021, 2021
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Source apportionment of solid-fuel-burning emissions can be complicated by the use of different fuels, stoves, and burning conditions. Here, the organic aerosol mass spectra produced from burning a range of solid fuels in several stoves were compared. This study accounts for the source variability and provides better constraints on the primary factor contributions to the ambient organic aerosol estimations, holding significant implications for public health and policymakers.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
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Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
Yuliang Liu, Wei Nie, Yuanyuan Li, Dafeng Ge, Chong Liu, Zhengning Xu, Liangduo Chen, Tianyi Wang, Lei Wang, Peng Sun, Ximeng Qi, Jiaping Wang, Zheng Xu, Jian Yuan, Chao Yan, Yanjun Zhang, Dandan Huang, Zhe Wang, Neil M. Donahue, Douglas Worsnop, Xuguang Chi, Mikael Ehn, and Aijun Ding
Atmos. Chem. Phys., 21, 14789–14814, https://doi.org/10.5194/acp-21-14789-2021, https://doi.org/10.5194/acp-21-14789-2021, 2021
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Oxygenated organic molecules (OOMs) are crucial intermediates linking volatile organic compounds to secondary organic aerosols. Using nitrate time-of-flight chemical ionization mass spectrometry in eastern China, we performed positive matrix factorization (PMF) on binned OOM mass spectra. We reconstructed over 1000 molecules from 14 derived PMF factors and identified about 72 % of the observed OOMs as organic nitrates, highlighting the decisive role of NOx in OOM formation in populated areas.
Alexandra Gutmann, Nicole Bobrowski, Marcello Liotta, and Thorsten Hoffmann
Atmos. Meas. Tech., 14, 6395–6406, https://doi.org/10.5194/amt-14-6395-2021, https://doi.org/10.5194/amt-14-6395-2021, 2021
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Motivated by a special interest in bromine chemistry in volcanic plumes, the study presented here describes a new method for the quantitative collection of gaseous hydrogen bromide in gas diffusion denuders. The hydrogen bromide reacted during sampling with appropriate epoxides applied to the denuder walls. The denuder sampling assembly was successfully deployed in the volcanic plume of Masaya volcano, Nicaragua.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Gloria Titos, María A. Burgos, Paul Zieger, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Ernest Weingartner, Bas Henzing, Krista Luoma, Colin O'Dowd, Alfred Wiedensohler, and Elisabeth Andrews
Atmos. Chem. Phys., 21, 13031–13050, https://doi.org/10.5194/acp-21-13031-2021, https://doi.org/10.5194/acp-21-13031-2021, 2021
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This paper investigates the impact of water uptake on aerosol optical properties, in particular the aerosol light-scattering coefficient. Although in situ measurements are performed at low relative humidity (typically at
RH < 40 %), to address the climatic impact of aerosol particles it is necessary to take into account the effect that water uptake may have on the aerosol optical properties.
Xi Cheng, Qi Chen, Yong Jie Li, Yan Zheng, Keren Liao, and Guancong Huang
Atmos. Chem. Phys., 21, 12005–12019, https://doi.org/10.5194/acp-21-12005-2021, https://doi.org/10.5194/acp-21-12005-2021, 2021
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In this study, we conducted laboratory studies to investigate the formation of gas-phase highly oxygenated organic molecules (HOMs). We provide a thorough analysis on the importance of multistep auto-oxidation and multigeneration OH reactions. We also give an intensive investigation on the roles of high-NO2 conditions that represent a wide range of anthropogenically influenced environments.
Xiaolong Fan, Jing Cai, Chao Yan, Jian Zhao, Yishuo Guo, Chang Li, Kaspar R. Dällenbach, Feixue Zheng, Zhuohui Lin, Biwu Chu, Yonghong Wang, Lubna Dada, Qiaozhi Zha, Wei Du, Jenni Kontkanen, Theo Kurtén, Siddhart Iyer, Joni T. Kujansuu, Tuukka Petäjä, Douglas R. Worsnop, Veli-Matti Kerminen, Yongchun Liu, Federico Bianchi, Yee Jun Tham, Lei Yao, and Markku Kulmala
Atmos. Chem. Phys., 21, 11437–11452, https://doi.org/10.5194/acp-21-11437-2021, https://doi.org/10.5194/acp-21-11437-2021, 2021
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We observed significant concentrations of gaseous HBr and HCl throughout the winter and springtime in urban Beijing, China. Our results indicate that gaseous HCl and HBr are most likely originated from anthropogenic emissions such as burning activities, and the gas–aerosol partitioning may play a crucial role in contributing to the gaseous HCl and HBr. These observations suggest that there is an important recycling pathway of halogen species in inland megacities.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Gang Chen, Olga Garmash, Diego Aliaga, Frans Graeffe, Meri Räty, Krista Luoma, Pasi Aalto, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 21, 10081–10109, https://doi.org/10.5194/acp-21-10081-2021, https://doi.org/10.5194/acp-21-10081-2021, 2021
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In many locations worldwide aerosol particles have been shown to be made up of organic aerosol (OA). The boreal forest is a region where aerosol particles possess a high OA mass fraction. Here, we studied OA composition using the longest time series of OA composition ever obtained from a boreal environment. For this purpose, we tested a new analysis framework and discovered that most of the OA was highly oxidized, with strong seasonal behaviour reflecting different sources in summer and winter.
Yandong Tong, Veronika Pospisilova, Lu Qi, Jing Duan, Yifang Gu, Varun Kumar, Pragati Rai, Giulia Stefenelli, Liwei Wang, Ying Wang, Haobin Zhong, Urs Baltensperger, Junji Cao, Ru-Jin Huang, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 21, 9859–9886, https://doi.org/10.5194/acp-21-9859-2021, https://doi.org/10.5194/acp-21-9859-2021, 2021
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We investigate SOA sources and formation processes by a field deployment of the EESI-TOF-MS and L-TOF AMS in Beijing in late autumn and early winter. Our study shows that the sources and processes giving rise to haze events in Beijing are variable and seasonally dependent: (1) in the heating season, SOA formation is driven by oxidation of aromatics from solid fuel combustion; and (2) under high-NOx and RH conditions, aqueous-phase chemistry can be a major contributor to SOA formation.
Xu Feng, Haipeng Lin, Tzung-May Fu, Melissa P. Sulprizio, Jiawei Zhuang, Daniel J. Jacob, Heng Tian, Yaping Ma, Lijuan Zhang, Xiaolin Wang, Qi Chen, and Zhiwei Han
Geosci. Model Dev., 14, 3741–3768, https://doi.org/10.5194/gmd-14-3741-2021, https://doi.org/10.5194/gmd-14-3741-2021, 2021
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WRF-GC is an online coupling of the WRF meteorological model and GEOS-Chem chemical transport model for regional atmospheric chemistry and air quality modeling. In WRF-GC v2.0, we implemented the aerosol–radiation interactions and aerosol–cloud interactions, as well as the capability to nest multiple domains for high-resolution simulations based on the modular framework of WRF-GC v1.0. This allows the GEOS-Chem users to investigate the meteorology–atmospheric chemistry interactions.
Kai Wang, Ru-Jin Huang, Martin Brüggemann, Yun Zhang, Lu Yang, Haiyan Ni, Jie Guo, Meng Wang, Jiajun Han, Merete Bilde, Marianne Glasius, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 9089–9104, https://doi.org/10.5194/acp-21-9089-2021, https://doi.org/10.5194/acp-21-9089-2021, 2021
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Here we present the detailed molecular composition of the organic aerosol collected in three eastern Chinese cities from north to south, Changchun, Shanghai and Guangzhou, by applying LC–Orbitrap analysis. Accordingly, the aromaticity degree of chemical compounds decreases from north to south, while the oxidation degree increases from north to south, which can be explained by the different anthropogenic emissions and photochemical oxidation processes.
Bo Galle, Santiago Arellano, Nicole Bobrowski, Vladimir Conde, Tobias P. Fischer, Gustav Gerdes, Alexandra Gutmann, Thorsten Hoffmann, Ima Itikarai, Tomas Krejci, Emma J. Liu, Kila Mulina, Scott Nowicki, Tom Richardson, Julian Rüdiger, Kieran Wood, and Jiazhi Xu
Atmos. Meas. Tech., 14, 4255–4277, https://doi.org/10.5194/amt-14-4255-2021, https://doi.org/10.5194/amt-14-4255-2021, 2021
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Measurements of volcanic gases are important for geophysical research, risk assessment and environmental impact studies. Some gases, like SO2 and BrO, may be studied from the ground at a safe distance using remote sensing techniques. Many other gases require in situ access to the gas plume. Here, a drone may be an attractive alternative. This paper describes a drone specially adapted for volcanic gas studies and demonstrates its use in a field campaign at Manam volcano in Papua New Guinea.
Wei Xu, Kirsten N. Fossum, Jurgita Ovadnevaite, Chunshui Lin, Ru-Jin Huang, Colin O'Dowd, and Darius Ceburnis
Atmos. Chem. Phys., 21, 8655–8675, https://doi.org/10.5194/acp-21-8655-2021, https://doi.org/10.5194/acp-21-8655-2021, 2021
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Cloud condensation nuclei (CCN) are an important topic in atmospheric studies, especially for evaluating the climate impact of aerosol. Here in this study, CCN closure is studied by using chemical composition based on an aerosol mass spectrometer (AMS) and hygroscopicity growth measurements based on a humidified tandem differential mobility analyzer (HTDMA) at the Mace Head atmospheric research station.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys., 21, 8455–8478, https://doi.org/10.5194/acp-21-8455-2021, https://doi.org/10.5194/acp-21-8455-2021, 2021
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We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 3895–3907, https://doi.org/10.5194/amt-14-3895-2021, https://doi.org/10.5194/amt-14-3895-2021, 2021
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Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
Weiqi Xu, Masayuki Takeuchi, Chun Chen, Yanmei Qiu, Conghui Xie, Wanyun Xu, Nan Ma, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Meas. Tech., 14, 3693–3705, https://doi.org/10.5194/amt-14-3693-2021, https://doi.org/10.5194/amt-14-3693-2021, 2021
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Here we developed a method for estimation of particulate organic nitrates (pON) from the measurements of a high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally had improvements in reducing negative values due to the influences of a high concentration of inorganic nitrate and a constant ratio of NO+ to NO2+ of organic nitrates (RON).
Chao Peng, Patricia N. Razafindrambinina, Kotiba A. Malek, Lanxiadi Chen, Weigang Wang, Ru-Jin Huang, Yuqing Zhang, Xiang Ding, Maofa Ge, Xinming Wang, Akua A. Asa-Awuku, and Mingjin Tang
Atmos. Chem. Phys., 21, 7135–7148, https://doi.org/10.5194/acp-21-7135-2021, https://doi.org/10.5194/acp-21-7135-2021, 2021
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Organosulfates are important constituents in tropospheric aerosol particles, but their hygroscopic properties and cloud condensation nuclei activities are not well understood. In our work, three complementary techniques were employed to investigate the interactions of 11 organosulfates with water vapor under sub- and supersaturated conditions.
Inken Heidke, Adam Hartland, Denis Scholz, Andrew Pearson, John Hellstrom, Sebastian F. M. Breitenbach, and Thorsten Hoffmann
Biogeosciences, 18, 2289–2300, https://doi.org/10.5194/bg-18-2289-2021, https://doi.org/10.5194/bg-18-2289-2021, 2021
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We analyzed lignin oxidation products (LOPs) in leaf litter and different soil horizons as well as dripwater and flowstone samples from four different cave sites from different vegetation zones in New Zealand using liquid chromatography coupled to mass spectrometry. We test whether the original source-dependent LOP signal of the overlying vegetation is preserved and can be recovered from flowstone samples and investigate how the signal is altered by the transport from the soil to the cave.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Mengdi Song, Xin Li, Suding Yang, Xuena Yu, Songxiu Zhou, Yiming Yang, Shiyi Chen, Huabin Dong, Keren Liao, Qi Chen, Keding Lu, Ningning Zhang, Junji Cao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 4939–4958, https://doi.org/10.5194/acp-21-4939-2021, https://doi.org/10.5194/acp-21-4939-2021, 2021
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Due to their lower diffusion capacities and higher conversion capacities, urban areas in Xi’an experienced severe ozone pollution in the summer. In this study, a campaign of comprehensive field observations and VOC grid sampling was conducted in Xi’an from 20 June to 20 July 2019. We found that Xi'an has a strong local emission source of VOCs, and vehicle exhaust was the primary VOC source. In addition, alkenes, aromatics, and oxygenated VOCs played a dominant role in secondary transformations.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
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For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
Wei Yuan, Ru-Jin Huang, Lu Yang, Ting Wang, Jing Duan, Jie Guo, Haiyan Ni, Yang Chen, Qi Chen, Yongjie Li, Ulrike Dusek, Colin O'Dowd, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3685–3697, https://doi.org/10.5194/acp-21-3685-2021, https://doi.org/10.5194/acp-21-3685-2021, 2021
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We characterized the seasonal variations in nitrated aromatic compounds (NACs) in composition, sources, and their light absorption contribution to brown carbon (BrC) aerosol in Xi'an, Northwest China. Our results show that secondary formation and vehicular emission were dominant sources in summer (~80 %), and biomass burning and coal combustion were major sources in winter (~75 %), and they indicate that the composition and sources of NACs have a profound impact on the light absorption of BrC
Julian Rüdiger, Alexandra Gutmann, Nicole Bobrowski, Marcello Liotta, J. Maarten de Moor, Rolf Sander, Florian Dinger, Jan-Lukas Tirpitz, Martha Ibarra, Armando Saballos, María Martínez, Elvis Mendoza, Arnoldo Ferrufino, John Stix, Juan Valdés, Jonathan M. Castro, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3371–3393, https://doi.org/10.5194/acp-21-3371-2021, https://doi.org/10.5194/acp-21-3371-2021, 2021
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We present an innovative approach to study halogen chemistry in the plume of Masaya volcano in Nicaragua. An unique data set was collected using multiple techniques, including drones. These data enabled us to determine the fraction of activation of the respective halogens at various plume ages, where in-mixing of ambient air causes chemical reactions. An atmospheric chemistry box model was employed to further examine the field results and help our understanding of volcanic plume chemistry.
Runlong Cai, Chao Yan, Dongsen Yang, Rujing Yin, Yiqun Lu, Chenjuan Deng, Yueyun Fu, Jiaxin Ruan, Xiaoxiao Li, Jenni Kontkanen, Qiang Zhang, Juha Kangasluoma, Yan Ma, Jiming Hao, Douglas R. Worsnop, Federico Bianchi, Pauli Paasonen, Veli-Matti Kerminen, Yongchun Liu, Lin Wang, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 21, 2457–2468, https://doi.org/10.5194/acp-21-2457-2021, https://doi.org/10.5194/acp-21-2457-2021, 2021
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Based on long-term measurements, we discovered that the collision of H2SO4–amine clusters is the governing mechanism that initializes fast new particle formation in the polluted atmospheric environment of urban Beijing. The mechanism and the governing factors for H2SO4–amine nucleation in the polluted atmosphere are quantitatively investigated in this study.
Francesco Canonaco, Anna Tobler, Gang Chen, Yulia Sosedova, Jay Gates Slowik, Carlo Bozzetti, Kaspar Rudolf Daellenbach, Imad El Haddad, Monica Crippa, Ru-Jin Huang, Markus Furger, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Meas. Tech., 14, 923–943, https://doi.org/10.5194/amt-14-923-2021, https://doi.org/10.5194/amt-14-923-2021, 2021
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Long-term ambient aerosol mass spectrometric data were analyzed with a statistical model (PMF) to obtain source contributions and fingerprints. The new aspects of this paper involve time-dependent source fingerprints by a rolling technique and the replacement of the full visual inspection of each run by a user-defined set of criteria to monitor the quality of each of these runs more efficiently. More reliable sources will finally provide better instruments for political mitigation strategies.
Huikun Liu, Qiyuan Wang, Li Xing, Yong Zhang, Ting Zhang, Weikang Ran, and Junji Cao
Atmos. Chem. Phys., 21, 973–987, https://doi.org/10.5194/acp-21-973-2021, https://doi.org/10.5194/acp-21-973-2021, 2021
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We conducted black carbon (BC) source apportionment on the southeastern Tibetan Plateau (TP) by an improved aethalometer model with the site-dependent Ångström exponent and BC mass absorption cross section (MAC). The result shows that the biomass-burning BC on the TP is slightly higher than fossil fuel BC, mainly from cross-border transportation instead of the local region, and the BC radiative effect is lower than that in the southwestern Himalaya but higher than that on the northeastern TP.
Pragati Rai, Jay G. Slowik, Markus Furger, Imad El Haddad, Suzanne Visser, Yandong Tong, Atinderpal Singh, Günther Wehrle, Varun Kumar, Anna K. Tobler, Deepika Bhattu, Liwei Wang, Dilip Ganguly, Neeraj Rastogi, Ru-Jin Huang, Jaroslaw Necki, Junji Cao, Sachchida N. Tripathi, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 717–730, https://doi.org/10.5194/acp-21-717-2021, https://doi.org/10.5194/acp-21-717-2021, 2021
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We present a simple conceptual framework based on elemental size distributions and enrichment factors that allows for a characterization of major sources, site-to-site similarities, and local differences and the identification of key information required for efficient policy development. Absolute concentrations are by far the highest in Delhi, followed by Beijing, and then the European cities.
Arttu Ylisirniö, Luis M. F. Barreira, Iida Pullinen, Angela Buchholz, John Jayne, Jordan E. Krechmer, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Meas. Tech., 14, 355–367, https://doi.org/10.5194/amt-14-355-2021, https://doi.org/10.5194/amt-14-355-2021, 2021
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FIGAERO-ToF-CIMS enables online volatility measurements of chemical compounds in ambient aerosols. Previously published volatility calibration results however differ from each other significantly. In this study we investigate the reason for this discrepancy. We found a major source of error in the widely used syringe deposition method and propose a new method for volatility calibration by using atomized calibration compounds.
Megan S. Claflin, Demetrios Pagonis, Zachary Finewax, Anne V. Handschy, Douglas A. Day, Wyatt L. Brown, John T. Jayne, Douglas R. Worsnop, Jose L. Jimenez, Paul J. Ziemann, Joost de Gouw, and Brian M. Lerner
Atmos. Meas. Tech., 14, 133–152, https://doi.org/10.5194/amt-14-133-2021, https://doi.org/10.5194/amt-14-133-2021, 2021
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We have developed a field-deployable gas chromatograph with thermal desorption preconcentration and detector switching between two high-resolution mass spectrometers for in situ measurements of volatile organic compounds (VOCs). This system combines chromatography with both proton transfer and electron ionization to offer fast time response and continuous molecular speciation. This technique was applied during the 2018 ATHLETIC campaign to characterize VOC emissions in an indoor environment.
Haiyan Ni, Ru-Jin Huang, Max M. Cosijn, Lu Yang, Jie Guo, Junji Cao, and Ulrike Dusek
Atmos. Chem. Phys., 20, 16041–16053, https://doi.org/10.5194/acp-20-16041-2020, https://doi.org/10.5194/acp-20-16041-2020, 2020
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We investigated sources of carbonaceous aerosols in Beijing and Xi'an during severe winter haze. Elemental carbon (EC) was dominated by vehicle emissions in Xi’an and coal burning in Beijing. Organic carbon (OC) increment during haze days was driven by the increase in primary and secondary OC (SOC). SOC was more from fossil sources in Beijing than Xi’an, especially during haze days. In Xi’an, no strong day–night differences in EC or OC sources suggest a large accumulation of particles.
Qiyuan Wang, Huikun Liu, Ping Wang, Wenting Dai, Ting Zhang, Youzhi Zhao, Jie Tian, Wenyan Zhang, Yongming Han, and Junji Cao
Atmos. Chem. Phys., 20, 15537–15549, https://doi.org/10.5194/acp-20-15537-2020, https://doi.org/10.5194/acp-20-15537-2020, 2020
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Light-absorbing carbonaceous (LAC) aerosol is an important influencing factor for global climate forcing. In this study, we used a receptor model coupling multi-wavelength absorption with chemical species to explore the source-specific LAC optical properties at a tropical marine monsoon climate zone. The results can improve our understanding of the LAC radiative effects caused by ship emissions.
Qiyuan Wang, Li Li, Jiamao Zhou, Jianhuai Ye, Wenting Dai, Huikun Liu, Yong Zhang, Renjian Zhang, Jie Tian, Yang Chen, Yunfei Wu, Weikang Ran, and Junji Cao
Atmos. Chem. Phys., 20, 15427–15442, https://doi.org/10.5194/acp-20-15427-2020, https://doi.org/10.5194/acp-20-15427-2020, 2020
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Recently, China has promulgated a series of regulations to reduce air pollutants. The decreased black carbon (BC) and co-emitted pollutants could affect the interactions between BC and other aerosols, which in turn results in changes in BC. Herein, we re-assessed the characteristics of BC of a representative pollution site in northern China in the final year of the Chinese
Action Plan for the Prevention and Control of Air Pollution.
Liqing Hao, Eetu Kari, Ari Leskinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 20, 14393–14405, https://doi.org/10.5194/acp-20-14393-2020, https://doi.org/10.5194/acp-20-14393-2020, 2020
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Our work presents the observational results of secondary organic aerosol (SOA) formation in the presence of ammonia. The particle-phase ammonium was continuously produced even after SOA formation had ceased. The gas-phase organic acids were observed to contribute to the formed particle-phase ammonium salts. This study suggests that the presence of ammonia may change the mass and chemical composition of large-size SOA particles and can potentially alter the aerosol impact on climate change.
Jingsha Xu, Shaojie Song, Roy M. Harrison, Congbo Song, Lianfang Wei, Qiang Zhang, Yele Sun, Lu Lei, Chao Zhang, Xiaohong Yao, Dihui Chen, Weijun Li, Miaomiao Wu, Hezhong Tian, Lining Luo, Shengrui Tong, Weiran Li, Junling Wang, Guoliang Shi, Yanqi Huangfu, Yingze Tian, Baozhu Ge, Shaoli Su, Chao Peng, Yang Chen, Fumo Yang, Aleksandra Mihajlidi-Zelić, Dragana Đorđević, Stefan J. Swift, Imogen Andrews, Jacqueline F. Hamilton, Ye Sun, Agung Kramawijaya, Jinxiu Han, Supattarachai Saksakulkrai, Clarissa Baldo, Siqi Hou, Feixue Zheng, Kaspar R. Daellenbach, Chao Yan, Yongchun Liu, Markku Kulmala, Pingqing Fu, and Zongbo Shi
Atmos. Meas. Tech., 13, 6325–6341, https://doi.org/10.5194/amt-13-6325-2020, https://doi.org/10.5194/amt-13-6325-2020, 2020
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An interlaboratory comparison was conducted for the first time to examine differences in water-soluble inorganic ions (WSIIs) measured by 10 labs using ion chromatography (IC) and by two online aerosol chemical speciation monitor (ACSM) methods. Major ions including SO42−, NO3− and NH4+ agreed well in 10 IC labs and correlated well with ACSM data. WSII interlab variability strongly affected aerosol acidity results based on ion balance, but aerosol pH computed by ISORROPIA II was very similar.
Chao Peng, Yu Wang, Zhijun Wu, Lanxiadi Chen, Ru-Jin Huang, Weigang Wang, Zhe Wang, Weiwei Hu, Guohua Zhang, Maofa Ge, Min Hu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13877–13903, https://doi.org/10.5194/acp-20-13877-2020, https://doi.org/10.5194/acp-20-13877-2020, 2020
Jing Cai, Biwu Chu, Lei Yao, Chao Yan, Liine M. Heikkinen, Feixue Zheng, Chang Li, Xiaolong Fan, Shaojun Zhang, Daoyuan Yang, Yonghong Wang, Tom V. Kokkonen, Tommy Chan, Ying Zhou, Lubna Dada, Yongchun Liu, Hong He, Pauli Paasonen, Joni T. Kujansuu, Tuukka Petäjä, Claudia Mohr, Juha Kangasluoma, Federico Bianchi, Yele Sun, Philip L. Croteau, Douglas R. Worsnop, Veli-Matti Kerminen, Wei Du, Markku Kulmala, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 20, 12721–12740, https://doi.org/10.5194/acp-20-12721-2020, https://doi.org/10.5194/acp-20-12721-2020, 2020
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By applying both OA PMF and size PMF at the same urban measurement site in Beijing, similar particle source types, including vehicular emissions, cooking emissions and secondary formation-related sources, were resolved by both frameworks and agreed well. It is also found that in the absence of new particle formation, vehicular and cooking emissions dominate the particle number concentration, while secondary particulate matter governed PM2.5 mass during spring and summer in Beijing.
Marcel Weloe and Thorsten Hoffmann
Atmos. Meas. Tech., 13, 5725–5738, https://doi.org/10.5194/amt-13-5725-2020, https://doi.org/10.5194/amt-13-5725-2020, 2020
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Aerosol mass spectrometers (AMSs) are frequently applied in atmospheric aerosol research in connection with climate, environmental or health-related projects. The paper describes a new real-time technique for the measurement of organic peroxides, which play an important role in new particle formation and as
reactive oxygen speciesin aerosol–health-related aspects of atmospheric aerosols.
Ruqian Miao, Qi Chen, Yan Zheng, Xi Cheng, Yele Sun, Paul I. Palmer, Manish Shrivastava, Jianping Guo, Qiang Zhang, Yuhan Liu, Zhaofeng Tan, Xuefei Ma, Shiyi Chen, Limin Zeng, Keding Lu, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 12265–12284, https://doi.org/10.5194/acp-20-12265-2020, https://doi.org/10.5194/acp-20-12265-2020, 2020
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In this study we evaluated the model performances for simulating secondary inorganic aerosol (SIA) and organic aerosol (OA) in PM2.5 in China against comprehensive datasets. The potential biases from factors related to meteorology, emission, chemistry, and atmospheric removal are systematically investigated. This study provides a comprehensive understanding of modeling PM2.5, which is important for studies on the effectiveness of emission control strategies.
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Short summary
We characterized secondary aerosol formation in Beijing. Our results showed that relative humidity (RH) and Ox have opposite effects on sulfate and nitrate formation in summer and winter. The wintertime more-oxidized OOA (MO-OOA) showed a good correlation with aerosol liquid water content (ALWC). Meanwhile, the dependence of less-oxidized OOA (LO-OOA) and the mass ratio of LO-OOA to MO-OOA in Ox both degraded when RH > 60 %, suggesting that RH or ALWC may also affect LO-OOA formation.
We characterized secondary aerosol formation in Beijing. Our results showed that relative...
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