Articles | Volume 24, issue 23
https://doi.org/10.5194/acp-24-13793-2024
© Author(s) 2024. 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-24-13793-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
12 Dec 2024
Research article |
| 12 Dec 2024
| 12 Dec 2024
Molecular and seasonal characteristics of organic vapors in urban Beijing: insights from Vocus-PTR measurements
Zhaojin An
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, 100084, Beijing, China
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
Rujing Yin
Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, 116024, Dalian, China
Xinyan Zhao
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, 100084, Beijing, China
Xiaoxiao Li
School of Resource and Environmental Sciences, Wuhan University, 430072, Wuhan, China
Yuyang Li
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, 100084, Beijing, China
Yi Yuan
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, 100084, Beijing, China
Junchen Guo
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, 100084, Beijing, China
Yiqi Zhao
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, 100084, Beijing, China
School of Environment, Henan Normal University, 453007, Xinxiang, China
Dandan Li
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, 100084, Beijing, China
Yaowei Li
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
Dongbin Wang
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, 100084, Beijing, China
Joint International Research Laboratory of Atmospheric and Earth System Research, School of Atmospheric Sciences, Nanjing University, 210023, Nanjing, China
Kebin He
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, 100084, Beijing, China
Douglas R. Worsnop
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki 00014, Finland
Aerodyne Research, Inc., Billerica, MA 01821, USA
Frank N. Keutsch
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
Jingkun Jiang
CORRESPONDING AUTHOR
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, 100084, Beijing, China
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Earth Syst. Sci. Data, 16, 4497–4509, https://doi.org/10.5194/essd-16-4497-2024, https://doi.org/10.5194/essd-16-4497-2024, 2024
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Jiewen Shen, Bin Zhao, Shuxiao Wang, An Ning, Yuyang Li, Runlong Cai, Da Gao, Biwu Chu, Yang Gao, Manish Shrivastava, Jingkun Jiang, Xiuhui Zhang, and Hong He
Atmos. Chem. Phys., 24, 10261–10278, https://doi.org/10.5194/acp-24-10261-2024, https://doi.org/10.5194/acp-24-10261-2024, 2024
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Dandan Li, Dongyu Wang, Lucia Caudillo, Wiebke Scholz, Mingyi Wang, Sophie Tomaz, Guillaume Marie, Mihnea Surdu, Elias Eccli, Xianda Gong, Loic Gonzalez-Carracedo, Manuel Granzin, Joschka Pfeifer, Birte Rörup, Benjamin Schulze, Pekka Rantala, Sébastien Perrier, Armin Hansel, Joachim Curtius, Jasper Kirkby, Neil M. Donahue, Christian George, Imad El-Haddad, and Matthieu Riva
Atmos. Meas. Tech., 17, 5413–5428, https://doi.org/10.5194/amt-17-5413-2024, https://doi.org/10.5194/amt-17-5413-2024, 2024
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Due to the analytical challenges of measuring organic vapors, it remains challenging to identify and quantify organic molecules present in the atmosphere. Here, we explore the performance of the Orbitrap chemical ionization mass spectrometer (CI-Orbitrap) using ammonium ion chemistry. This study shows that ammonium-ion-based chemistry associated with the high mass resolution of the Orbitrap mass analyzer can measure almost all inclusive compounds.
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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Yusheng Zhang, Feixue Zheng, Zemin Feng, Chaofan Lian, Weigang Wang, Xiaolong Fan, Wei Ma, Zhuohui Lin, Chang Li, Gen Zhang, Chao Yan, Ying Zhang, Veli-Matti Kerminen, Federico Bianch, Tuukka Petäjä, Juha Kangasluoma, Markku Kulmala, and Yongchun Liu
Atmos. Chem. Phys., 24, 8569–8587, https://doi.org/10.5194/acp-24-8569-2024, https://doi.org/10.5194/acp-24-8569-2024, 2024
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The nitrous acid (HONO) budget was validated during a COVID-19 lockdown event. The main conclusions are (1) HONO concentrations showed a significant decrease from 0.97 to 0.53 ppb during lockdown; (2) vehicle emissions accounted for 53 % of nighttime sources, with the heterogeneous conversion of NO2 on ground surfaces more important than aerosol; and (3) the dominant daytime source shifted from the homogenous reaction between NO and OH (51 %) to nitrate photolysis (53 %) during lockdown.
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.
Nana Wu, Guannan Geng, Ruochong Xu, Shigan Liu, Xiaodong Liu, Qinren Shi, Ying Zhou, Yu Zhao, Huan Liu, Yu Song, Junyu Zheng, Qiang Zhang, and Kebin He
Earth Syst. Sci. Data, 16, 2893–2915, https://doi.org/10.5194/essd-16-2893-2024, https://doi.org/10.5194/essd-16-2893-2024, 2024
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The commonly used method for developing large-scale air pollutant emission datasets for China faces challenges due to limited availability of detailed parameter information. In this study, we develop an efficient integrated framework to gather such information by harmonizing seven heterogeneous inventories from five research institutions. Emission characterizations are analyzed and validated, demonstrating that the dataset provides more accurate emission magnitudes and spatiotemporal patterns.
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.
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.
Shiyi Lai, Ximeng Qi, Xin Huang, Sijia Lou, Xuguang Chi, Liangduo Chen, Chong Liu, Yuliang Liu, Chao Yan, Mengmeng Li, Tengyu Liu, Wei Nie, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Aijun Ding
Atmos. Chem. Phys., 24, 2535–2553, https://doi.org/10.5194/acp-24-2535-2024, https://doi.org/10.5194/acp-24-2535-2024, 2024
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By combining in situ measurements and chemical transport modeling, this study investigates new particle formation (NPF) on the southeastern Tibetan Plateau. We found that the NPF was driven by the presence of biogenic gases and the transport of anthropogenic precursors. The NPF was vertically heterogeneous and shaped by the vertical mixing. This study highlights the importance of anthropogenic–biogenic interactions and meteorological dynamics in NPF in this climate-sensitive region.
Ying Zhang, Duzitian Li, Xu-Cheng He, Wei Nie, Chenjuan Deng, Runlong Cai, Yuliang Liu, Yishuo Guo, Chong Liu, Yiran Li, Liangduo Chen, Yuanyuan Li, Chenjie Hua, Tingyu Liu, Zongcheng Wang, Jiali Xie, Lei Wang, Tuukka Petäjä, Federico Bianchi, Ximeng Qi, Xuguang Chi, Pauli Paasonen, Yongchun Liu, Chao Yan, Jingkun Jiang, Aijun Ding, and Markku Kulmala
Atmos. Chem. Phys., 24, 1873–1893, https://doi.org/10.5194/acp-24-1873-2024, https://doi.org/10.5194/acp-24-1873-2024, 2024
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This study conducts a long-term observation of gaseous iodine oxoacids in two Chinese megacities, revealing their ubiquitous presence with peak concentrations (up to 0.1 pptv) in summer. Our analysis suggests a mix of terrestrial and marine sources for iodine. Additionally, iodic acid is identified as a notable contributor to sub-3 nm particle growth and particle survival probability.
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.
Yaowei Li, Corey Pedersen, John Dykema, Jean-Paul Vernier, Sandro Vattioni, Amit Kumar Pandit, Andrea Stenke, Elizabeth Asher, Troy Thornberry, Michael A. Todt, Thao Paul Bui, Jonathan Dean-Day, and Frank N. Keutsch
Atmos. Chem. Phys., 23, 15351–15364, https://doi.org/10.5194/acp-23-15351-2023, https://doi.org/10.5194/acp-23-15351-2023, 2023
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In 2021, the eruption of La Soufrière released sulfur dioxide into the stratosphere, resulting in a spread of volcanic aerosol over the Northern Hemisphere. We conducted extensive aircraft and balloon-borne measurements after that, revealing enhanced particle concentration and altered size distribution due to the eruption. The eruption's impact on ozone depletion was minimal, contributing ~0.6 %, and its global radiative forcing effect was modest, mainly affecting tropical and midlatitude areas.
Markku Kulmala, Anna Lintunen, Hanna Lappalainen, Annele Virtanen, Chao Yan, Ekaterina Ezhova, Tuomo Nieminen, Ilona Riipinen, Risto Makkonen, Johanna Tamminen, Anu-Maija Sundström, Antti Arola, Armin Hansel, Kari Lehtinen, Timo Vesala, Tuukka Petäjä, Jaana Bäck, Tom Kokkonen, and Veli-Matti Kerminen
Atmos. Chem. Phys., 23, 14949–14971, https://doi.org/10.5194/acp-23-14949-2023, https://doi.org/10.5194/acp-23-14949-2023, 2023
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To be able to meet global grand challenges, we need comprehensive open data with proper metadata. In this opinion paper, we describe the SMEAR (Station for Measuring Earth surface – Atmosphere Relations) concept and include several examples (cases), such as new particle formation and growth, feedback loops and the effect of COVID-19, and what has been learned from these investigations. The future needs and the potential of comprehensive observations of the environment are summarized.
Xiaoxiao Li, Yijing Chen, Yuyang Li, Runlong Cai, Yiran Li, Chenjuan Deng, Jin Wu, Chao Yan, Hairong Cheng, Yongchun Liu, Markku Kulmala, Jiming Hao, James N. Smith, and Jingkun Jiang
Atmos. Chem. Phys., 23, 14801–14812, https://doi.org/10.5194/acp-23-14801-2023, https://doi.org/10.5194/acp-23-14801-2023, 2023
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Near-continuous measurements show the composition, sources, and seasonal variations of ultrafine particles (UFPs) in urban Beijing. Vehicle and cooking emissions and new particle formation are the main sources of UFPs, and aqueous/heterogeneous processes increase UFP mode diameters. UFPs are the highest in winter due to the highest primary particle emission rates and new particle formation rates, and CHO fractions are the highest in summer due to the strongest photooxidation.
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.
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.
Chupeng Zhang, Shangfei Hai, Yang Gao, Yuhang Wang, Shaoqing Zhang, Lifang Sheng, Bin Zhao, Shuxiao Wang, Jingkun Jiang, Xin Huang, Xiaojing Shen, Junying Sun, Aura Lupascu, Manish Shrivastava, Jerome D. Fast, Wenxuan Cheng, Xiuwen Guo, Ming Chu, Nan Ma, Juan Hong, Qiaoqiao Wang, Xiaohong Yao, and Huiwang Gao
Atmos. Chem. Phys., 23, 10713–10730, https://doi.org/10.5194/acp-23-10713-2023, https://doi.org/10.5194/acp-23-10713-2023, 2023
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New particle formation is an important source of atmospheric particles, exerting critical influences on global climate. Numerical models are vital tools to understanding atmospheric particle evolution, which, however, suffer from large biases in simulating particle numbers. Here we improve the model chemical processes governing particle sizes and compositions. The improved model reveals substantial contributions of newly formed particles to climate through effects on cloud condensation nuclei.
Brandon Bottorff, Michelle M. Lew, Youngjun Woo, Pamela Rickly, Matthew D. Rollings, Benjamin Deming, Daniel C. Anderson, Ezra Wood, Hariprasad D. Alwe, Dylan B. Millet, Andrew Weinheimer, Geoff Tyndall, John Ortega, Sebastien Dusanter, Thierry Leonardis, James Flynn, Matt Erickson, Sergio Alvarez, Jean C. Rivera-Rios, Joshua D. Shutter, Frank Keutsch, Detlev Helmig, Wei Wang, Hannah M. Allen, Johnathan H. Slade, Paul B. Shepson, Steven Bertman, and Philip S. Stevens
Atmos. Chem. Phys., 23, 10287–10311, https://doi.org/10.5194/acp-23-10287-2023, https://doi.org/10.5194/acp-23-10287-2023, 2023
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The hydroxyl (OH), hydroperoxy (HO2), and organic peroxy (RO2) radicals play important roles in atmospheric chemistry and have significant air quality implications. Here, we compare measurements of OH, HO2, and total peroxy radicals (XO2) made in a remote forest in Michigan, USA, to predictions from a series of chemical models. Lower measured radical concentrations suggest that the models may be missing an important radical sink and overestimating the rate of ozone production in this forest.
Vigneshkumar Balamurugan, Jia Chen, Adrian Wenzel, and Frank N. Keutsch
Atmos. Chem. Phys., 23, 10267–10285, https://doi.org/10.5194/acp-23-10267-2023, https://doi.org/10.5194/acp-23-10267-2023, 2023
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In this study, machine learning models are employed to model NO2 and O3 concentrations. We employed a wide range of sources of data, including meteorological and column satellite measurements, to model NO2 and O3 concentrations. The spatial and temporal variability, and their drivers, were investigated. Notably, the machine learning model established the relationship between NOx and O3. Despite the fact that metropolitan regions are NO2 hotspots, rural areas have high O3 concentrations.
Sophie L. Haslett, David M. Bell, Varun Kumar, Jay G. Slowik, Dongyu S. Wang, Suneeti Mishra, Neeraj Rastogi, Atinderpal Singh, Dilip Ganguly, Joel Thornton, Feixue Zheng, Yuanyuan Li, Wei Nie, Yongchun Liu, Wei Ma, Chao Yan, Markku Kulmala, Kaspar R. Daellenbach, David Hadden, Urs Baltensperger, Andre S. H. Prevot, Sachchida N. Tripathi, and Claudia Mohr
Atmos. Chem. Phys., 23, 9023–9036, https://doi.org/10.5194/acp-23-9023-2023, https://doi.org/10.5194/acp-23-9023-2023, 2023
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In Delhi, some aspects of daytime and nighttime atmospheric chemistry are inverted, and parodoxically, vehicle emissions may be limiting other forms of particle production. This is because the nighttime emissions of nitrogen oxide (NO) by traffic and biomass burning prevent some chemical processes that would otherwise create even more particles and worsen the urban haze.
Yuyang Li, Jiewen Shen, Bin Zhao, Runlong Cai, Shuxiao Wang, Yang Gao, Manish Shrivastava, Da Gao, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 23, 8789–8804, https://doi.org/10.5194/acp-23-8789-2023, https://doi.org/10.5194/acp-23-8789-2023, 2023
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We set up a new parameterization for 1.4 nm particle formation rates from sulfuric acid–dimethylamine (SA–DMA) nucleation, fully including the effects of coagulation scavenging and cluster stability. Incorporating the new parameterization into 3-D chemical transport models, we achieved better consistencies between simulation results and observation data. This new parameterization provides new insights into atmospheric nucleation simulations and its effects on atmospheric pollution or health.
Chenxi Li, Yuyang Li, Xiaoxiao Li, Runlong Cai, Yaxin Fan, Xiaohui Qiao, Rujing Yin, Chao Yan, Yishuo Guo, Yongchun Liu, Jun Zheng, Veli-Matti Kerminen, Markku Kulmala, Huayun Xiao, and Jingkun Jiang
Atmos. Chem. Phys., 23, 6879–6896, https://doi.org/10.5194/acp-23-6879-2023, https://doi.org/10.5194/acp-23-6879-2023, 2023
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New particle formation and growth in polluted environments are not fully understood despite intensive research. We applied a cluster dynamics–multicomponent sectional model to simulate the new particle formation events observed in Beijing, China. The simulation approximately captures how the events evolve. Further diagnosis shows that the oxygenated organic molecules may have been under-detected, and modulating their abundance leads to significantly improved simulation–observation agreement.
Yishuo Guo, Chenjuan Deng, Aino Ovaska, Feixue Zheng, Chenjie Hua, Junlei Zhan, Yiran Li, Jin Wu, Zongcheng Wang, Jiali Xie, Ying Zhang, Tingyu Liu, Yusheng Zhang, Boying Song, Wei Ma, Yongchun Liu, Chao Yan, Jingkun Jiang, Veli-Matti Kerminen, Men Xia, Tuomo Nieminen, Wei Du, Tom Kokkonen, and Markku Kulmala
Atmos. Chem. Phys., 23, 6663–6690, https://doi.org/10.5194/acp-23-6663-2023, https://doi.org/10.5194/acp-23-6663-2023, 2023
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Using the comprehensive datasets, we investigated the long-term variations of air pollutants during winter in Beijing from 2019 to 2022 and analyzed the characteristics of atmospheric pollution cocktail during different short-term special events (e.g., Beijing Winter Olympics, COVID lockdown and Chinese New Year) associated with substantial emission reductions. Our results are useful in planning more targeted and sustainable long-term pollution control plans.
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.
Juan Hong, Min Tang, Qiaoqiao Wang, Nan Ma, Shaowen Zhu, Shaobin Zhang, Xihao Pan, Linhong Xie, Guo Li, Uwe Kuhn, Chao Yan, Jiangchuan Tao, Ye Kuang, Yao He, Wanyun Xu, Runlong Cai, Yaqing Zhou, Zhibin Wang, Guangsheng Zhou, Bin Yuan, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 23, 5699–5713, https://doi.org/10.5194/acp-23-5699-2023, https://doi.org/10.5194/acp-23-5699-2023, 2023
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A comprehensive investigation of the characteristics of new particle formation (NPF) events was conducted at a rural site on the North China Plain (NCP), China, during the wintertime of 2018 by covering the particle number size distribution down to sub–3 nm. Potential mechanisms for NPF under the current environment were explored, followed by a further discussion on the factors governing the occurrence of NPF at this rural site compared with other regions (e.g., urban areas) in the NCP region.
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.
Rujing Yin, Xiaoxiao Li, Chao Yan, Runlong Cai, Ying Zhou, Juha Kangasluoma, Nina Sarnela, Janne Lampilahti, Tuukka Petäjä, Veli-Matti Kerminen, Federico Bianchi, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 23, 5279–5296, https://doi.org/10.5194/acp-23-5279-2023, https://doi.org/10.5194/acp-23-5279-2023, 2023
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Atmospheric cluster ions are important constituents in the atmosphere. However, the quantitative research on their compositions is still limited, especially in urban environments. Here we demonstrate the feasibility of an in situ quantification method of cluster ions measured by a high-resolution mass spectrometer and reveal their governing factors, sources, and sinks in urban Beijing through quantitative analysis of cluster ions, reagent ions, neutral molecules, and condensation sink.
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.
Qing Ye, Matthew B. Goss, Jordan E. Krechmer, Francesca Majluf, Alexander Zaytsev, Yaowei Li, Joseph R. Roscioli, Manjula Canagaratna, Frank N. Keutsch, Colette L. Heald, and Jesse H. Kroll
Atmos. Chem. Phys., 22, 16003–16015, https://doi.org/10.5194/acp-22-16003-2022, https://doi.org/10.5194/acp-22-16003-2022, 2022
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The atmospheric oxidation of dimethyl sulfide (DMS) is a major natural source of sulfate particles in the atmosphere. However, its mechanism is poorly constrained. In our work, laboratory measurements and mechanistic modeling were conducted to comprehensively investigate DMS oxidation products and key reaction rates. We find that the peroxy radical (RO2) has a controlling effect on product distribution and aerosol yield, with the isomerization of RO2 leading to the suppression of aerosol yield.
Zhaofeng Lv, Zhenyu Luo, Fanyuan Deng, Xiaotong Wang, Junchao Zhao, Lucheng Xu, Tingkun He, Yingzhi Zhang, Huan Liu, and Kebin He
Atmos. Chem. Phys., 22, 15685–15702, https://doi.org/10.5194/acp-22-15685-2022, https://doi.org/10.5194/acp-22-15685-2022, 2022
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This study developed a hybrid model, CMAQ-RLINE_URBAN, to predict the urban NO2 concentrations at a high spatial resolution. To estimate the influence of various street canyons on the dispersion of air pollutants, a new parameterization scheme was established based on computational fluid dynamics and machine learning methods. This work created a new method to identify the characteristics of vehicle-related air pollution at both city and street scales simultaneously and accurately.
Santeri Tuovinen, Runlong Cai, Veli-Matti Kerminen, Jingkun Jiang, Chao Yan, Markku Kulmala, and Jenni Kontkanen
Atmos. Chem. Phys., 22, 15071–15091, https://doi.org/10.5194/acp-22-15071-2022, https://doi.org/10.5194/acp-22-15071-2022, 2022
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We compare observed survival probabilities of atmospheric particles from Beijing, China, with survival probabilities based on analytical formulae and model simulations. We find observed survival probabilities under polluted conditions at smaller sizes to be higher, while at larger sizes they are lower than or similar to theoretical survival probabilities. Uncertainties in condensation sink and growth rate are unlikely to explain higher-than-predicted survival probabilities at smaller sizes.
Runlong Cai, Chenjuan Deng, Dominik Stolzenburg, Chenxi Li, Junchen Guo, Veli-Matti Kerminen, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys., 22, 14571–14587, https://doi.org/10.5194/acp-22-14571-2022, https://doi.org/10.5194/acp-22-14571-2022, 2022
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The survival probability of new particles is the key parameter governing their influences on the atmosphere and climate, yet the knowledge of particle survival in the atmosphere is rather limited. We propose methods to compute the size-resolved particle survival probability and validate them using simulations and measurements from diverse environments. Using these methods, we could explain particle survival from the cluster size to the cloud condensation nuclei size.
Chenjuan Deng, Yiran Li, Chao Yan, Jin Wu, Runlong Cai, Dongbin Wang, Yongchun Liu, Juha Kangasluoma, Veli-Matti Kerminen, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 22, 13569–13580, https://doi.org/10.5194/acp-22-13569-2022, https://doi.org/10.5194/acp-22-13569-2022, 2022
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The size distributions of urban atmospheric particles convey important information on their origins and impacts. This study investigates the characteristics of typical particle size distributions and key gaseous precursors in the long term in urban Beijing. A fitting function is proposed to represent and help interpret size distribution including particles and gaseous precursors. In addition to NPF (new particle formation) as the major source, vehicles can emit sub-3 nm particles as well
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.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866, https://doi.org/10.5194/acp-22-11845-2022, https://doi.org/10.5194/acp-22-11845-2022, 2022
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This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Runlong Cai, Ella Häkkinen, Chao Yan, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys., 22, 11529–11541, https://doi.org/10.5194/acp-22-11529-2022, https://doi.org/10.5194/acp-22-11529-2022, 2022
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The influences of new particle formation on the climate and air quality are governed by particle survival, which has been under debate due to uncertainties in the coagulation sink. Here we measure the coagulation coefficient of sub-10 nm particles and demonstrate that collisions between the freshly nucleated and background particles can effectively lead to coagulation. We further show that the effective coagulation sink is consistent with the new particle formation measured in urban Beijing.
Benjamin Foreback, Lubna Dada, Kaspar R. Daellenbach, Chao Yan, Lili Wang, Biwu Chu, Ying Zhou, Tom V. Kokkonen, Mona Kurppa, Rosaria E. Pileci, Yonghong Wang, Tommy Chan, Juha Kangasluoma, Lin Zhuohui, Yishou Guo, Chang Li, Rima Baalbaki, Joni Kujansuu, Xiaolong Fan, Zemin Feng, Pekka Rantala, Shahzad Gani, Federico Bianchi, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, Yongchun Liu, and Pauli Paasonen
Atmos. Chem. Phys., 22, 11089–11104, https://doi.org/10.5194/acp-22-11089-2022, https://doi.org/10.5194/acp-22-11089-2022, 2022
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This study analyzed air quality in Beijing during the Chinese New Year over 7 years, including data from a new in-depth measurement station. This is one of few studies to look at long-term impacts, including the outcome of firework restrictions starting in 2018. Results show that firework pollution has gone down since 2016, indicating a positive result from the restrictions. Results of this study may be useful in making future decisions about the use of fireworks to improve air quality.
Yawen Kong, Bo Zheng, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 22, 10769–10788, https://doi.org/10.5194/acp-22-10769-2022, https://doi.org/10.5194/acp-22-10769-2022, 2022
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We developed a Bayesian atmospheric inversion system based on the 4D local ensemble transform Kalman filter (4D-LETKF) algorithm coupled with GEOS-Chem from the latest Orbiting Carbon Observatory-2 (OCO-2) V10r XCO2 retrievals. This is the first adaptation of 4D-LETKF to an OCO-2-based global carbon inversion system. We inferred global gridded carbon fluxes and investigated their magnitudes, variations, and partitioning schemes to understand the global and regional carbon budgets for 2015–2020.
Yishuo Guo, Chao Yan, Yuliang Liu, Xiaohui Qiao, Feixue Zheng, Ying Zhang, Ying Zhou, Chang Li, Xiaolong Fan, Zhuohui Lin, Zemin Feng, Yusheng Zhang, Penggang Zheng, Linhui Tian, Wei Nie, Zhe Wang, Dandan Huang, Kaspar R. Daellenbach, Lei Yao, Lubna Dada, Federico Bianchi, Jingkun Jiang, Yongchun Liu, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 22, 10077–10097, https://doi.org/10.5194/acp-22-10077-2022, https://doi.org/10.5194/acp-22-10077-2022, 2022
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Gaseous oxygenated organic molecules (OOMs) are able to form atmospheric aerosols, which will impact on human health and climate change. Here, we find that OOMs in urban Beijing are dominated by anthropogenic sources, i.e. aromatic (29 %–41 %) and aliphatic (26 %–41 %) OOMs. They are also the main contributors to the condensational growth of secondary organic aerosols (SOAs). Therefore, the restriction on anthropogenic VOCs is crucial for the reduction of SOAs and haze formation.
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.
Vigneshkumar Balamurugan, Jia Chen, Zhen Qu, Xiao Bi, and Frank N. Keutsch
Atmos. Chem. Phys., 22, 7105–7129, https://doi.org/10.5194/acp-22-7105-2022, https://doi.org/10.5194/acp-22-7105-2022, 2022
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In this study, we investigated the response of secondary pollutants to changes in precursor emissions, focusing on the formation of secondary PM, during the COVID-19 lockdown period. We show that, due to the decrease in primary NOx emissions, atmospheric oxidizing capacity is increased. The nighttime increase in ozone, caused by less NO titration, results in higher NO3 radicals, which contribute significantly to the formation of PM nitrates. O3 should be limited in order to control PM pollution.
Jiandong Wang, Jia Xing, Shuxiao Wang, Rohit Mathur, Jiaping Wang, Yuqiang Zhang, Chao Liu, Jonathan Pleim, Dian Ding, Xing Chang, Jingkun Jiang, Peng Zhao, Shovan Kumar Sahu, Yuzhi Jin, David C. Wong, and Jiming Hao
Atmos. Chem. Phys., 22, 5147–5156, https://doi.org/10.5194/acp-22-5147-2022, https://doi.org/10.5194/acp-22-5147-2022, 2022
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Aerosols reduce surface solar radiation and change the photolysis rate and planetary boundary layer stability. In this study, the online coupled meteorological and chemistry model was used to explore the detailed pathway of how aerosol direct effects affect secondary inorganic aerosol. The effects through the dynamics pathway act as an equally or even more important route compared with the photolysis pathway in affecting secondary aerosol concentration in both summer and winter.
Jingwei Zhang, Chaofan Lian, Weigang Wang, Maofa Ge, Yitian Guo, Haiyan Ran, Yusheng Zhang, Feixue Zheng, Xiaolong Fan, Chao Yan, Kaspar R. Daellenbach, Yongchun Liu, Markku Kulmala, and Junling An
Atmos. Chem. Phys., 22, 3275–3302, https://doi.org/10.5194/acp-22-3275-2022, https://doi.org/10.5194/acp-22-3275-2022, 2022
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This study added six potential HONO sources to the WRF-Chem model, evaluated their impact on HONO and O3 concentrations, including surface and vertical concentrations. The simulations extend our knowledge on atmospheric HONO sources, especially for nitrate photolysis. The study also explains the HONO difference in O3 formation on clean and hazy days, and reveals key potential HONO sources to O3 enhancements in haze-aggravating processes with a co-occurrence of high PM2.5 and O3 concentrations.
Jing Cai, Cheng Wu, Jiandong Wang, Wei Du, Feixue Zheng, Simo Hakala, Xiaolong Fan, Biwu Chu, Lei Yao, Zemin Feng, Yongchun Liu, Yele Sun, Jun Zheng, Chao Yan, Federico Bianchi, Markku Kulmala, Claudia Mohr, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 22, 1251–1269, https://doi.org/10.5194/acp-22-1251-2022, https://doi.org/10.5194/acp-22-1251-2022, 2022
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This study investigates the connection between organic aerosol (OA) molecular composition and particle absorptive properties in autumn in Beijing. We find that the molecular properties of OA compounds in different episodes influence particle light absorption properties differently: the light absorption enhancement of black carbon and light absorption coefficient of brown carbon were mostly related to more oxygenated OA (low C number and four O atoms) and aromatics/nitro-aromatics, respectively.
Ying Zhou, Simo Hakala, Chao Yan, Yang Gao, Xiaohong Yao, Biwu Chu, Tommy Chan, Juha Kangasluoma, Shahzad Gani, Jenni Kontkanen, Pauli Paasonen, Yongchun Liu, Tuukka Petäjä, Markku Kulmala, and Lubna Dada
Atmos. Chem. Phys., 21, 17885–17906, https://doi.org/10.5194/acp-21-17885-2021, https://doi.org/10.5194/acp-21-17885-2021, 2021
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We characterized the connection between new particle formation (NPF) events in terms of frequency, intensity and growth at a near-highway location in central Beijing and at a background mountain site 80 km away. Due to the substantial contribution of NPF to the global aerosol budget, identifying the conditions that promote the occurrence of regional NPF events could help understand their contribution on a large scale and would improve their implementation in global models.
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.
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.
Dandan Wei, Hariprasad D. Alwe, Dylan B. Millet, Brandon Bottorff, Michelle Lew, Philip S. Stevens, Joshua D. Shutter, Joshua L. Cox, Frank N. Keutsch, Qianwen Shi, Sarah C. Kavassalis, Jennifer G. Murphy, Krystal T. Vasquez, Hannah M. Allen, Eric Praske, John D. Crounse, Paul O. Wennberg, Paul B. Shepson, Alexander A. T. Bui, Henry W. Wallace, Robert J. Griffin, Nathaniel W. May, Megan Connor, Jonathan H. Slade, Kerri A. Pratt, Ezra C. Wood, Mathew Rollings, Benjamin L. Deming, Daniel C. Anderson, and Allison L. Steiner
Geosci. Model Dev., 14, 6309–6329, https://doi.org/10.5194/gmd-14-6309-2021, https://doi.org/10.5194/gmd-14-6309-2021, 2021
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Over the past decade, understanding of isoprene oxidation has improved, and proper representation of isoprene oxidation and isoprene-derived SOA (iSOA) formation in canopy–chemistry models is now recognized to be important for an accurate understanding of forest–atmosphere exchange. The updated FORCAsT version 2.0 improves the estimation of some isoprene oxidation products and is one of the few canopy models currently capable of simulating SOA formation from monoterpenes and isoprene.
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.
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.
Xiaotong Wang, Wen Yi, Zhaofeng Lv, Fanyuan Deng, Songxin Zheng, Hailian Xu, Junchao Zhao, Huan Liu, and Kebin He
Atmos. Chem. Phys., 21, 13835–13853, https://doi.org/10.5194/acp-21-13835-2021, https://doi.org/10.5194/acp-21-13835-2021, 2021
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This study updates our previous Ship Emission Inventory Model to version 2.0 (SEIM v2.0) and develops high-spatiotemporal ship emission inventories of China’s inland rivers and a 200 nautical mile coastal zone in 2016–2019. The 4-year consecutive daily ship emissions and emission structure changes are analyzed from the national to port levels. The results of this study can provide high-quality datasets for air quality modeling and observation experiment verifications.
Yongchun Liu, Zemin Feng, Feixue Zheng, Xiaolei Bao, Pengfei Liu, Yanli Ge, Yan Zhao, Tao Jiang, Yunwen Liao, Yusheng Zhang, Xiaolong Fan, Chao Yan, Biwu Chu, Yonghong Wang, Wei Du, Jing Cai, Federico Bianchi, Tuukka Petäjä, Yujing Mu, Hong He, and Markku Kulmala
Atmos. Chem. Phys., 21, 13269–13286, https://doi.org/10.5194/acp-21-13269-2021, https://doi.org/10.5194/acp-21-13269-2021, 2021
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The mechanisms and kinetics of particulate sulfate formation in the atmosphere are still open questions although they have been extensively discussed. We found that uptake of SO2 is the rate-determining step for the conversion of SO2 to particulate sulfate. NH4NO3 plays an important role in AWC, the phase state of aerosol particles, and subsequently the uptake kinetics of SO2 under high-RH conditions. This work is a good example of the feedback between aerosol physics and aerosol chemistry.
Zhuohui Lin, Yonghong Wang, Feixue Zheng, Ying Zhou, Yishuo Guo, Zemin Feng, Chang Li, Yusheng Zhang, Simo Hakala, Tommy Chan, Chao Yan, Kaspar R. Daellenbach, Biwu Chu, Lubna Dada, Juha Kangasluoma, Lei Yao, Xiaolong Fan, Wei Du, Jing Cai, Runlong Cai, Tom V. Kokkonen, Putian Zhou, Lili Wang, Tuukka Petäjä, Federico Bianchi, Veli-Matti Kerminen, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 12173–12187, https://doi.org/10.5194/acp-21-12173-2021, https://doi.org/10.5194/acp-21-12173-2021, 2021
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We find that ammonium nitrate and aerosol water content contributed most during low mixing layer height conditions; this may further trigger enhanced formation of sulfate and organic aerosol via heterogeneous reactions. The results of this study contribute towards a more detailed understanding of the aerosol–chemistry–radiation–boundary layer feedback that is likely to be responsible for explosive aerosol mass growth events in urban Beijing.
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.
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.
Qingyang Xiao, Yixuan Zheng, Guannan Geng, Cuihong Chen, Xiaomeng Huang, Huizheng Che, Xiaoye Zhang, Kebin He, and Qiang Zhang
Atmos. Chem. Phys., 21, 9475–9496, https://doi.org/10.5194/acp-21-9475-2021, https://doi.org/10.5194/acp-21-9475-2021, 2021
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We used both statistical methods and a chemical transport model to assess the contribution of meteorology and emissions to PM2.5 during 2000–2018. Both methods revealed that emissions dominated the long-term PM2.5 trend with notable meteorological effects ranged up to 37.9 % of regional annual average PM2.5. The meteorological contribution became more beneficial to PM2.5 control in southern China but more unfavorable in northern China during the studied period.
Eleni Dovrou, Kelvin H. Bates, Jean C. Rivera-Rios, Joshua L. Cox, Joshua D. Shutter, and Frank N. Keutsch
Atmos. Chem. Phys., 21, 8999–9008, https://doi.org/10.5194/acp-21-8999-2021, https://doi.org/10.5194/acp-21-8999-2021, 2021
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We examined the mechanism and products of oxidation of dissolved sulfur dioxide with the main isomers of isoprene hydroxyl hydroperoxides, via laboratory and model analysis. Two chemical mechanism pathways are proposed and the results provide an improved understanding of the broader atmospheric chemistry and role of multifunctional organic hydroperoxides, which should be the dominant VOC oxidation products under low-NO conditions, highlighting their significant contribution to sulfate formation.
Jack C. Hensley, Adam W. Birdsall, Gregory Valtierra, Joshua L. Cox, and Frank N. Keutsch
Atmos. Chem. Phys., 21, 8809–8821, https://doi.org/10.5194/acp-21-8809-2021, https://doi.org/10.5194/acp-21-8809-2021, 2021
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We measured reactions of butenedial, an atmospheric dicarbonyl, in aqueous mixtures that mimic the conditions of aerosol particles. Major reaction products and rates were determined to assess their atmospheric relevance and to compare against other well-studied dicarbonyls. We suggest that the structure of the carbon backbone, not just the dominant functional group, plays a major role in dicarbonyl reactivity, influencing the fate and ability of dicarbonyls to produce brown carbon.
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).
Yishuo Guo, Chao Yan, Chang Li, Wei Ma, Zemin Feng, Ying Zhou, Zhuohui Lin, Lubna Dada, Dominik Stolzenburg, Rujing Yin, Jenni Kontkanen, Kaspar R. Daellenbach, Juha Kangasluoma, Lei Yao, Biwu Chu, Yonghong Wang, Runlong Cai, Federico Bianchi, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 5499–5511, https://doi.org/10.5194/acp-21-5499-2021, https://doi.org/10.5194/acp-21-5499-2021, 2021
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Fog, cloud and haze are very common natural phenomena. Sulfuric acid (SA) is one of the key compounds forming those suspended particles, technically called aerosols, through gas-to-particle conversion. Therefore, the concentration level, source and sink of SA is very important. Our results show that ozonolysis of alkenes plays a major role in nighttime SA formation under unpolluted conditions in urban Beijing, and nighttime cluster mode particles are probably driven by SA in urban environments.
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.
Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 14, 2501–2513, https://doi.org/10.5194/amt-14-2501-2021, https://doi.org/10.5194/amt-14-2501-2021, 2021
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We have developed an online method for speciated measurements of organic peroxy radicals and stabilized Criegee intermediates using chemical derivatization combined with chemical ionization mass spectrometry. Chemical derivatization prevents secondary radical reactions and eliminates potential interferences. Comparison between our measurements and results from numeric modeling shows that the method can be used for the quantification of a wide range of atmospheric radicals and intermediates.
Clémence Rose, Matti P. Rissanen, Siddharth Iyer, Jonathan Duplissy, Chao Yan, John B. Nowak, Aurélie Colomb, Régis Dupuy, Xu-Cheng He, Janne Lampilahti, Yee Jun Tham, Daniela Wimmer, Jean-Marc Metzger, Pierre Tulet, Jérôme Brioude, Céline Planche, Markku Kulmala, and Karine Sellegri
Atmos. Chem. Phys., 21, 4541–4560, https://doi.org/10.5194/acp-21-4541-2021, https://doi.org/10.5194/acp-21-4541-2021, 2021
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Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation. However, direct measurements of [H2SO4] remain challenging, motivating the development of proxies. Using data collected in two different volcanic plumes, we show, under these specific conditions, the good performance of a proxy from the literature and also highlight the benefit of the newly developed proxies for the prediction of the highest [H2SO4] values.
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.
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.
Runlong Cai, Chenxi Li, Xu-Cheng He, Chenjuan Deng, Yiqun Lu, Rujing Yin, Chao Yan, Lin Wang, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys., 21, 2287–2304, https://doi.org/10.5194/acp-21-2287-2021, https://doi.org/10.5194/acp-21-2287-2021, 2021
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Growth rate determines the survival probability of atmospheric new particles and hence their impacts. We clarify the impacts of coagulation on the values retrieved by the appearance time method, which is widely used for growth rate evaluation. A new formula with coagulation correction is proposed based on derivation and tested using both models and atmospheric data. We show that the sub-3 nm particle growth rate in polluted environments may be overestimated without the coagulation correction.
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.
Shaojie Song, Tao Ma, Yuzhong Zhang, Lu Shen, Pengfei Liu, Ke Li, Shixian Zhai, Haotian Zheng, Meng Gao, Jonathan M. Moch, Fengkui Duan, Kebin He, and Michael B. McElroy
Atmos. Chem. Phys., 21, 457–481, https://doi.org/10.5194/acp-21-457-2021, https://doi.org/10.5194/acp-21-457-2021, 2021
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We simulate the atmospheric chemical processes of an important sulfur-containing organic aerosol species, which is produced by the reaction between sulfur dioxide and formaldehyde. We can predict its distribution on a global scale. We find it is particularly rich in East Asia. This aerosol species is more abundant in the colder season partly because of weaker sunlight.
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.
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.
Yongchun Liu, Yusheng Zhang, Chaofan Lian, Chao Yan, Zeming Feng, Feixue Zheng, Xiaolong Fan, Yan Chen, Weigang Wang, Biwu Chu, Yonghong Wang, Jing Cai, Wei Du, Kaspar R. Daellenbach, Juha Kangasluoma, Federico Bianchi, Joni Kujansuu, Tuukka Petäjä, Xuefei Wang, Bo Hu, Yuesi Wang, Maofa Ge, Hong He, and Markku Kulmala
Atmos. Chem. Phys., 20, 13023–13040, https://doi.org/10.5194/acp-20-13023-2020, https://doi.org/10.5194/acp-20-13023-2020, 2020
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Understanding of the chemical and physical processes leading to atmospheric aerosol particle formation is crucial to devising effective mitigation strategies to protect the public and reduce uncertainties in climate predictions. We found that the photolysis of nitrous acid could promote the formation of organic and nitrate aerosol and that traffic-related emission is a major contributor to ambient nitrous acid on haze days in wintertime in Beijing.
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.
Lei Zhu, Gonzalo González Abad, Caroline R. Nowlan, Christopher Chan Miller, Kelly Chance, Eric C. Apel, Joshua P. DiGangi, Alan Fried, Thomas F. Hanisco, Rebecca S. Hornbrook, Lu Hu, Jennifer Kaiser, Frank N. Keutsch, Wade Permar, Jason M. St. Clair, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 12329–12345, https://doi.org/10.5194/acp-20-12329-2020, https://doi.org/10.5194/acp-20-12329-2020, 2020
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We develop a validation platform for satellite HCHO retrievals using in situ observations from 12 aircraft campaigns. The platform offers an alternative way to quickly assess systematic biases in HCHO satellite products over large domains and long periods, facilitating optimization of retrieval settings and the minimization of retrieval biases. Application to the NASA operational HCHO product indicates that relative biases range from −44.5 % to +112.1 % depending on locations and seasons.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Lubna Dada, Ilona Ylivinkka, Rima Baalbaki, Chang Li, Yishuo Guo, Chao Yan, Lei Yao, Nina Sarnela, Tuija Jokinen, Kaspar R. Daellenbach, Rujing Yin, Chenjuan Deng, Biwu Chu, Tuomo Nieminen, Yonghong Wang, Zhuohui Lin, Roseline C. Thakur, Jenni Kontkanen, Dominik Stolzenburg, Mikko Sipilä, Tareq Hussein, Pauli Paasonen, Federico Bianchi, Imre Salma, Tamás Weidinger, Michael Pikridas, Jean Sciare, Jingkun Jiang, Yongchun Liu, Tuukka Petäjä, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 20, 11747–11766, https://doi.org/10.5194/acp-20-11747-2020, https://doi.org/10.5194/acp-20-11747-2020, 2020
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We rely on sulfuric acid measurements in four contrasting environments, Hyytiälä, Finland; Agia Marina, Cyprus; Budapest, Hungary; and Beijing, China, representing semi-pristine boreal forest, rural environment in the Mediterranean area, urban environment, and heavily polluted megacity, respectively, in order to define the sources and sinks of sulfuric acid in these environments and to derive a new sulfuric acid proxy to be utilized in locations and during periods when it is not measured.
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Short summary
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.
Online Vocus-PTR measurements show the compositions and seasonal variations in organic vapors in...
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