Articles | Volume 19, issue 4
Atmos. Chem. Phys., 19, 2283–2298, 2019
https://doi.org/10.5194/acp-19-2283-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 19, 2283–2298, 2019
https://doi.org/10.5194/acp-19-2283-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
21 Feb 2019
Research article
| 21 Feb 2019
Primary emissions versus secondary formation of fine particulate matter in the most polluted city (Shijiazhuang) in North China
Ru-Jin Huang et al.
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Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-725, https://doi.org/10.5194/acp-2022-725, 2022
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This work investigated seasonal variation of aerosol Fe solubility for coarse and fine particles in Xi’an, a megacity severely in northwestern China 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.
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. Discuss., https://doi.org/10.5194/acp-2022-573, https://doi.org/10.5194/acp-2022-573, 2022
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Secondary organic aerosol (SOA) could be produced by various pathways but its formation mechanisms are unclear. Observations were conducted in North China Plain during a highly oxidizing atmosphere in summer. We found here 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.
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.
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.
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.
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.
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.
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
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.
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.
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.
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
Chunshui Lin, Darius Ceburnis, Wei Xu, Eimear Heffernan, Stig Hellebust, John Gallagher, Ru-Jin Huang, Colin O'Dowd, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 20, 10513–10529, https://doi.org/10.5194/acp-20-10513-2020, https://doi.org/10.5194/acp-20-10513-2020, 2020
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Chemical composition and sources of submicron aerosols (PM1) were simultaneously investigated at a kerbside site in the Dublin city center and at a residential site in suburban Dublin (~5 km apart) during both a nonheating and a heating period in 2018. This study highlights the temporal and spatial variability of sources within the Dublin city center and the need for additional aerosol characterization studies to improve targeted mitigation solutions for a greater impact on urban air quality.
Ru-Jin Huang, Yao He, Jing Duan, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Weiwei Hu, Chunshui Lin, Haiyan Ni, Wenting Dai, Junji Cao, Yunfei Wu, Renjian Zhang, Wei Xu, Jurgita Ovadnevaite, Darius Ceburnis, Thorsten Hoffmann, and Colin D. O'Dowd
Atmos. Chem. Phys., 20, 9101–9114, https://doi.org/10.5194/acp-20-9101-2020, https://doi.org/10.5194/acp-20-9101-2020, 2020
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We systematically compared the submicron particle (PM1) processes in haze days with low and high relative humidity (RH) in wintertime Beijing. Nitrate had similar daytime growth rates in low-RH and high-RH pollution. OOA had a higher growth rate in low-RH pollution than in high-RH pollution. Sulfate had a decreasing trend in low-RH pollution, while it increased significantly in high-RH pollution. This distinction may be explained by the different processes affected by meteorological conditions.
Yan Zheng, Xi Cheng, Keren Liao, Yaowei Li, Yong Jie Li, Ru-Jin Huang, Weiwei Hu, Ying Liu, Tong Zhu, Shiyi Chen, Limin Zeng, Douglas R. Worsnop, and Qi Chen
Atmos. Meas. Tech., 13, 2457–2472, https://doi.org/10.5194/amt-13-2457-2020, https://doi.org/10.5194/amt-13-2457-2020, 2020
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This paper provides important information to help researchers to understand the mass quantification and source apportionment by Aerodyne aerosol mass spectrometers.
Wei Yuan, Ru-Jin Huang, Lu Yang, Jie Guo, Ziyi Chen, Jing Duan, Ting Wang, Haiyan Ni, Yongming Han, Yongjie Li, Qi Chen, Yang Chen, Thorsten Hoffmann, and Colin O'Dowd
Atmos. Chem. Phys., 20, 5129–5144, https://doi.org/10.5194/acp-20-5129-2020, https://doi.org/10.5194/acp-20-5129-2020, 2020
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We characterized light-absorbing properties, chromophore composition and sources of brown carbon (BrC) in Xi'an; identified three groups of light-absorbing organics; and quantified their contribution to overall BrC absorption. Our results showed that vehicle emissions and secondary formation are major sources of BrC in spring, coal combustion and vehicle emissions are major sources in fall, biomass burning and coal combustion become major sources in winter, and secondary BrC dominates in summer.
Jing Duan, Ru-Jin Huang, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Chunshui Lin, Haiyan Ni, Meng Wang, Jurgita Ovadnevaite, Darius Ceburnis, Chunying Chen, Douglas R. Worsnop, Thorsten Hoffmann, Colin O'Dowd, and Junji Cao
Atmos. Chem. Phys., 20, 3793–3807, https://doi.org/10.5194/acp-20-3793-2020, https://doi.org/10.5194/acp-20-3793-2020, 2020
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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.
Wei Xu, Jurgita Ovadnevaite, Kirsten N. Fossum, Chunshui Lin, Ru-Jin Huang, Colin O'Dowd, and Darius Ceburnis
Atmos. Chem. Phys., 20, 3777–3791, https://doi.org/10.5194/acp-20-3777-2020, https://doi.org/10.5194/acp-20-3777-2020, 2020
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A humidified tandem differential mobility analyser (HTDMA) and a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) were simultaneously deployed during winter at Mace Head observatory to characterise the hygroscopicity of marine aerosols and their link to chemical composition. Good agreement was generally found between measured and estimated growth factors. A significant degree of external mixing was found in all air masses manifesting primary and secondary sources.
Haiyan Ni, Ru-Jin Huang, Junji Cao, Jie Guo, Haoyue Deng, and Ulrike Dusek
Atmos. Chem. Phys., 19, 15609–15628, https://doi.org/10.5194/acp-19-15609-2019, https://doi.org/10.5194/acp-19-15609-2019, 2019
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We present a 1-year source apportionment record of carbonaceous aerosols in Xi'an, China. Biomass burning strongly increases in winter, while seasonal changes of coal and liquid fossil fuel combustion are moderate. We find strong evidence for fossil secondary OC formation during the warm period that is further enhanced in stagnant, polluted conditions due to longer atmospheric residence times. At the same time we find that water-insoluble (primary) fossil is lost due to photochemical processing.
Jun Zhou, Miriam Elser, Ru-Jin Huang, Manuel Krapf, Roman Fröhlich, Deepika Bhattu, Giulia Stefenelli, Peter Zotter, Emily A. Bruns, Simone M. Pieber, Haiyan Ni, Qiyuan Wang, Yichen Wang, Yaqing Zhou, Chunying Chen, Mao Xiao, Jay G. Slowik, Samuel Brown, Laure-Estelle Cassagnes, Kaspar R. Daellenbach, Thomas Nussbaumer, Marianne Geiser, André S. H. Prévôt, Imad El-Haddad, Junji Cao, Urs Baltensperger, and Josef Dommen
Atmos. Chem. Phys., 19, 14703–14720, https://doi.org/10.5194/acp-19-14703-2019, https://doi.org/10.5194/acp-19-14703-2019, 2019
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Reactive oxygen species (ROS) are believed to contribute to the adverse health effects of aerosols. We measured particle-bound ROS (PB-ROS) with an online instrument in two distinct environments, i.e., Beijing (China) and Bern (Switzerland). In both cities these exogenic ROS are predominantly related to secondary organic aerosol (SOA). PB-ROS content in SOA from various anthropogenic emission sources tested in the laboratory was comparable to that in the ambient measurements.
Chunshui Lin, Darius Ceburnis, Ru-Jin Huang, Wei Xu, Teresa Spohn, Damien Martin, Paul Buckley, John Wenger, Stig Hellebust, Matteo Rinaldi, Maria Cristina Facchini, Colin O'Dowd, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 19, 14091–14106, https://doi.org/10.5194/acp-19-14091-2019, https://doi.org/10.5194/acp-19-14091-2019, 2019
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To gain insight into the spatial and chemical variation in submicron aerosol, a nationwide characterization of wintertime PM1 was performed at four representative sites across Ireland. This nationwide source apportionment study highlights the large contribution of residential solid fuel burning to urban air pollution and has significant implications for aerosol regional-transport models.
Meng Wang, Ru-Jin Huang, Junji Cao, Wenting Dai, Jiamao Zhou, Chunshui Lin, Haiyan Ni, Jing Duan, Ting Wang, Yang Chen, Yongjie Li, Qi Chen, Imad El Haddad, and Thorsten Hoffmann
Atmos. Meas. Tech., 12, 4779–4789, https://doi.org/10.5194/amt-12-4779-2019, https://doi.org/10.5194/amt-12-4779-2019, 2019
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The analytical performances of SE-GC-MS and TD-GC-MS for the determination of n-alkanes, PAHs and hopanes were evaluated and compared. The two methods show a good agreement with a high correlation efficient (R2 > 0.98) and a slope close to unity. The concentrations of n-alkanes, PAHs and hopanes are found to be much higher in Beijing than those in Chengdu, Shanghai and Guangzhou, most likely due to emissions from coal combustion for wintertime heating in Beijing.
Haiyan Ni, Ru-Jin Huang, Junji Cao, Wenting Dai, Jiamao Zhou, Haoyue Deng, Anita Aerts-Bijma, Harro A. J. Meijer, and Ulrike Dusek
Atmos. Chem. Phys., 19, 10405–10422, https://doi.org/10.5194/acp-19-10405-2019, https://doi.org/10.5194/acp-19-10405-2019, 2019
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We apply radiocarbon source apportionment of more volatile organic carbon (mvOC) to winter aerosol samples from six Chinese cities. We find a consistently larger contribution of fossil sources to mvOC than to secondary or total organic carbon. Fossil mvOC concentrations are strongly correlated with primary fossil OC but not with secondary fossil OC. The variability in nonfossil mvOC seems to be related to both primary and secondary biomass burning sources.
Jing Duan, Ru-Jin Huang, Chunshui Lin, Wenting Dai, Meng Wang, Yifang Gu, Ying Wang, Haobin Zhong, Yan Zheng, Haiyan Ni, Uli Dusek, Yang Chen, Yongjie Li, Qi Chen, Douglas R. Worsnop, Colin D. O'Dowd, and Junji Cao
Atmos. Chem. Phys., 19, 10319–10334, https://doi.org/10.5194/acp-19-10319-2019, https://doi.org/10.5194/acp-19-10319-2019, 2019
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We present the seasonal distinction of secondary aerosol formation in urban Beijing. Both photochemical oxidation and aqueous-phase processing played important roles in SOA (secondary organic aerosol) formation during all three seasons; while for sulfate formation, gas-phase photochemical oxidation was the major pathway in late summer, aqueous-phase reactions were more responsible during early winter, and both processes had contributions during autumn.
Yunfei Wu, Yunjie Xia, Rujin Huang, Zhaoze Deng, Ping Tian, Xiangao Xia, and Renjian Zhang
Atmos. Meas. Tech., 12, 4347–4359, https://doi.org/10.5194/amt-12-4347-2019, https://doi.org/10.5194/amt-12-4347-2019, 2019
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The morphology and effective density of externally mixed black carbon (extBC) aerosols were studied using a tandem technique coupling a DMA with a SP2. The study extended the mass–mobility relationship to large extBC with a mobility diameter larger than 350 nm, a size range seldom included in previous tandem measurements of BC aggregates. On this basis, quantities such as the mass–mobility scaling exponent were revealed for extBC in urban Beijing.
Kun Li, Junling Li, Shengrui Tong, Weigang Wang, Ru-Jin Huang, and Maofa Ge
Atmos. Chem. Phys., 19, 8021–8036, https://doi.org/10.5194/acp-19-8021-2019, https://doi.org/10.5194/acp-19-8021-2019, 2019
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Wintertime volatile organic compounds (VOCs) in suburban and urban Beijing were measured. Urban VOC concentrations were much higher than suburban ones, but the emission features were similar. The photochemical processes were more active in the urban site, resulting in the high daytime formation of oxygenated VOCs. In addition, human activities during holidays can largely influence the VOC levels. These results are helpful in better understanding the atmospheric chemistry of VOCs in Beijing.
Yang Chen, Mi Tian, Ru-Jin Huang, Guangming Shi, Huanbo Wang, Chao Peng, Junji Cao, Qiyuan Wang, Shumin Zhang, Dongmei Guo, Leiming Zhang, and Fumo Yang
Atmos. Chem. Phys., 19, 3245–3255, https://doi.org/10.5194/acp-19-3245-2019, https://doi.org/10.5194/acp-19-3245-2019, 2019
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Amine-containing particles were characterized in an urban area of Chongqing during both summer and winter using a single-particle aerosol mass spectrometer (SPAMS). Amines were observed to internally mix with elemental carbon (EC), organic carbon (OC), sulfate, and nitrate. Diethylamine (DEA) was the most abundant in both number and peak area among amine-containing particles. Vegetation and traffic were the primary sources of particulate amines.
Li Xing, Jiarui Wu, Miriam Elser, Shengrui Tong, Suixin Liu, Xia Li, Lang Liu, Junji Cao, Jiamao Zhou, Imad El-Haddad, Rujin Huang, Maofa Ge, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 19, 2343–2359, https://doi.org/10.5194/acp-19-2343-2019, https://doi.org/10.5194/acp-19-2343-2019, 2019
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We used the WRF-CHEM model to simulate wintertime secondary organic aerosol (SOA) concentrations over Beijing–Tianjin–Hebei (BTH), China. Heterogeneous HONO sources increased the near-surface SOA by 46.3 % in BTH. Direct emissions of glyoxal and methylglyoxal from residential sources contributed 25.5 % to the total SOA mass. Our study highlights the importance of heterogeneous HONO sources and primary residential emissions of glyoxal and methylglyoxal to SOA formation in winter over BTH.
Mingjin Tang, Wenjun Gu, Qingxin Ma, Yong Jie Li, Cheng Zhong, Sheng Li, Xin Yin, Ru-Jin Huang, Hong He, and Xinming Wang
Atmos. Chem. Phys., 19, 2247–2258, https://doi.org/10.5194/acp-19-2247-2019, https://doi.org/10.5194/acp-19-2247-2019, 2019
Haiyan Ni, Ru-Jin Huang, Junji Cao, Weiguo Liu, Ting Zhang, Meng Wang, Harro A. J. Meijer, and Ulrike Dusek
Atmos. Chem. Phys., 18, 16363–16383, https://doi.org/10.5194/acp-18-16363-2018, https://doi.org/10.5194/acp-18-16363-2018, 2018
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Seasonal changes in organic carbon (OC) and elemental carbon (EC) sources in Xi'an, China, are investigated based on measurements of radiocarbon and the stable isotope 13C. Relative contributions to EC from biomass burning, coal combustion, and vehicle emissions change substantially between different seasons. Biomass burning contributes 60 % to the EC increment in winter. Comparing concentrations and sources of primary OC to total OC suggests non-negligible OC loss due to active photochemistry.
Xia Li, Jiarui Wu, Miriam Elser, Tian Feng, Junji Cao, Imad El-Haddad, Rujin Huang, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 18, 10675–10691, https://doi.org/10.5194/acp-18-10675-2018, https://doi.org/10.5194/acp-18-10675-2018, 2018
Ru-Jin Huang, Junji Cao, Yang Chen, Lu Yang, Jincan Shen, Qihua You, Kai Wang, Chunshui Lin, Wei Xu, Bo Gao, Yongjie Li, Qi Chen, Thorsten Hoffmann, Colin D. O'Dowd, Merete Bilde, and Marianne Glasius
Atmos. Meas. Tech., 11, 3447–3456, https://doi.org/10.5194/amt-11-3447-2018, https://doi.org/10.5194/amt-11-3447-2018, 2018
Doğuşhan Kılıç, Imad El Haddad, Benjamin T. Brem, Emily Bruns, Carlo Bozetti, Joel Corbin, Lukas Durdina, Ru-Jin Huang, Jianhui Jiang, Felix Klein, Avi Lavi, Simone M. Pieber, Theo Rindlisbacher, Yinon Rudich, Jay G. Slowik, Jing Wang, Urs Baltensperger, and Andre S. H. Prévôt
Atmos. Chem. Phys., 18, 7379–7391, https://doi.org/10.5194/acp-18-7379-2018, https://doi.org/10.5194/acp-18-7379-2018, 2018
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We study primary emissions and secondary aerosol (SA) from an aircraft turbofan. By monitoring the chemical composition of both gaseous and particulate emissions at different engine loads, we explained SA formed in an oxidation flow reactor (PAM) by the oxidation of gaseous species. At idle, more than 90 % of the secondary particle mass was organic and could be explained by the oxidation of gaseous aromatic species, while at an approximated cruise load sulfates comprised 85 % of the total SA.
Yan-Lin Zhang, Imad El-Haddad, Ru-Jin Huang, Kin-Fai Ho, Jun-Ji Cao, Yongming Han, Peter Zotter, Carlo Bozzetti, Kaspar R. Daellenbach, Jay G. Slowik, Gary Salazar, André S. H. Prévôt, and Sönke Szidat
Atmos. Chem. Phys., 18, 4005–4017, https://doi.org/10.5194/acp-18-4005-2018, https://doi.org/10.5194/acp-18-4005-2018, 2018
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Here we present a quantitative source apportionment of WSOC, isolated from aerosols in China using radiocarbon (14C) and offline high-resolution time of flight aerosol mass spectrometer measurements. We demonstrate a dominant contribution of non-fossil emissions to WSOC aerosols in the Northern Hemisphere. However, the fossil fraction is substantially larger in aerosols from East Asia and the east Asian pollution outflow, especially during winter, due to increasing coal combustion.
Naifang Bei, Jiarui Wu, Miriam Elser, Tian Feng, Junji Cao, Imad El-Haddad, Xia Li, Rujin Huang, Zhengqiang Li, Xin Long, Li Xing, Shuyu Zhao, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 17, 14579–14591, https://doi.org/10.5194/acp-17-14579-2017, https://doi.org/10.5194/acp-17-14579-2017, 2017
Yunfei Wu, Xiaojia Wang, Jun Tao, Rujin Huang, Ping Tian, Junji Cao, Leiming Zhang, Kin-Fai Ho, Zhiwei Han, and Renjian Zhang
Atmos. Chem. Phys., 17, 7965–7975, https://doi.org/10.5194/acp-17-7965-2017, https://doi.org/10.5194/acp-17-7965-2017, 2017
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As black carbon (BC) aerosols play an important role in the climate and environment, the size distribution of refractory BC (rBC) was investigated. On this basis, the source of rBC was further analyzed. The local traffic exhausts contributed greatly to the rBC in urban areas. However, its contribution decreased significantly in the polluted period compared to the clean period, implying the increasing contribution of other sources, e.g., coal combustion or biomass burning, in the polluted period.
Guohui Li, Naifang Bei, Junji Cao, Rujin Huang, Jiarui Wu, Tian Feng, Yichen Wang, Suixin Liu, Qiang Zhang, Xuexi Tie, and Luisa T. Molina
Atmos. Chem. Phys., 17, 3301–3316, https://doi.org/10.5194/acp-17-3301-2017, https://doi.org/10.5194/acp-17-3301-2017, 2017
Jiarui Wu, Guohui Li, Junji Cao, Naifang Bei, Yichen Wang, Tian Feng, Rujin Huang, Suixin Liu, Qiang Zhang, and Xuexi Tie
Atmos. Chem. Phys., 17, 2035–2051, https://doi.org/10.5194/acp-17-2035-2017, https://doi.org/10.5194/acp-17-2035-2017, 2017
Tian Feng, Guohui Li, Junji Cao, Naifang Bei, Zhenxing Shen, Weijian Zhou, Suixin Liu, Ting Zhang, Yichen Wang, Ru-jin Huang, Xuexi Tie, and Luisa T. Molina
Atmos. Chem. Phys., 16, 10045–10061, https://doi.org/10.5194/acp-16-10045-2016, https://doi.org/10.5194/acp-16-10045-2016, 2016
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The springtime organic aerosol (OA) concentrations in the Guanzhong Basin, China are simulated using the WRF-Chem model with two secondary OA (SOA) modules. Model results are verified with near-surface observations. The non-traditional SOA module significantly improves SOA simulation. Oxidation and partitioning of primary OAs is the most important pathway in SOA formation. Residential emissions are the dominant anthropogenic OA source.
Xin Long, Xuexi Tie, Junji Cao, Rujin Huang, Tian Feng, Nan Li, Suyu Zhao, Jie Tian, Guohui Li, and Qiang Zhang
Atmos. Chem. Phys., 16, 9675–9691, https://doi.org/10.5194/acp-16-9675-2016, https://doi.org/10.5194/acp-16-9675-2016, 2016
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We studied the impact of crop field burning (CFB) on air pollution in North China Plain (NCP) using MODIS observations and the numerical model WRF-CHEM. The CFB plume emitted in southern NCP and went through a long-range transport to northern NCP. The long-range transport and the effect of mountains obviously enhanced the PM2.5 pollution in northern NCP. The prohibition of CFB should be strict not just in or around Beijing, but also on the ulterior crop growth areas of southern NCP.
Naifang Bei, Guohui Li, Ru-Jin Huang, Junji Cao, Ning Meng, Tian Feng, Suixin Liu, Ting Zhang, Qiang Zhang, and Luisa T. Molina
Atmos. Chem. Phys., 16, 7373–7387, https://doi.org/10.5194/acp-16-7373-2016, https://doi.org/10.5194/acp-16-7373-2016, 2016
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Rapid industrialization and urbanization have caused severe air pollution in the Guanzhong basin, northwestern China with heavy haze events occurring frequently in recent winters. Due to frequent occurrence of unfavorable synoptic situations during wintertime, mitigation of emissions is the optimum approach to mitigate the air pollution in the Guanzhong basin.
Tian Feng, Naifang Bei, Ru-Jin Huang, Junji Cao, Qiang Zhang, Weijian Zhou, Xuexi Tie, Suixin Liu, Ting Zhang, Xiaoli Su, Wenfang Lei, Luisa T. Molina, and Guohui Li
Atmos. Chem. Phys., 16, 4323–4342, https://doi.org/10.5194/acp-16-4323-2016, https://doi.org/10.5194/acp-16-4323-2016, 2016
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The occurrence of high O3 levels with high PM2.5 concentrations constitutes a dilemma for the design of O3 control strategies in Xi’an and surrounding areas. If the O3 mitigation approach decreases aerosols in the atmosphere directly or indirectly, the enhanced photolysis caused by aerosol reduction would compensate for the O3 loss. If only the PM2.5 control strategy is implemented, the O3 pollution will decrease.
Miriam Elser, Ru-Jin Huang, Robert Wolf, Jay G. Slowik, Qiyuan Wang, Francesco Canonaco, Guohui Li, Carlo Bozzetti, Kaspar R. Daellenbach, Yu Huang, Renjian Zhang, Zhengqiang Li, Junji Cao, Urs Baltensperger, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 3207–3225, https://doi.org/10.5194/acp-16-3207-2016, https://doi.org/10.5194/acp-16-3207-2016, 2016
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This work represents the first online chemical characterization of the PM2.5 using a high-resolution time-of flight aerosol mass spectrometer during extreme haze events China. The application of novel source apportionment techniques allowed for an improved identification and quantification of the sources of organic aerosols. The main sources and processes driving the extreme haze events are assessed.
K. R. Daellenbach, C. Bozzetti, A. Křepelová, F. Canonaco, R. Wolf, P. Zotter, P. Fermo, M. Crippa, J. G. Slowik, Y. Sosedova, Y. Zhang, R.-J. Huang, L. Poulain, S. Szidat, U. Baltensperger, I. El Haddad, and A. S. H. Prévôt
Atmos. Meas. Tech., 9, 23–39, https://doi.org/10.5194/amt-9-23-2016, https://doi.org/10.5194/amt-9-23-2016, 2016
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In this study, we developed an offline technique using the AMS for the characterization of the chemical fingerprints of aerosols collected on quartz filters, and evaluated the suitability of the organic mass spectral data for source apportionment. This technique may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved long-term data sets.
Q. Y. Wang, R.-J. Huang, J. J. Cao, X. X. Tie, H. Y. Ni, Y. Q. Zhou, Y. M. Han, T. F. Hu, C. S. Zhu, T. Feng, N. Li, and J. D. Li
Atmos. Chem. Phys., 15, 13059–13069, https://doi.org/10.5194/acp-15-13059-2015, https://doi.org/10.5194/acp-15-13059-2015, 2015
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An intensive campaign was conducted at the Qinghai-Tibetan Plateau using a ground-based single particle soot photometer and a photoacoustic extinctiometer. Significant enhancements of rBC loadings and number fraction of coated rBC were observed during the pollution episode. Biomass burning from N. India is determined to be an important potential source influencing the northeastern Qinghai-Tibetan Plateau. The rBC mixing state is important in determining absorption during the pollution episode.
K. F. Ho, R.-J. Huang, K. Kawamura, E. Tachibana, S. C. Lee, S. S. H. Ho, T. Zhu, and L. Tian
Atmos. Chem. Phys., 15, 3111–3123, https://doi.org/10.5194/acp-15-3111-2015, https://doi.org/10.5194/acp-15-3111-2015, 2015
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The objective of this study is to identify the influence of traffic emissions and regional transport to the atmosphere in Beijing during the CAREBeijing-2007 in summer. This study demonstrates that even when primary exhaust was controlled by traffic restrictions, the contribution of secondary organic species formed from photochemical processes was critical with long-range atmospheric transport of pollutants.
Y.-L. Zhang, R.-J. Huang, I. El Haddad, K.-F. Ho, J.-J. Cao, Y. Han, P. Zotter, C. Bozzetti, K. R. Daellenbach, F. Canonaco, J. G. Slowik, G. Salazar, M. Schwikowski, J. Schnelle-Kreis, G. Abbaszade, R. Zimmermann, U. Baltensperger, A. S. H. Prévôt, and S. Szidat
Atmos. Chem. Phys., 15, 1299–1312, https://doi.org/10.5194/acp-15-1299-2015, https://doi.org/10.5194/acp-15-1299-2015, 2015
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Source apportionment of fine carbonaceous aerosols using radiocarbon and other organic markers measurements during 2013 winter haze episodes was conducted at four megacities in China. Our results demonstrate that fossil emissions predominate EC with a mean contribution of 75±8%, whereas non-fossil sources account for 55±10% of OC; and the increment of TC on heavily polluted days was mainly driven by the increase of secondary OC from both fossil-fuel and non-fossil emissions.
P. Zotter, V. G. Ciobanu, Y. L. Zhang, I. El-Haddad, M. Macchia, K. R. Daellenbach, G. A. Salazar, R.-J. Huang, L. Wacker, C. Hueglin, A. Piazzalunga, P. Fermo, M. Schwikowski, U. Baltensperger, S. Szidat, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 13551–13570, https://doi.org/10.5194/acp-14-13551-2014, https://doi.org/10.5194/acp-14-13551-2014, 2014
U. R. Thorenz, L. J. Carpenter, R.-J. Huang, M. Kundel, J. Bosle, and T. Hoffmann
Atmos. Chem. Phys., 14, 13327–13335, https://doi.org/10.5194/acp-14-13327-2014, https://doi.org/10.5194/acp-14-13327-2014, 2014
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Phytoplankton suspensions were treated with high and low ozone levels, and volatile iodine (I2)-containing compounds were measured. Iodocarbon emissions were independent of the ozone level. I2 emission showed a strong dependency on the ozone level in the air as well as on the iodide concentration in the sample suspension. The experiments show that microalgae suspensions are capable of emitting I2 by the reaction of ozone with dissolved iodide at the air-water interface under natural conditions.
R.-J. Huang, W.-B. Li, Y.-R. Wang, Q. Y. Wang, W. T. Jia, K.-F. Ho, J. J. Cao, G. H. Wang, X. Chen, I. EI Haddad, Z. X. Zhuang, X. R. Wang, A. S. H. Prévôt, C. D. O'Dowd, and T. Hoffmann
Atmos. Meas. Tech., 7, 2027–2035, https://doi.org/10.5194/amt-7-2027-2014, https://doi.org/10.5194/amt-7-2027-2014, 2014
R.-J. Huang, U. R. Thorenz, M. Kundel, D. S. Venables, D. Ceburnis, K. F. Ho, J. Chen, A. L. Vogel, F. C. Küpper, P. P. A. Smyth, U. Nitschke, D. B. Stengel, H. Berresheim, C. D. O'Dowd, and T. Hoffmann
Atmos. Chem. Phys., 13, 5255–5264, https://doi.org/10.5194/acp-13-5255-2013, https://doi.org/10.5194/acp-13-5255-2013, 2013
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
EGUsphere, https://doi.org/10.5194/egusphere-2022-1317, https://doi.org/10.5194/egusphere-2022-1317, 2022
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Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOM) from α-pinene ozonolysis, enhancement of C16-C19 HOM dimers in particles was observed. Especially, C17H26Oz, which has often been reported by offline measurements, dominates the particle-phase HOM. Our results indicate that these C17 compounds might be closely related to particle-phase HOM formation. These results are important for a better understanding of SOA formation in the atmosphere.
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.
Vaishali Jain, Sachchida N. Tripathi, Nidhi Tripathi, Mansi Gupta, Lokesh K. Sahu, Vishnu Murari, Sreenivas Gaddamidi, Ashutosh K. Shukla, and Andre S. H. Prevot
EGUsphere, https://doi.org/10.5194/egusphere-2022-1165, https://doi.org/10.5194/egusphere-2022-1165, 2022
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This research chemically characterises 173 different NMVOCs (non-methane volatile organic compounds) measured in real-time for three seasons in the urban city of the central Indo-Gangetic Basin of India, Lucknow. Receptor modelling is used to analyze probable sources of NMVOCs and their crucial role in forming ozone and secondary organic aerosols. It is observed that vehicular emissions and solid fuel combustion are the most contributing towards the emission of primary and secondary NMVOCs.
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. Discuss., https://doi.org/10.5194/acp-2022-725, https://doi.org/10.5194/acp-2022-725, 2022
Preprint under review for ACP
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This work investigated seasonal variation of aerosol Fe solubility for coarse and fine particles in Xi’an, a megacity severely in northwestern China 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.
David M. Bell, Cheng Wu, Amelie Bertrand, Emelie Graham, Janne Schoonbaert, Stamatios Giannoukos, Urs Baltensperger, Andre S. H. Prevot, Ilona Riipinen, Imad El Haddad, and Claudia Mohr
Atmos. Chem. Phys., 22, 13167–13182, https://doi.org/10.5194/acp-22-13167-2022, https://doi.org/10.5194/acp-22-13167-2022, 2022
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A series of studies designed to investigate the evolution of organic aerosol were performed in an atmospheric simulation chamber, using a common oxidant found at night (NO3). The chemical composition steadily changed from its initial composition via different chemical reactions that were taking place inside of the aerosol particle. These results show that the composition of organic aerosol steadily changes during its lifetime in the atmosphere.
Emelie L. Graham, Cheng Wu, David M. Bell, Amelie Bertrand, Sophie L. Haslett, Urs Baltensperger, Imad El Haddad, Radovan Krejci, Ilona Riipinen, and Claudia Mohr
EGUsphere, https://doi.org/10.5194/egusphere-2022-1043, https://doi.org/10.5194/egusphere-2022-1043, 2022
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The volatility of an aerosol particle is an important parameter for describing its atmospheric lifetime. We studied the volatility of secondary organic aerosols from nitrate initiated oxidation of three biogenic precursors with experimental methods and model simulations. We saw higher volatility than for the corresponding ozone system and our simulations produced variable results with different parameterizations which warrant for a re-evaluation of the treatment of the nitrate functional group.
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.
Ella Häkkinen, Jian Zhao, Frans Graeffe, Nicolas Fauré, Jordan Krechmer, Douglas Worsnop, Hilkka Timonen, Mikael Ehn, and Juha Kangasluoma
EGUsphere, https://doi.org/10.5194/egusphere-2022-933, https://doi.org/10.5194/egusphere-2022-933, 2022
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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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.
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 Cai, Kaspar Daellenbach, Cheng Wu, Yan Zheng, Feixue Zheng, Wei Du, Sophie Haslett, Qi Chen, Markku Kulmala, and Claudia Mohr
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-248, https://doi.org/10.5194/amt-2022-248, 2022
Preprint under review for AMT
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In this manuscript, 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 described 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.
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. Discuss., https://doi.org/10.5194/acp-2022-573, https://doi.org/10.5194/acp-2022-573, 2022
Preprint under review for ACP
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Secondary organic aerosol (SOA) could be produced by various pathways but its formation mechanisms are unclear. Observations were conducted in North China Plain during a highly oxidizing atmosphere in summer. We found here 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.
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. Discuss., https://doi.org/10.5194/acp-2022-498, https://doi.org/10.5194/acp-2022-498, 2022
Preprint under review for ACP
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In this study, we present an intercomparison study 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.
Tingting Feng, Yingkun Wang, Weiwei Hu, Ming Zhu, Wei Song, Wei Chen, Yanyan Sang, Zheng Fang, Wei Deng, Hua Fang, Xu Yu, Cheng Wu, Bin Yuan, Shan Huang, Min Shao, Xiaofeng Huang, Lingyan He, Young Ro Lee, L. Gregory Huey, Francesco Canonaco, Andre S. H. Prevot, and Xinming Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-575, https://doi.org/10.5194/acp-2022-575, 2022
Revised manuscript accepted for ACP
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To investigate the impact of aging processes on the organic aerosols (OA), we conducted a comprehensive field study at a continental remote site using on-line mass spectrometers. The results show that OA in the Chinese outflows was strongly influenced by upwind anthropogenic emissions. The aging processes can significantly decrease the OA volatility and result in a varied viscosity of OA under different circumstances, signifying the complex physiochemistry properties of OA in the aged plumes.
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. Discuss., https://doi.org/10.5194/acp-2022-566, https://doi.org/10.5194/acp-2022-566, 2022
Revised manuscript accepted for ACP
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The atmospheric oxidation of dimethyl sulfide (DMS) represents a major natural source of sulfate aerosols, and thus plays an important role in global aerosol climate effects. However, the mechanism is poorly constrained. In this work, laboratory measurements were conducted to comprehensively investigate DMS oxidation products. The results show that peroxy radical (RO2) fate has a controlling influence on product distributions, and the isomerization of RO2 suppresses aerosol formation.
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.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Josef Dommen, Mao Xiao, Xueqin Zhou, Andrea Baccarini, Stamatios Giannoukos, Günther Wehrle, Pascal André Schneider, Andre S. H. Prevot, Jay G. Slowik, Houssni Lamkaddam, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 15, 3747–3760, https://doi.org/10.5194/amt-15-3747-2022, https://doi.org/10.5194/amt-15-3747-2022, 2022
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Real-time detection of both the gas and particle phase is needed to elucidate the sources and chemical reaction pathways of organic vapors and particulate matter. The Dual-EESI was developed to measure gas- and particle-phase species to provide new insights into aerosol sources or formation mechanisms. After characterizing the relative gas and particle response factors of EESI via organic aerosol uptake experiments, the Dual-EESI is more sensitive toward gas-phase analyes.
Varun Kumar, Stamatios Giannoukos, Sophie L. Haslett, Yandong Tong, Atinderpal Singh, Amelie Bertrand, Chuan Ping Lee, Dongyu S. Wang, Deepika Bhattu, Giulia Stefenelli, Jay S. Dave, Joseph V. Puthussery, Lu Qi, Pawan Vats, Pragati Rai, Roberto Casotto, Rangu Satish, Suneeti Mishra, Veronika Pospisilova, Claudia Mohr, David M. Bell, Dilip Ganguly, Vishal Verma, Neeraj Rastogi, Urs Baltensperger, Sachchida N. Tripathi, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 22, 7739–7761, https://doi.org/10.5194/acp-22-7739-2022, https://doi.org/10.5194/acp-22-7739-2022, 2022
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Here we present source apportionment results from the first field deployment in Delhi of an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF). The EESI-TOF is a recently developed instrument capable of providing uniquely detailed online chemical characterization of organic aerosol (OA), in particular the secondary OA (SOA) fraction. Here, we are able to apportion not only primary OA but also SOA to specific sources, which is performed for the first time in Delhi.
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.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2857–2874, https://doi.org/10.5194/amt-15-2857-2022, https://doi.org/10.5194/amt-15-2857-2022, 2022
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While the aerosol mass spectrometer provides high-time-resolution characterization of the overall extent of oxidation, the extensive fragmentation of molecules and specificity of the technique have posed challenges toward deeper understanding of molecular structures in aerosols. This work demonstrates how functional group information can be extracted from a suite of commonly measured mass fragments using collocated infrared spectroscopy measurements.
Yandong Tong, Lu Qi, Giulia Stefenelli, Dongyu Simon Wang, Francesco Canonaco, Urs Baltensperger, André Stephan Henry Prévôt, and Jay Gates Slowik
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-78, https://doi.org/10.5194/amt-2022-78, 2022
Revised manuscript accepted for AMT
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We present a method for positive matrix factorisation (PMF) analysis on a single dataset that includes measurements from both EESI-TOF and AMS in Zurich, Switzerland. For the first time, we resolved and quantified secondary organic aerosol (SOA) sources. Meanwhile, we also determined the retrieved EESI-TOF factor-dependent sensitivities. This method provides a framework for exploiting semi-quantitative, high-resolution instrumentation for quantitative source apportionment.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
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.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Dongyu S. Wang, Chuan Ping Lee, Jordan E. Krechmer, Francesca Majluf, Yandong Tong, Manjula R. Canagaratna, Julia Schmale, André S. H. Prévôt, Urs Baltensperger, Josef Dommen, Imad El Haddad, Jay G. Slowik, and David M. Bell
Atmos. Meas. Tech., 14, 6955–6972, https://doi.org/10.5194/amt-14-6955-2021, https://doi.org/10.5194/amt-14-6955-2021, 2021
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To understand the sources and fate of particulate matter in the atmosphere, the ability to quantitatively describe its chemical composition is essential. In this work, we developed a calibration method for a state-of-the-art measurement technique without the need for chemical standards. Statistical analyses identified the driving factors behind instrument sensitivity variability towards individual components of particulate matter.
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.
Gang Chen, Yulia Sosedova, Francesco Canonaco, Roman Fröhlich, Anna Tobler, Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Christoph Hueglin, Peter Graf, Urs Baltensperger, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 15081–15101, https://doi.org/10.5194/acp-21-15081-2021, https://doi.org/10.5194/acp-21-15081-2021, 2021
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A novel, advanced source apportionment technique was applied to a dataset measured in Magadino. Rolling positive matrix factorisation (PMF) allows for retrieving more realistic, time-dependent, and detailed information on organic aerosol sources. The strength of the rolling PMF mechanism is highlighted by comparing it with results derived from conventional seasonal PMF. Overall, this comprehensive interpretation of aerosol chemical speciation monitor data could be a role model for similar work.
Wenfei Zhu, Song Guo, Zirui Zhang, Hui Wang, Ying Yu, Zheng Chen, Ruizhe Shen, Rui Tan, Kai Song, Kefan Liu, Rongzhi Tang, Yi Liu, Shengrong Lou, Yuanju Li, Wenbin Zhang, Zhou Zhang, Shijin Shuai, Hongming Xu, Shuangde Li, Yunfa Chen, Min Hu, Francesco Canonaco, and Andre S. H. Prévôt
Atmos. Chem. Phys., 21, 15065–15079, https://doi.org/10.5194/acp-21-15065-2021, https://doi.org/10.5194/acp-21-15065-2021, 2021
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The experiments of primary emissions and secondary organic aerosol (SOA) formation from urban lifestyle sources (cooking and vehicles) were conducted. The mass spectral features of primary organic aerosol (POA) and SOA were characterized by using a high-resolution time-of-flight aerosol mass spectrometer. This work, for the first time, establishes the vehicle and cooking SOA source profiles and can be further used as source constraints in the OA source apportionment in the ambient atmosphere.
Chenyang Bi, Jordan E. Krechmer, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6551–6560, https://doi.org/10.5194/amt-14-6551-2021, https://doi.org/10.5194/amt-14-6551-2021, 2021
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Calibration techniques have been recently developed to log-linearly correlate analyte sensitivity with CIMS operating conditions particularly for compounds without authentic standards. In this work, we examine the previously ignored bias in the log-linear-based calibration method and estimate an average bias of 30 %, with 1 order of magnitude for less sensitive compounds in some circumstances. A step-by-step guide was provided to reduce and even remove the bias.
Rebecca A. Wernis, Nathan M. Kreisberg, Robert J. Weber, Yutong Liang, John Jayne, Susanne Hering, and Allen H. Goldstein
Atmos. Meas. Tech., 14, 6533–6550, https://doi.org/10.5194/amt-14-6533-2021, https://doi.org/10.5194/amt-14-6533-2021, 2021
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cTAG is a new scientific instrument that measures concentrations of organic chemicals in the atmosphere. cTAG is the first instrument capable of measuring small, light chemicals as well as heavier chemicals and everything in between on a single detector, every hour. In this work we explain how cTAG works and some of the tests we performed to verify that it works properly and reliably. We also present measurements of alkanes that suggest they have three dominant sources in a Bay Area suburb.
Anna K. Tobler, Alicja Skiba, Francesco Canonaco, Griša Močnik, Pragati Rai, Gang Chen, Jakub Bartyzel, Miroslaw Zimnoch, Katarzyna Styszko, Jaroslaw Nęcki, Markus Furger, Kazimierz Różański, Urs Baltensperger, Jay G. Slowik, and Andre S. H. Prevot
Atmos. Chem. Phys., 21, 14893–14906, https://doi.org/10.5194/acp-21-14893-2021, https://doi.org/10.5194/acp-21-14893-2021, 2021
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Kraków is among the cities with the highest particulate matter levels within Europe. We conducted long-term and highly time-resolved measurements of the chemical composition of submicron particlulate matter (PM1). Combined with advanced source apportionment techniques, which allow for time-dependent factor profiles, our results elucidate that traffic and residential heating (biomass burning and coal combustion) as well as oxygenated organic aerosol are the key PM sources in Kraków.
Cheng Wu, David M. Bell, Emelie L. Graham, Sophie Haslett, Ilona Riipinen, Urs Baltensperger, Amelie Bertrand, Stamatios Giannoukos, Janne Schoonbaert, Imad El Haddad, Andre S. H. Prevot, Wei Huang, and Claudia Mohr
Atmos. Chem. Phys., 21, 14907–14925, https://doi.org/10.5194/acp-21-14907-2021, https://doi.org/10.5194/acp-21-14907-2021, 2021
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Night-time reactions of biogenic volatile organic compounds and nitrate radicals can lead to the formation of secondary organic aerosol (BSOANO3). Here, we study the impacts of light exposure on the BSOANO3 from three biogenic precursors. Our results suggest that photolysis causes photodegradation of a substantial fraction of BSOANO3, changes the chemical composition and bulk volatility, and might be a potentially important loss pathway of BSOANO3 during the night-to-day transition.
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.
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.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Houssni Lamkaddam, Mingyi Wang, Farnoush Ataei, Victoria Hofbauer, Brandon Lopez, Neil M. Donahue, Josef Dommen, Andre S. H. Prevot, Jay G. Slowik, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 14, 5913–5923, https://doi.org/10.5194/amt-14-5913-2021, https://doi.org/10.5194/amt-14-5913-2021, 2021
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Extractive electrospray ionization mass spectrometry (EESI-MS) has been deployed for high throughput online detection of particles with minimal fragmentation. Our study elucidates the extraction mechanism between the particles and electrospray (ES) droplets of different properties. The results show that the extraction rate is likely affected by the coagulation rate between the particles and ES droplets. Once coagulated, the particles undergo complete extraction within the ES droplet.
Vaios Moschos, Martin Gysel-Beer, Robin L. Modini, Joel C. Corbin, Dario Massabò, Camilla Costa, Silvia G. Danelli, Athanasia Vlachou, Kaspar R. Daellenbach, Sönke Szidat, Paolo Prati, André S. H. Prévôt, Urs Baltensperger, and Imad El Haddad
Atmos. Chem. Phys., 21, 12809–12833, https://doi.org/10.5194/acp-21-12809-2021, https://doi.org/10.5194/acp-21-12809-2021, 2021
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This study provides a holistic approach to studying the spectrally resolved light absorption by atmospheric brown carbon (BrC) and black carbon using long time series of daily samples from filter-based measurements. The obtained results provide (1) a better understanding of the aerosol absorption profile and its dependence on BrC and on lensing from less absorbing coatings and (2) an estimation of the most important absorbers at typical European locations.
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.
Louise N. Jensen, Manjula R. Canagaratna, Kasper Kristensen, Lauriane L. J. Quéléver, Bernadette Rosati, Ricky Teiwes, Marianne Glasius, Henrik B. Pedersen, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 21, 11545–11562, https://doi.org/10.5194/acp-21-11545-2021, https://doi.org/10.5194/acp-21-11545-2021, 2021
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This work targets the chemical composition of α-pinene-derived secondary organic aerosol (SOA) formed in the temperature range from -15 to 20°C. Experiments were conducted in an atmospheric simulation chamber. Positive matrix factorization analysis of data obtained by a high-resolution time-of-flight aerosol mass spectrometer shows that the elemental aerosol composition is controlled by the initial α-pinene concentration and temperature during SOA formation.
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.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Evelyn Freney, Karine Sellegri, Alessia Nicosia, Leah R. Williams, Matteo Rinaldi, Jonathan T. Trueblood, André S. H. Prévôt, Melilotus Thyssen, Gérald Grégori, Nils Haëntjens, Julie Dinasquet, Ingrid Obernosterer, France Van Wambeke, Anja Engel, Birthe Zäncker, Karine Desboeufs, Eija Asmi, Hilkka Timonen, and Cécile Guieu
Atmos. Chem. Phys., 21, 10625–10641, https://doi.org/10.5194/acp-21-10625-2021, https://doi.org/10.5194/acp-21-10625-2021, 2021
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In this work, we present observations of the organic aerosol content in primary sea spray aerosols (SSAs) continuously generated along a 5-week cruise in the Mediterranean. This information is combined with seawater biogeochemical properties also measured continuously along the ship track to develop a number of parametrizations that can be used in models to determine SSA organic content in oligotrophic waters that represent 60 % of the oceans from commonly measured seawater variables.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Chem. Phys., 21, 10273–10293, https://doi.org/10.5194/acp-21-10273-2021, https://doi.org/10.5194/acp-21-10273-2021, 2021
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Functional group compositions of primary and aged aerosols from wood burning and coal combustion sources from chamber experiments are interpreted through compounds present in the fuels and known gas-phase oxidation products. Infrared spectra of aged wood burning in the chamber and ambient biomass burning samples reveal striking similarities, and a new method for identifying burning-impacted samples in monitoring network measurements is presented.
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.
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.
Siqi Hou, Di Liu, Jingsha Xu, Tuan V. Vu, Xuefang Wu, Deepchandra Srivastava, Pingqing Fu, Linjie Li, Yele Sun, Athanasia Vlachou, Vaios Moschos, Gary Salazar, Sönke Szidat, André S. H. Prévôt, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 8273–8292, https://doi.org/10.5194/acp-21-8273-2021, https://doi.org/10.5194/acp-21-8273-2021, 2021
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This study provides a newly developed method which combines radiocarbon (14C) with organic tracers to enable source apportionment of primary and secondary fossil vs. non-fossil sources of carbonaceous aerosols at an urban and a rural site of Beijing. The source apportionment results were compared with those by chemical mass balance and AMS/ACSM-PMF methods. Correlations of WINSOC and WSOC with different sources of OC were also performed to elucidate the formation mechanisms of SOC.
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).
Karl Espen Yttri, Francesco Canonaco, Sabine Eckhardt, Nikolaos Evangeliou, Markus Fiebig, Hans Gundersen, Anne-Gunn Hjellbrekke, Cathrine Lund Myhre, Stephen Matthew Platt, André S. H. Prévôt, David Simpson, Sverre Solberg, Jason Surratt, Kjetil Tørseth, Hilde Uggerud, Marit Vadset, Xin Wan, and Wenche Aas
Atmos. Chem. Phys., 21, 7149–7170, https://doi.org/10.5194/acp-21-7149-2021, https://doi.org/10.5194/acp-21-7149-2021, 2021
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Carbonaceous aerosol sources and trends were studied at the Birkenes Observatory. A large decrease in elemental carbon (EC; 2001–2018) and a smaller decline in levoglucosan (2008–2018) suggest that organic carbon (OC)/EC from traffic/industry is decreasing, whereas the abatement of OC/EC from biomass burning has been less successful. Positive matrix factorization apportioned 72 % of EC to fossil fuel sources and 53 % (PM2.5) and 78 % (PM10–2.5) of OC to biogenic sources.
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.
Mutian Ma, Laura-Hélèna Rivellini, YuXi Cui, Megan D. Willis, Rio Wilkie, Jonathan P. D. Abbatt, Manjula R. Canagaratna, Junfeng Wang, Xinlei Ge, and Alex K. Y. Lee
Atmos. Meas. Tech., 14, 2799–2812, https://doi.org/10.5194/amt-14-2799-2021, https://doi.org/10.5194/amt-14-2799-2021, 2021
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Chemical characterization of organic coatings is important to advance our understanding of the physio-chemical properties and atmospheric processing of black carbon (BC) particles. This work develops two approaches to improve the elemental analysis of oxygenated organic coatings using a soot-particle aerosol mass spectrometer. Analyzing ambient data with the new approaches indicated that secondary organics that coated on BC were likely less oxygenated compared to those externally mixed with BC.
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.
Jianhui Jiang, Imad El Haddad, Sebnem Aksoyoglu, Giulia Stefenelli, Amelie Bertrand, Nicolas Marchand, Francesco Canonaco, Jean-Eudes Petit, Olivier Favez, Stefania Gilardoni, Urs Baltensperger, and André S. H. Prévôt
Geosci. Model Dev., 14, 1681–1697, https://doi.org/10.5194/gmd-14-1681-2021, https://doi.org/10.5194/gmd-14-1681-2021, 2021
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We developed a box model with a volatility basis set to simulate organic aerosol (OA) from biomass burning and optimized the vapor-wall-loss-corrected OA yields with a genetic algorithm. The optimized parameterizations were then implemented in the air quality model CAMx v6.5. Comparisons with ambient measurements indicate that the vapor-wall-loss-corrected parameterization effectively improves the model performance in predicting OA, which reduced the mean fractional bias from −72.9 % to −1.6 %.
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
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.
Sebnem Aksoyoglu, Jianhui Jiang, Giancarlo Ciarelli, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 15665–15680, https://doi.org/10.5194/acp-20-15665-2020, https://doi.org/10.5194/acp-20-15665-2020, 2020
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We investigated the role of ammonia in European air quality between 1990 and 2030 under varying land and ship emissions. If ship emissions will be regulated more strictly in the future, particulate nitrate will decrease in coastal areas in northern Europe, while sulfate aerosol will decrease in the Mediterranean region. We predict a shift in the sensitivity of aerosol formation from NH3 towards NOx emissions between 1990 and 2030 in most of Europe except the eastern part of the model domain.
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.
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.
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.
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.
Anna K. Tobler, Alicja Skiba, Dongyu S. Wang, Philip Croteau, Katarzyna Styszko, Jarosław Nęcki, Urs Baltensperger, Jay G. Slowik, and André S. H. Prévôt
Atmos. Meas. Tech., 13, 5293–5301, https://doi.org/10.5194/amt-13-5293-2020, https://doi.org/10.5194/amt-13-5293-2020, 2020
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Some quadrupole aerosol chemical speciation monitors (Q-ACSMs) have had issues with the quantification of particulate chloride, resulting in apparent negative chloride concentrations. We can show that this is due to the different behavior of Cl+ and HCl+, and we present a correction for the more accurate quantification of chloride. The correction can be applied to measurements in environments where the particulate chloride is dominated by NH4Cl.
Archit Mehra, Jordan E. Krechmer, Andrew Lambe, Chinmoy Sarkar, Leah Williams, Farzaneh Khalaj, Alex Guenther, John Jayne, Hugh Coe, Douglas Worsnop, Celia Faiola, and Manjula Canagaratna
Atmos. Chem. Phys., 20, 10953–10965, https://doi.org/10.5194/acp-20-10953-2020, https://doi.org/10.5194/acp-20-10953-2020, 2020
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Emissions of volatile organic compounds (VOCs) from plants are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Real plant emissions are much more diverse than the few proxies widely used for studies of plant SOA. Here we present the first study of SOA from Californian sage plants and the oxygenated monoterpenes representing their major emissions. We identify SOA products and show the importance of the formation of highly oxygenated organic molecules and oligomers.
Chunshui Lin, Darius Ceburnis, Wei Xu, Eimear Heffernan, Stig Hellebust, John Gallagher, Ru-Jin Huang, Colin O'Dowd, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 20, 10513–10529, https://doi.org/10.5194/acp-20-10513-2020, https://doi.org/10.5194/acp-20-10513-2020, 2020
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Chemical composition and sources of submicron aerosols (PM1) were simultaneously investigated at a kerbside site in the Dublin city center and at a residential site in suburban Dublin (~5 km apart) during both a nonheating and a heating period in 2018. This study highlights the temporal and spatial variability of sources within the Dublin city center and the need for additional aerosol characterization studies to improve targeted mitigation solutions for a greater impact on urban air quality.
Archit Mehra, Yuwei Wang, Jordan E. Krechmer, Andrew Lambe, Francesca Majluf, Melissa A. Morris, Michael Priestley, Thomas J. Bannan, Daniel J. Bryant, Kelly L. Pereira, Jacqueline F. Hamilton, Andrew R. Rickard, Mike J. Newland, Harald Stark, Philip Croteau, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, Lin Wang, and Hugh Coe
Atmos. Chem. Phys., 20, 9783–9803, https://doi.org/10.5194/acp-20-9783-2020, https://doi.org/10.5194/acp-20-9783-2020, 2020
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Aromatic volatile organic compounds (VOCs) emitted from anthropogenic activity are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Here we present a detailed chemical characterisation of SOA from four C9-aromatic isomers and a polycyclic aromatic hydrocarbon (PAH). We identify and compare their oxidation products in the gas and particle phases, showing the different relative importance of oxidation pathways and proportions of highly oxygenated organic molecules.
Liwei Wang, Jay G. Slowik, Nidhi Tripathi, Deepika Bhattu, Pragati Rai, Varun Kumar, Pawan Vats, Rangu Satish, Urs Baltensperger, Dilip Ganguly, Neeraj Rastogi, Lokesh K. Sahu, Sachchida N. Tripathi, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 9753–9770, https://doi.org/10.5194/acp-20-9753-2020, https://doi.org/10.5194/acp-20-9753-2020, 2020
Martin Rigler, Luka Drinovec, Gašper Lavrič, Athanasia Vlachou, André S. H. Prévôt, Jean Luc Jaffrezo, Iasonas Stavroulas, Jean Sciare, Judita Burger, Irena Kranjc, Janja Turšič, Anthony D. A. Hansen, and Griša Močnik
Atmos. Meas. Tech., 13, 4333–4351, https://doi.org/10.5194/amt-13-4333-2020, https://doi.org/10.5194/amt-13-4333-2020, 2020
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Carbonaceous aerosols are a large fraction of fine particulate matter. They are extremely diverse, and they directly impact air quality, visibility, cloud formation and public health. In this paper we present a new instrument and new method to measure carbon content in particulate matter in real time and at a high time resolution. The new method was validated in a 1-month winter field campaign in Ljubljana, Slovenia.
Yuwei Wang, Archit Mehra, Jordan E. Krechmer, Gan Yang, Xiaoyu Hu, Yiqun Lu, Andrew Lambe, Manjula Canagaratna, Jianmin Chen, Douglas Worsnop, Hugh Coe, and Lin Wang
Atmos. Chem. Phys., 20, 9563–9579, https://doi.org/10.5194/acp-20-9563-2020, https://doi.org/10.5194/acp-20-9563-2020, 2020
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A series of OH-initiated oxidation experiments of trimethylbenzene were investigated in the absence and presence of NOx. Many C9 products with 1–11 oxygen atoms and C18 products presumably formed from dimerization of C9 peroxy radicals were observed, hinting at the extensive existence of autoxidation and accretion reaction pathways. The presence of NOx would suppress the formation of highly oxygenated C18 molecules and enhance the formation of organonitrates and even dinitrate compounds.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
Ru-Jin Huang, Yao He, Jing Duan, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Weiwei Hu, Chunshui Lin, Haiyan Ni, Wenting Dai, Junji Cao, Yunfei Wu, Renjian Zhang, Wei Xu, Jurgita Ovadnevaite, Darius Ceburnis, Thorsten Hoffmann, and Colin D. O'Dowd
Atmos. Chem. Phys., 20, 9101–9114, https://doi.org/10.5194/acp-20-9101-2020, https://doi.org/10.5194/acp-20-9101-2020, 2020
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We systematically compared the submicron particle (PM1) processes in haze days with low and high relative humidity (RH) in wintertime Beijing. Nitrate had similar daytime growth rates in low-RH and high-RH pollution. OOA had a higher growth rate in low-RH pollution than in high-RH pollution. Sulfate had a decreasing trend in low-RH pollution, while it increased significantly in high-RH pollution. This distinction may be explained by the different processes affected by meteorological conditions.
Eirini Boleti, Christoph Hueglin, Stuart K. Grange, André S. H. Prévôt, and Satoshi Takahama
Atmos. Chem. Phys., 20, 9051–9066, https://doi.org/10.5194/acp-20-9051-2020, https://doi.org/10.5194/acp-20-9051-2020, 2020
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Long-term temporal evolution of ozone concentrations between 2000 and 2015 in Europe was estimated using a signal decomposition technique. The seasonal cycles are correlated with local climate conditions and vary according to geographic region, while ozone levels are indicative of distance to emission sources. The site's environment plays a key role in ozone trends, with the most polluted environments showing the least reduction in ozone, while in less polluted areas ozone has decreased.
Tuukka Petäjä, Ella-Maria Duplissy, Ksenia Tabakova, Julia Schmale, Barbara Altstädter, Gerard Ancellet, Mikhail Arshinov, Yurii Balin, Urs Baltensperger, Jens Bange, Alison Beamish, Boris Belan, Antoine Berchet, Rossana Bossi, Warren R. L. Cairns, Ralf Ebinghaus, Imad El Haddad, Beatriz Ferreira-Araujo, Anna Franck, Lin Huang, Antti Hyvärinen, Angelika Humbert, Athina-Cerise Kalogridis, Pavel Konstantinov, Astrid Lampert, Matthew MacLeod, Olivier Magand, Alexander Mahura, Louis Marelle, Vladimir Masloboev, Dmitri Moisseev, Vaios Moschos, Niklas Neckel, Tatsuo Onishi, Stefan Osterwalder, Aino Ovaska, Pauli Paasonen, Mikhail Panchenko, Fidel Pankratov, Jakob B. Pernov, Andreas Platis, Olga Popovicheva, Jean-Christophe Raut, Aurélie Riandet, Torsten Sachs, Rosamaria Salvatori, Roberto Salzano, Ludwig Schröder, Martin Schön, Vladimir Shevchenko, Henrik Skov, Jeroen E. Sonke, Andrea Spolaor, Vasileios K. Stathopoulos, Mikko Strahlendorff, Jennie L. Thomas, Vito Vitale, Sterios Vratolis, Carlo Barbante, Sabine Chabrillat, Aurélien Dommergue, Konstantinos Eleftheriadis, Jyri Heilimo, Kathy S. Law, Andreas Massling, Steffen M. Noe, Jean-Daniel Paris, André S. H. Prévôt, Ilona Riipinen, Birgit Wehner, Zhiyong Xie, and Hanna K. Lappalainen
Atmos. Chem. Phys., 20, 8551–8592, https://doi.org/10.5194/acp-20-8551-2020, https://doi.org/10.5194/acp-20-8551-2020, 2020
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The role of polar regions is increasing in terms of megatrends such as globalization, new transport routes, demography, and the use of natural resources with consequent effects on regional and transported pollutant concentrations. Here we summarize initial results from our integrative project exploring the Arctic environment and pollution to deliver data products, metrics, and indicators for stakeholders.
Yunle Chen, Masayuki Takeuchi, Theodora Nah, Lu Xu, Manjula R. Canagaratna, Harald Stark, Karsten Baumann, Francesco Canonaco, André S. H. Prévôt, L. Gregory Huey, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 20, 8421–8440, https://doi.org/10.5194/acp-20-8421-2020, https://doi.org/10.5194/acp-20-8421-2020, 2020
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Two online mass spectrometry instruments, an aerosol mass spectrometer and a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols, were deployed at Yorkville, GA, for a comprehensive characterization of organic aerosol. We observed notable secondary organic aerosol formation from isoprene and monoterpenes via different pathways during both day and night, and a series of highly oxidized acid-like compounds was found to be closely related to aged SOA.
Lu Qi, Alexander L. Vogel, Sepideh Esmaeilirad, Liming Cao, Jing Zheng, Jean-Luc Jaffrezo, Paola Fermo, Anne Kasper-Giebl, Kaspar R. Daellenbach, Mindong Chen, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 20, 7875–7893, https://doi.org/10.5194/acp-20-7875-2020, https://doi.org/10.5194/acp-20-7875-2020, 2020
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We present the first application of this online and offline strategy using the new extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF), which achieves increased chemical specificity relative to other online techniques. Measurement and source apportionment of 1 year of filter samples collected in Zurich, Switzerland, show seasonal contributions from fresh and aged wood combustion in winter and biogenic emission-derived SOA in summer, as well as other sources.
Angela Buchholz, Arttu Ylisirniö, Wei Huang, Claudia Mohr, Manjula Canagaratna, Douglas R. Worsnop, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 20, 7693–7716, https://doi.org/10.5194/acp-20-7693-2020, https://doi.org/10.5194/acp-20-7693-2020, 2020
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To understand the role of aerosol particles in the atmosphere, it is necessary to know their detailed chemical composition and physical properties, especially volatility. The thermal desorption data from FIGAERO–CIMS provides both but are difficult to analyse. With positive matrix factorisation, we can separate instrument background from the real signal. Compounds can be classified by their apparent volatility, and the contribution of thermal decomposition in the instrument can be identified.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Weiqi Xu, Yao He, Yanmei Qiu, Chun Chen, Conghui Xie, Lu Lei, Zhijie Li, Jiaxing Sun, Junyao Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Meas. Tech., 13, 3205–3219, https://doi.org/10.5194/amt-13-3205-2020, https://doi.org/10.5194/amt-13-3205-2020, 2020
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We characterized mass spectral features of organic aerosol (OA) and water-soluble OA (WSOA) from 21 cooking, crop straw, wood, and coal burning experiments using aerosol mass spectrometers with standard and capture vaporizers, and we demonstrated the applications of source spectral profiles in improving source apportionment of ambient OA at a highly polluted rural site in the North China Plain in winter.
Yanjun Zhang, Otso Peräkylä, Chao Yan, Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Qiaozhi Zha, Matthieu Riva, Olga Garmash, Heikki Junninen, Pentti Paatero, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 20, 5945–5961, https://doi.org/10.5194/acp-20-5945-2020, https://doi.org/10.5194/acp-20-5945-2020, 2020
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By utilizing a new analysis approach, we investigated atmospheric oxidation of biogenic volatile emissions in a Finnish forest, measured by chemical ionization mass spectrometry. We identified several new compound groups, including low-volatility accretion products and their formation pathways. Results from this study are important for understanding atmospheric aerosol formation, as well as providing new perspectives on future lab studies and data analysis of short-lived species.
Yan Zheng, Xi Cheng, Keren Liao, Yaowei Li, Yong Jie Li, Ru-Jin Huang, Weiwei Hu, Ying Liu, Tong Zhu, Shiyi Chen, Limin Zeng, Douglas R. Worsnop, and Qi Chen
Atmos. Meas. Tech., 13, 2457–2472, https://doi.org/10.5194/amt-13-2457-2020, https://doi.org/10.5194/amt-13-2457-2020, 2020
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This paper provides important information to help researchers to understand the mass quantification and source apportionment by Aerodyne aerosol mass spectrometers.
Arttu Ylisirniö, Angela Buchholz, Claudia Mohr, Zijun Li, Luis Barreira, Andrew Lambe, Celia Faiola, Eetu Kari, Taina Yli-Juuti, Sergey A. Nizkorodov, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Chem. Phys., 20, 5629–5644, https://doi.org/10.5194/acp-20-5629-2020, https://doi.org/10.5194/acp-20-5629-2020, 2020
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We studied the chemical composition and volatility of secondary organic aerosol (SOA) particles formed from emissions of Scots pines and compared those results to SOA formed from α-pinene and from a sesquiterpene mixture. We found that SOA formed from single precursors cannot capture the properties of SOA formed from real plant emissions.
Yonggang Xue, Yu Huang, Steven Sai Hang Ho, Long Chen, Liqin Wang, Shuncheng Lee, and Junji Cao
Atmos. Chem. Phys., 20, 5425–5436, https://doi.org/10.5194/acp-20-5425-2020, https://doi.org/10.5194/acp-20-5425-2020, 2020
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Particulate active metallic oxides in dust were proposed to influence the photochemical reactions of ambient volatile organic compounds (VOCs). A case study investigated the origin and transformation of VOCs during a windblown dust-to-haze pollution episode. In the dust event, a sharp decrease in VOC loading and aging of their components was observed. An increase in Ti and Fe and a fast decrease in trans-/cis-2-butene ratios demonstrated that dust can accelerate the oxidation of ambient VOCs.
Wei Yuan, Ru-Jin Huang, Lu Yang, Jie Guo, Ziyi Chen, Jing Duan, Ting Wang, Haiyan Ni, Yongming Han, Yongjie Li, Qi Chen, Yang Chen, Thorsten Hoffmann, and Colin O'Dowd
Atmos. Chem. Phys., 20, 5129–5144, https://doi.org/10.5194/acp-20-5129-2020, https://doi.org/10.5194/acp-20-5129-2020, 2020
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We characterized light-absorbing properties, chromophore composition and sources of brown carbon (BrC) in Xi'an; identified three groups of light-absorbing organics; and quantified their contribution to overall BrC absorption. Our results showed that vehicle emissions and secondary formation are major sources of BrC in spring, coal combustion and vehicle emissions are major sources in fall, biomass burning and coal combustion become major sources in winter, and secondary BrC dominates in summer.
Jianjun Li, Qi Zhang, Gehui Wang, Jin Li, Can Wu, Lang Liu, Jiayuan Wang, Wenqing Jiang, Lijuan Li, Kin Fai Ho, and Junji Cao
Atmos. Chem. Phys., 20, 4889–4904, https://doi.org/10.5194/acp-20-4889-2020, https://doi.org/10.5194/acp-20-4889-2020, 2020
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We examined light absorption properties and molecular composition of water-soluble (WS) and water-insoluble (WI) BrC in PM2.5 collected from northwest China. We found that photochemical formation contributes significantly to light absorption of WI-BrC in summer, whereas aqueous-phase reactions play an important role in secondary WS-BrC formation in winter. BrC was estimated to account for 1.36 % and 3.74 %, respectively, of total down-welling solar radiation in the UV range in summer and winter.
Stefano Decesari, Marco Paglione, Matteo Rinaldi, Manuel Dall'Osto, Rafel Simó, Nicola Zanca, Francesca Volpi, Maria Cristina Facchini, Thorsten Hoffmann, Sven Götz, Christopher Johannes Kampf, Colin O'Dowd, Darius Ceburnis, Jurgita Ovadnevaite, and Emilio Tagliavini
Atmos. Chem. Phys., 20, 4193–4207, https://doi.org/10.5194/acp-20-4193-2020, https://doi.org/10.5194/acp-20-4193-2020, 2020
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Atmospheric aerosols in Antarctica contribute to regulate the delicate budget of cloud formation and precipitations. Besides the well-known biogenic production of sulfur-containing aerosol components such as methanesulfonate (MSA), the assessment of biological sources of organic particles in Antarctica remains an active area of research. Here we present the results of aerosol organic characterization during a research cruise performed in the Weddell Sea and in the Southern Ocean in Jan–Feb 2015.
Jing Duan, Ru-Jin Huang, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Chunshui Lin, Haiyan Ni, Meng Wang, Jurgita Ovadnevaite, Darius Ceburnis, Chunying Chen, Douglas R. Worsnop, Thorsten Hoffmann, Colin O'Dowd, and Junji Cao
Atmos. Chem. Phys., 20, 3793–3807, https://doi.org/10.5194/acp-20-3793-2020, https://doi.org/10.5194/acp-20-3793-2020, 2020
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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.
Wei Xu, Jurgita Ovadnevaite, Kirsten N. Fossum, Chunshui Lin, Ru-Jin Huang, Colin O'Dowd, and Darius Ceburnis
Atmos. Chem. Phys., 20, 3777–3791, https://doi.org/10.5194/acp-20-3777-2020, https://doi.org/10.5194/acp-20-3777-2020, 2020
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A humidified tandem differential mobility analyser (HTDMA) and a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) were simultaneously deployed during winter at Mace Head observatory to characterise the hygroscopicity of marine aerosols and their link to chemical composition. Good agreement was generally found between measured and estimated growth factors. A significant degree of external mixing was found in all air masses manifesting primary and secondary sources.
Liine Heikkinen, Mikko Äijälä, Matthieu Riva, Krista Luoma, Kaspar Dällenbach, Juho Aalto, Pasi Aalto, Diego Aliaga, Minna Aurela, Helmi Keskinen, Ulla Makkonen, Pekka Rantala, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 20, 3151–3180, https://doi.org/10.5194/acp-20-3151-2020, https://doi.org/10.5194/acp-20-3151-2020, 2020
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Atmospheric aerosols are solid or liquid particles suspended in the air. They are known as a health risk, but they also influence the Earth's climate. The composition of aerosols becomes important when predicting their effect on climate. We show both seasonal and year-to-year variability of aerosol chemical composition in the boreal forest of Finland. We observed a consistent bimodal seasonal trend: a biogenic summertime maximum and an anthropogenic wintertime maximum in the mass concentration.
Lu Lei, Conghui Xie, Dawei Wang, Yao He, Qingqing Wang, Wei Zhou, Wei Hu, Pingqing Fu, Yong Chen, Xiaole Pan, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 20, 2877–2890, https://doi.org/10.5194/acp-20-2877-2020, https://doi.org/10.5194/acp-20-2877-2020, 2020
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We characterized aerosol composition and sources near two steel plants in a coastal region in fall and spring seasons. Our results showed substantially different aerosol composition and sources between the two seasons. We observed significant impacts of steel plant emissions on aerosol chemistry nearby, and we found that aerosol particles emitted from the steel plants were dominated by ammonium sulfate/bisulfate; NOx/CO and NOx/SO2 were distinct from those in the absence of industrial plumes.
Haiyan Li, Matthieu Riva, Pekka Rantala, Liine Heikkinen, Kaspar Daellenbach, Jordan E. Krechmer, Pierre-Marie Flaud, Douglas Worsnop, Markku Kulmala, Eric Villenave, Emilie Perraudin, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 20, 1941–1959, https://doi.org/10.5194/acp-20-1941-2020, https://doi.org/10.5194/acp-20-1941-2020, 2020
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We deployed the recently developed Vocus PTR-TOF in the French Landes forest during summertime to gain insights into terpene chemistry. In addition to isoprene, monoterpenes, sesquiterpenes, and the low-volatility diterpenes, various terpene reaction products are characterized. Through the analysis of terpene chemistry, we demonstrate the capability of the Vocus PTR-TOF for the detection of oxidized reaction products, highlighting its importance in investigating atmospheric oxidation processes.
Pragati Rai, Markus Furger, Jay G. Slowik, Francesco Canonaco, Roman Fröhlich, Christoph Hüglin, María Cruz Minguillón, Krag Petterson, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 1657–1674, https://doi.org/10.5194/acp-20-1657-2020, https://doi.org/10.5194/acp-20-1657-2020, 2020
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A source apportionment study of hourly resolved elements in PM10 measured at a traffic-influenced site in Härkingen, Switzerland, using positive matrix factorization (PMF) and multilinear engine-2 (ME-2) offered resolution of robust and unambiguous factor profiles and contributions. We show that the rotational control available in ME-2 provides a means for treating extreme events such as fireworks within a PMF analysis.
Marco Paglione, Stefania Gilardoni, Matteo Rinaldi, Stefano Decesari, Nicola Zanca, Silvia Sandrini, Lara Giulianelli, Dimitri Bacco, Silvia Ferrari, Vanes Poluzzi, Fabiana Scotto, Arianna Trentini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Francesco Canonaco, André S. H. Prévôt, Paola Massoli, Claudio Carbone, Maria Cristina Facchini, and Sandro Fuzzi
Atmos. Chem. Phys., 20, 1233–1254, https://doi.org/10.5194/acp-20-1233-2020, https://doi.org/10.5194/acp-20-1233-2020, 2020
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Our multi-year observational study regarding organic aerosol (OA) in the Po Valley indicates that more than half of OA is of secondary origin (SOA) through all the year and at both urban and rural sites. Within the SOA, the measurements show the importance of biomass burning (BB) aging products during cold seasons and indicate aqueous-phase processing of BB emissions as a fundamental driver of SOA formation in wintertime, with important consequences for air quality policy at the global level.
Abigail R. Koss, Manjula R. Canagaratna, Alexander Zaytsev, Jordan E. Krechmer, Martin Breitenlechner, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joseph R. Roscioli, Frank N. Keutsch, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 1021–1041, https://doi.org/10.5194/acp-20-1021-2020, https://doi.org/10.5194/acp-20-1021-2020, 2020
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Oxidation chemistry of organic compounds in the atmosphere produces a diverse spectrum of products. This diversity is difficult to represent in air quality and climate models, and in laboratory experiments it results in large and complex datasets. This work evaluates several methods to simplify the chemistry of oxidation systems in environmental chambers, including positive matrix factorization, hierarchical clustering analysis, and gamma kinetics parameterization.
Haiyan Ni, Ru-Jin Huang, Junji Cao, Jie Guo, Haoyue Deng, and Ulrike Dusek
Atmos. Chem. Phys., 19, 15609–15628, https://doi.org/10.5194/acp-19-15609-2019, https://doi.org/10.5194/acp-19-15609-2019, 2019
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We present a 1-year source apportionment record of carbonaceous aerosols in Xi'an, China. Biomass burning strongly increases in winter, while seasonal changes of coal and liquid fossil fuel combustion are moderate. We find strong evidence for fossil secondary OC formation during the warm period that is further enhanced in stagnant, polluted conditions due to longer atmospheric residence times. At the same time we find that water-insoluble (primary) fossil is lost due to photochemical processing.
Jianhui Jiang, Sebnem Aksoyoglu, Imad El-Haddad, Giancarlo Ciarelli, Hugo A. C. Denier van der Gon, Francesco Canonaco, Stefania Gilardoni, Marco Paglione, María Cruz Minguillón, Olivier Favez, Yunjiang Zhang, Nicolas Marchand, Liqing Hao, Annele Virtanen, Kalliopi Florou, Colin O'Dowd, Jurgita Ovadnevaite, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 15247–15270, https://doi.org/10.5194/acp-19-15247-2019, https://doi.org/10.5194/acp-19-15247-2019, 2019
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We use an air quality model with a modified organic aerosol (OA) module based on chamber experiments to identify the OA sources and their contributions in Europe. Comparisons with long-term measurements at nine sites in 2011 show an improvement in OA simulation. Our results suggest that the biomass burning and biogenic emissions are the dominant sources in winter and summer, respectively. Contributions of diesel and gasoline vehicles are relatively small compared to a previous study in the US.
Alexander Zaytsev, Abigail R. Koss, Martin Breitenlechner, Jordan E. Krechmer, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joshua L. Cox, Joshua Moss, Joseph R. Roscioli, Manjula R. Canagaratna, Douglas R. Worsnop, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Chem. Phys., 19, 15117–15129, https://doi.org/10.5194/acp-19-15117-2019, https://doi.org/10.5194/acp-19-15117-2019, 2019
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Aromatic hydrocarbons contribute significantly to the production of tropospheric ozone and secondary organic aerosol (SOA). Here later-generation low-volatility oxygenated products from toluene and 1,2,4-TMB oxidation by OH are detected in the gas and particle phases. We show that these products, previously identified as highly oxygenated molecules (HOMs), are formed in more than one pathway with differing numbers of reaction steps with OH. They also make up a significant fraction of SOA.
Giulia Stefenelli, Veronika Pospisilova, Felipe D. Lopez-Hilfiker, Kaspar R. Daellenbach, Christoph Hüglin, Yandong Tong, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 19, 14825–14848, https://doi.org/10.5194/acp-19-14825-2019, https://doi.org/10.5194/acp-19-14825-2019, 2019
Yunjiang Zhang, Olivier Favez, Jean-Eudes Petit, Francesco Canonaco, Francois Truong, Nicolas Bonnaire, Vincent Crenn, Tanguy Amodeo, Andre S. H. Prévôt, Jean Sciare, Valerie Gros, and Alexandre Albinet
Atmos. Chem. Phys., 19, 14755–14776, https://doi.org/10.5194/acp-19-14755-2019, https://doi.org/10.5194/acp-19-14755-2019, 2019
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We present 6-year source apportionment of organic aerosol (OA) achieved with near-continuous online measurements and subsequent receptor model analysis in the Paris region, France. The OA factors presented distinct seasonal patterns, associated with different atmospheric formation processes and roles in air pollution. Limited year-round trends for two primary anthropogenic factors and a biogenic-like secondary factor were observed, while a more oxidized secondary OA showed a decreasing feature.
Jun Zhou, Miriam Elser, Ru-Jin Huang, Manuel Krapf, Roman Fröhlich, Deepika Bhattu, Giulia Stefenelli, Peter Zotter, Emily A. Bruns, Simone M. Pieber, Haiyan Ni, Qiyuan Wang, Yichen Wang, Yaqing Zhou, Chunying Chen, Mao Xiao, Jay G. Slowik, Samuel Brown, Laure-Estelle Cassagnes, Kaspar R. Daellenbach, Thomas Nussbaumer, Marianne Geiser, André S. H. Prévôt, Imad El-Haddad, Junji Cao, Urs Baltensperger, and Josef Dommen
Atmos. Chem. Phys., 19, 14703–14720, https://doi.org/10.5194/acp-19-14703-2019, https://doi.org/10.5194/acp-19-14703-2019, 2019
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Reactive oxygen species (ROS) are believed to contribute to the adverse health effects of aerosols. We measured particle-bound ROS (PB-ROS) with an online instrument in two distinct environments, i.e., Beijing (China) and Bern (Switzerland). In both cities these exogenic ROS are predominantly related to secondary organic aerosol (SOA). PB-ROS content in SOA from various anthropogenic emission sources tested in the laboratory was comparable to that in the ambient measurements.
Chunshui Lin, Darius Ceburnis, Ru-Jin Huang, Wei Xu, Teresa Spohn, Damien Martin, Paul Buckley, John Wenger, Stig Hellebust, Matteo Rinaldi, Maria Cristina Facchini, Colin O'Dowd, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 19, 14091–14106, https://doi.org/10.5194/acp-19-14091-2019, https://doi.org/10.5194/acp-19-14091-2019, 2019
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To gain insight into the spatial and chemical variation in submicron aerosol, a nationwide characterization of wintertime PM1 was performed at four representative sites across Ireland. This nationwide source apportionment study highlights the large contribution of residential solid fuel burning to urban air pollution and has significant implications for aerosol regional-transport models.
Xiaoli Shen, Heike Vogel, Bernhard Vogel, Wei Huang, Claudia Mohr, Ramakrishna Ramisetty, Thomas Leisner, André S. H. Prévôt, and Harald Saathoff
Atmos. Chem. Phys., 19, 13189–13208, https://doi.org/10.5194/acp-19-13189-2019, https://doi.org/10.5194/acp-19-13189-2019, 2019
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This study provides good insight into the chemical nature and complex origin of aerosols by combining comprehensive field observations and transport modelling. We suggest that factors related to topography, metrological conditions, local emissions, in situ formation and growth, regional transport, and the interaction of biogenic and anthropogenic compounds need to be considered for a comprehensive understanding of aerosol processes.
Xuan Zhang, Haofei Zhang, Wen Xu, Xiaokang Wu, Geoffrey S. Tyndall, John J. Orlando, John T. Jayne, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Meas. Tech., 12, 5535–5545, https://doi.org/10.5194/amt-12-5535-2019, https://doi.org/10.5194/amt-12-5535-2019, 2019
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We develop a new technique to characterize organic nitrates as intact molecules in atmospheric aerosols, and we apply this technique to identify hydroxy nitrates in secondary organic aerosols produced from the photochemical oxidation of isoprene.
Mingjin Tang, Chak K. Chan, Yong Jie Li, Hang Su, Qingxin Ma, Zhijun Wu, Guohua Zhang, Zhe Wang, Maofa Ge, Min Hu, Hong He, and Xinming Wang
Atmos. Chem. Phys., 19, 12631–12686, https://doi.org/10.5194/acp-19-12631-2019, https://doi.org/10.5194/acp-19-12631-2019, 2019
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Hygroscopicity is one of the most important properties of aerosol particles, and a number of experimental techniques, which differ largely in principles, configurations and cost, have been developed to investigate hygroscopic properties of atmospherically relevant particles. Our paper provides a comprehensive and critical review of available techniques for aerosol hygroscopicity studies.
Eleni Dovrou, Christopher Y. Lim, Manjula R. Canagaratna, Jesse H. Kroll, Douglas R. Worsnop, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 5303–5315, https://doi.org/10.5194/amt-12-5303-2019, https://doi.org/10.5194/amt-12-5303-2019, 2019
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Measurement techniques commonly used to analyze particulate matter composition can result in the possible misidentification of sulfur-containing species, especially for the case of sulfate and hydroxymethanesulfonate (HMS). The efficiency and limitations of these techniques, along with a method that enables further studies of the contribution of sulfur-containing species, S(IV) versus S(VI), to particulate matter under low-light atmospheric conditions, are described in this work.
Leonid Nichman, Martin Wolf, Paul Davidovits, Timothy B. Onasch, Yue Zhang, Doug R. Worsnop, Janarjan Bhandari, Claudio Mazzoleni, and Daniel J. Cziczo
Atmos. Chem. Phys., 19, 12175–12194, https://doi.org/10.5194/acp-19-12175-2019, https://doi.org/10.5194/acp-19-12175-2019, 2019
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Previous studies showed widespread ice nucleation activity of soot. In this systematic study we investigated the factors that affect the heterogeneous ice nucleation activity of soot surrogates in the cirrus cloud regime. Our observations are consistent with an ice nucleation mechanism of pore condensation followed by freezing. The results show significant variations in ice nucleation activity as a function of size, morphology, and surface chemistry of the black-carbon-containing particles.
Xiaoxiao Li, Shaojie Song, Wei Zhou, Jiming Hao, Douglas R. Worsnop, and Jingkun Jiang
Atmos. Chem. Phys., 19, 12163–12174, https://doi.org/10.5194/acp-19-12163-2019, https://doi.org/10.5194/acp-19-12163-2019, 2019
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Aerosol liquid water is ubiquitous in ambient aerosol. Using long-term aerosol chemical composition to model the aerosol water in Beijing, we found that water absorbed by organics contributes a significant fraction to the total aerosol water. We emphasize the hygroscopicity of organics is highly variable and should be taken into consideration in modelling. A positive feedback loop between organic hygroscopicity and aerosol water was found as one of the driving factors of severe haze in Beijing.
Carly L. Reddington, Luke Conibear, Christoph Knote, Ben J. Silver, Yong J. Li, Chak K. Chan, Steve R. Arnold, and Dominick V. Spracklen
Atmos. Chem. Phys., 19, 11887–11910, https://doi.org/10.5194/acp-19-11887-2019, https://doi.org/10.5194/acp-19-11887-2019, 2019
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We use a high-resolution model over South and East Asia to explore air quality and human health benefits of eliminating emissions from six man-made pollution sources. We find that preventing emissions from either residential energy use, industry, or open biomass burning yields the largest reductions in ground-level particulate matter pollution and its associated disease burden over this region. We also summarize previous estimates of the source-specific disease burden in China and India.
Zhujie Li, Haobo Tan, Jun Zheng, Li Liu, Yiming Qin, Nan Wang, Fei Li, Yongjie Li, Mingfu Cai, Yan Ma, and Chak K. Chan
Atmos. Chem. Phys., 19, 11669–11685, https://doi.org/10.5194/acp-19-11669-2019, https://doi.org/10.5194/acp-19-11669-2019, 2019
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Comprehensive field measurements were conducted to investigate aerosol compositions, optical properties, source origins, and radiative forcing effects in Guangzhou. Particulate brown carbon (BrC) light absorption was differentiated from that of black carbon. BrC was mostly due to primary emissions, such as straw burning, rather than secondary formation. BrC may cause ∼2.3 W m−2 radiative forcing at the top of the atmosphere and contribute to ∼15.8 % of the aerosol warming effect.
Giulia Stefenelli, Jianhui Jiang, Amelie Bertrand, Emily A. Bruns, Simone M. Pieber, Urs Baltensperger, Nicolas Marchand, Sebnem Aksoyoglu, André S. H. Prévôt, Jay G. Slowik, and Imad El Haddad
Atmos. Chem. Phys., 19, 11461–11484, https://doi.org/10.5194/acp-19-11461-2019, https://doi.org/10.5194/acp-19-11461-2019, 2019
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Box model simulations, based on the volatility basis set approach, of smog chamber wood combustion experiments conducted at different temperatures (−10 °C, 2 °C, 15 °C), emission loads, combustion conditions (flaming and smoldering) and residential stoves fabricated in the last 2 decades. Novel parameterization methods based on a genetic algorithm approach allowed estimation of precursor class contributions to SOA and evaluation of the effect of emission variability on SOA yield predictions.
Felipe D. Lopez-Hilfiker, Veronika Pospisilova, Wei Huang, Markus Kalberer, Claudia Mohr, Giulia Stefenelli, Joel A. Thornton, Urs Baltensperger, Andre S. H. Prevot, and Jay G. Slowik
Atmos. Meas. Tech., 12, 4867–4886, https://doi.org/10.5194/amt-12-4867-2019, https://doi.org/10.5194/amt-12-4867-2019, 2019
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We present a novel, field-deployable extractive electrospray time-of-flight mass spectrometer (EESI-TOF), which provides real-time, near-molecular measurements of organic aerosol at atmospherically relevant concentrations, addressing a critical gap in existing measurement capabilities. Successful deployments of the EESI-TOF for laboratory measurements, ground-based ambient sampling, and aboard a research aircraft highlight the versatility and potential of the EESI-TOF system.
Meng Wang, Ru-Jin Huang, Junji Cao, Wenting Dai, Jiamao Zhou, Chunshui Lin, Haiyan Ni, Jing Duan, Ting Wang, Yang Chen, Yongjie Li, Qi Chen, Imad El Haddad, and Thorsten Hoffmann
Atmos. Meas. Tech., 12, 4779–4789, https://doi.org/10.5194/amt-12-4779-2019, https://doi.org/10.5194/amt-12-4779-2019, 2019
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The analytical performances of SE-GC-MS and TD-GC-MS for the determination of n-alkanes, PAHs and hopanes were evaluated and compared. The two methods show a good agreement with a high correlation efficient (R2 > 0.98) and a slope close to unity. The concentrations of n-alkanes, PAHs and hopanes are found to be much higher in Beijing than those in Chengdu, Shanghai and Guangzhou, most likely due to emissions from coal combustion for wintertime heating in Beijing.
Haiyan Ni, Ru-Jin Huang, Junji Cao, Wenting Dai, Jiamao Zhou, Haoyue Deng, Anita Aerts-Bijma, Harro A. J. Meijer, and Ulrike Dusek
Atmos. Chem. Phys., 19, 10405–10422, https://doi.org/10.5194/acp-19-10405-2019, https://doi.org/10.5194/acp-19-10405-2019, 2019
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We apply radiocarbon source apportionment of more volatile organic carbon (mvOC) to winter aerosol samples from six Chinese cities. We find a consistently larger contribution of fossil sources to mvOC than to secondary or total organic carbon. Fossil mvOC concentrations are strongly correlated with primary fossil OC but not with secondary fossil OC. The variability in nonfossil mvOC seems to be related to both primary and secondary biomass burning sources.
Jing Duan, Ru-Jin Huang, Chunshui Lin, Wenting Dai, Meng Wang, Yifang Gu, Ying Wang, Haobin Zhong, Yan Zheng, Haiyan Ni, Uli Dusek, Yang Chen, Yongjie Li, Qi Chen, Douglas R. Worsnop, Colin D. O'Dowd, and Junji Cao
Atmos. Chem. Phys., 19, 10319–10334, https://doi.org/10.5194/acp-19-10319-2019, https://doi.org/10.5194/acp-19-10319-2019, 2019
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We present the seasonal distinction of secondary aerosol formation in urban Beijing. Both photochemical oxidation and aqueous-phase processing played important roles in SOA (secondary organic aerosol) formation during all three seasons; while for sulfate formation, gas-phase photochemical oxidation was the major pathway in late summer, aqueous-phase reactions were more responsible during early winter, and both processes had contributions during autumn.
Weiqi Xu, Conghui Xie, Eleni Karnezi, Qi Zhang, Junfeng Wang, Spyros N. Pandis, Xinlei Ge, Jingwei Zhang, Junling An, Qingqing Wang, Jian Zhao, Wei Du, Yanmei Qiu, Wei Zhou, Yao He, Ying Li, Jie Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 19, 10205–10216, https://doi.org/10.5194/acp-19-10205-2019, https://doi.org/10.5194/acp-19-10205-2019, 2019
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We present the first aerosol volatility measurements in Beijing in summer using a thermodenuder coupled with aerosol mass spectrometers. Our results showed that organic aerosol (OA) comprised mainly semi-volatile organic compounds in summer, and the freshly oxidized secondary OA was the most volatile component. We also found quite different volatility distributions in black-carbon-containing primary and secondary OA, ambient OA, ambient secondary OA and the WRF-Chem model.
Yunfei Wu, Yunjie Xia, Rujin Huang, Zhaoze Deng, Ping Tian, Xiangao Xia, and Renjian Zhang
Atmos. Meas. Tech., 12, 4347–4359, https://doi.org/10.5194/amt-12-4347-2019, https://doi.org/10.5194/amt-12-4347-2019, 2019
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The morphology and effective density of externally mixed black carbon (extBC) aerosols were studied using a tandem technique coupling a DMA with a SP2. The study extended the mass–mobility relationship to large extBC with a mobility diameter larger than 350 nm, a size range seldom included in previous tandem measurements of BC aggregates. On this basis, quantities such as the mass–mobility scaling exponent were revealed for extBC in urban Beijing.
Sanna Saarikoski, Leah R. Williams, Steven R. Spielman, Gregory S. Lewis, Arantzazu Eiguren-Fernandez, Minna Aurela, Susanne V. Hering, Kimmo Teinilä, Philip Croteau, John T. Jayne, Thorsten Hohaus, Douglas R. Worsnop, and Hilkka Timonen
Atmos. Meas. Tech., 12, 3907–3920, https://doi.org/10.5194/amt-12-3907-2019, https://doi.org/10.5194/amt-12-3907-2019, 2019
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An air-to-air ultrafine particle concentrator (Aerosol Dynamics Inc. concentrator; ADIc) has been tailored for the low (~ 0.08 L min−1) inlet flow of aerosol mass spectrometers, and it provides a factor of 8–21 enrichment in the concentration of particles. The ADIc was evaluated in laboratory and field measurements. The results showed that the concentration factor depends primarily on the ratio between the sample flow and the output flow and is independent of particle size above about 10 nm.
Yanjun Zhang, Otso Peräkylä, Chao Yan, Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Qiaozhi Zha, Matthieu Riva, Olga Garmash, Heikki Junninen, Pentti Paatero, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 12, 3761–3776, https://doi.org/10.5194/amt-12-3761-2019, https://doi.org/10.5194/amt-12-3761-2019, 2019
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Recent advancements in atmospheric mass spectrometry provide large amounts of new information but at the same time present considerable challenges for the data analysis, for example, in high-resolution peak identification and separation. To address these problems, this study presents a simple and novel method, which succeeds in analyzing both synthetic and ambient datasets. We believe it will become a powerful approach in the data analysis of mass spectra.
Jiarui Wu, Naifang Bei, Bo Hu, Suixin Liu, Meng Zhou, Qiyuan Wang, Xia Li, Lang Liu, Tian Feng, Zirui Liu, Yichen Wang, Junji Cao, Xuexi Tie, Jun Wang, Luisa T. Molina, and Guohui Li
Atmos. Chem. Phys., 19, 8703–8719, https://doi.org/10.5194/acp-19-8703-2019, https://doi.org/10.5194/acp-19-8703-2019, 2019
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In the present study, simulations during a persistent and heavy haze pollution episode from 5 December 2015 to 4 January 2016 in the North China Plain (NCP) were performed using the WRF-Chem model to comprehensively quantify contributions of the aerosol shortwave radiative feedback (ARF) to near-surface PM2.5 mass concentrations. During the episode, the ARF deteriorates the haze pollution, increasing the near-surface PM2.5 concentration in the NCP by 10.2 μg m−3 (7.8 %) on average.
Jiarui Wu, Naifang Bei, Bo Hu, Suixin Liu, Meng Zhou, Qiyuan Wang, Xia Li, Lang Liu, Tian Feng, Zirui Liu, Yichen Wang, Junji Cao, Xuexi Tie, Jun Wang, Luisa T. Molina, and Guohui Li
Atmos. Chem. Phys., 19, 8721–8739, https://doi.org/10.5194/acp-19-8721-2019, https://doi.org/10.5194/acp-19-8721-2019, 2019
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The near-surface PM2.5 contribution of the ALW total effect is 17.5 % in NCP, indicating that ALW plays an important role in the PM2.5 formation during the wintertime haze pollution. Moreover, the ALW-HET overwhelmingly dominates the PM2.5 enhancement due to the ALW. The ALW does not consistently enhance near-surface [PM2.5] with increasing RH. When the RH exceeds 80 %, the contribution of the ALW begins to decrease, which is caused by the high occurrence frequencies of precipitation.
Jun Tao, Zhisheng Zhang, Yunfei Wu, Leiming Zhang, Zhijun Wu, Peng Cheng, Mei Li, Laiguo Chen, Renjian Zhang, and Junji Cao
Atmos. Chem. Phys., 19, 8471–8490, https://doi.org/10.5194/acp-19-8471-2019, https://doi.org/10.5194/acp-19-8471-2019, 2019
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Mass-scattering efficiencies (MSE) of dominant chemical species in atmospheric aerosols are important parameters for building the relationships between chemical species and the particle-scattering coefficient. Particle MSE mainly depends on the mass fractions of (NH4)2SO4, NH4NO3, and organic matter and their MSEs in the droplet mode. MSEs of (NH4)2SO4, NH4NO3 and organic matter were determined by their size distributions in the droplet mode.
Lu Qi, Mindong Chen, Giulia Stefenelli, Veronika Pospisilova, Yandong Tong, Amelie Bertrand, Christoph Hueglin, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 19, 8037–8062, https://doi.org/10.5194/acp-19-8037-2019, https://doi.org/10.5194/acp-19-8037-2019, 2019
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Current understanding of OA sources is limited by the chemical resolution of existing real-time measurement technology. We describe the first wintertime deployment of a novel extractive electrospray ionization time-of-flight mass spectrometer, which provides near-molecular OA measurements with high time resolution. We show that biomass combustion strongly influences winter OA. Via factor analysis, aging-dependent signatures and time contributions of biomass-combustion-derived OA are resolved.
Kun Li, Junling Li, Shengrui Tong, Weigang Wang, Ru-Jin Huang, and Maofa Ge
Atmos. Chem. Phys., 19, 8021–8036, https://doi.org/10.5194/acp-19-8021-2019, https://doi.org/10.5194/acp-19-8021-2019, 2019
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Wintertime volatile organic compounds (VOCs) in suburban and urban Beijing were measured. Urban VOC concentrations were much higher than suburban ones, but the emission features were similar. The photochemical processes were more active in the urban site, resulting in the high daytime formation of oxygenated VOCs. In addition, human activities during holidays can largely influence the VOC levels. These results are helpful in better understanding the atmospheric chemistry of VOCs in Beijing.
Tian Feng, Shuyu Zhao, Naifang Bei, Jiarui Wu, Suixin Liu, Xia Li, Lang Liu, Yang Qian, Qingchuan Yang, Yichen Wang, Weijian Zhou, Junji Cao, and Guohui Li
Atmos. Chem. Phys., 19, 7429–7443, https://doi.org/10.5194/acp-19-7429-2019, https://doi.org/10.5194/acp-19-7429-2019, 2019
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The observed ratio of organic carbon to element carbon has increased remarkably in Beijing. Here, based on the measurements and model simulation, we show that the enhanced atmospheric oxidizing capacity is an important contributor to that increase by facilitating the aging process of organic aerosols (add oxygen). Our results indicate a ubiquitous enhancement of secondary organic aerosol formation over Beijing–Tianjin–Hebei, China, in the context of increasing oxidizing capacity.
Athanasia Vlachou, Anna Tobler, Houssni Lamkaddam, Francesco Canonaco, Kaspar R. Daellenbach, Jean-Luc Jaffrezo, María Cruz Minguillón, Marek Maasikmets, Erik Teinemaa, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 7279–7295, https://doi.org/10.5194/acp-19-7279-2019, https://doi.org/10.5194/acp-19-7279-2019, 2019
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The resolution of rotational ambiguity in positive matrix factorization (PMF) models is a major challenge. Here, we developed a method based on bootstrapping and correlations to extract environmentally meaningful solutions from PMF analysis based on offline aerosol mass spectrometry data. The method has been tested on a dataset that covers 1 full year of filter samples collected at three different sites in Estonia.
Hongmei Xu, Jean-François Léon, Cathy Liousse, Benjamin Guinot, Véronique Yoboué, Aristide Barthélémy Akpo, Jacques Adon, Kin Fai Ho, Steven Sai Hang Ho, Lijuan Li, Eric Gardrat, Zhenxing Shen, and Junji Cao
Atmos. Chem. Phys., 19, 6637–6657, https://doi.org/10.5194/acp-19-6637-2019, https://doi.org/10.5194/acp-19-6637-2019, 2019
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This paper discusses the personal exposure characteristics and health implication of PM2.5 and bounded chemical species based on three anthropogenic sources and related populations (domestic fires for women, waste burning for students and motorcycle traffic for drivers) in Abidjan and Cotonou in dry and wet seasons of 2016. This work can be regarded as the first attempt at measuring personal exposure to PM2.5 and its related health risks in underdeveloped countries of Africa.
Kaspar R. Daellenbach, Ivan Kourtchev, Alexander L. Vogel, Emily A. Bruns, Jianhui Jiang, Tuukka Petäjä, Jean-Luc Jaffrezo, Sebnem Aksoyoglu, Markus Kalberer, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 5973–5991, https://doi.org/10.5194/acp-19-5973-2019, https://doi.org/10.5194/acp-19-5973-2019, 2019
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Here we present the molecular composition of the organic aerosol (OA) at an urban site in Central Europe (Zurich, Switzerland) and compare it to smog chamber wood smoke and ambient biogenic secondary OA (SOA) (Orbitrap analyses). Accordingly, we are able to explain the strong seasonality of the molecular composition by aged wood smoke and biogenic SOA during winter and summer. Our results could also explain the predominance of non-fossil organic carbon at European locations throughout the year.
Matthieu Riva, Pekka Rantala, Jordan E. Krechmer, Otso Peräkylä, Yanjun Zhang, Liine Heikkinen, Olga Garmash, Chao Yan, Markku Kulmala, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 12, 2403–2421, https://doi.org/10.5194/amt-12-2403-2019, https://doi.org/10.5194/amt-12-2403-2019, 2019
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The impact of aerosol particles on climate and air quality remains poorly understood due to multiple factors. One of the current limitations is the incomplete understanding of the contribution of oxygenated species, formed from the oxidation of volatile organic compounds (VOCs) to aerosol formation. Taking advantage of recent mass spectrometric developments, we have evaluated and compared the capability of multiple state-of-the-art mass spectrometers to detect a wide variety of oxygenated VOCs.
Karl Espen Yttri, David Simpson, Robert Bergström, Gyula Kiss, Sönke Szidat, Darius Ceburnis, Sabine Eckhardt, Christoph Hueglin, Jacob Klenø Nøjgaard, Cinzia Perrino, Ignazio Pisso, Andre Stephan Henry Prevot, Jean-Philippe Putaud, Gerald Spindler, Milan Vana, Yan-Lin Zhang, and Wenche Aas
Atmos. Chem. Phys., 19, 4211–4233, https://doi.org/10.5194/acp-19-4211-2019, https://doi.org/10.5194/acp-19-4211-2019, 2019
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Carbonaceous aerosols from natural sources were abundant regardless of season. Residential wood burning (RWB) emissions were occasionally equally as large as or larger than of fossil-fuel sources, depending on season and region. RWB emissions are poorly constrained; thus emissions inventories need improvement. Harmonizing emission factors between countries is likely the most important step to improve model calculations for biomass burning emissions and European PM2.5 concentrations in general.
Long Chen, Yu Huang, Yonggang Xue, Zhenxing Shen, Junji Cao, and Wenliang Wang
Atmos. Chem. Phys., 19, 4075–4091, https://doi.org/10.5194/acp-19-4075-2019, https://doi.org/10.5194/acp-19-4075-2019, 2019
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The present calculations show that the sequential addition of CIs to HHPs affords oligomers containing CIs as chain units. The addition of an –OOH group in HHPs to the central carbon atom of CIs is identified as the most energetically favorable channel, with a barrier height strongly dependent on both CI substituent number (one or two) and position (syn- or anti-). In particular, the introduction of a methyl group into the anti-position significantly increases the rate coefficient.
Angela Buchholz, Andrew T. Lambe, Arttu Ylisirniö, Zijun Li, Olli-Pekka Tikkanen, Celia Faiola, Eetu Kari, Liqing Hao, Olli Luoma, Wei Huang, Claudia Mohr, Douglas R. Worsnop, Sergey A. Nizkorodov, Taina Yli-Juuti, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 4061–4073, https://doi.org/10.5194/acp-19-4061-2019, https://doi.org/10.5194/acp-19-4061-2019, 2019
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We studied the evaporation of α-pinene secondary organic aerosol particles in clean air to derive their volatility from the observed size changes. We found that the particles became more resilient to evaporation with increased oxidative age, possibly increasing their lifetime in the atmosphere. Also, increased relative humidity increased the particle evaporation. Mass spectrometry measurements of the particles at different stages of evaporation revealed some water-induced composition changes.
Jianhui Jiang, Sebnem Aksoyoglu, Giancarlo Ciarelli, Emmanouil Oikonomakis, Imad El-Haddad, Francesco Canonaco, Colin O'Dowd, Jurgita Ovadnevaite, María Cruz Minguillón, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 3747–3768, https://doi.org/10.5194/acp-19-3747-2019, https://doi.org/10.5194/acp-19-3747-2019, 2019
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Biogenic volatile organic compound (BVOC) emissions from vegetation are essential inputs for air quality models but their uncertainties are very high. In this study we show the importance of BVOC emissions for modelled ozone and aerosol concentrations in Europe. Using different biogenic emissions from MEGAN and PSI models significantly affected organic aerosols (smaller effect on ozone), indicating the importance of harmonising the BVOC emissions in the model inter-comparison studies.
Mikko Äijälä, Kaspar R. Daellenbach, Francesco Canonaco, Liine Heikkinen, Heikki Junninen, Tuukka Petäjä, Markku Kulmala, André S. H. Prévôt, and Mikael Ehn
Atmos. Chem. Phys., 19, 3645–3672, https://doi.org/10.5194/acp-19-3645-2019, https://doi.org/10.5194/acp-19-3645-2019, 2019
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Aerosol mass spectrometry produces large amounts of complex data, the analysis of which necessitates chemometrics – the application of advanced statistical and mathematical tools to chemical data. Here, we perform a data-driven analysis of multiple aerosol mass spectrometric data sets, to show that the traditional separation of organics and inorganics is not necessary. The resulting 7-component aerosol speciation explains 83 % to 96 % of observed variability at our boreal forest experiment site.
Rachel E. O'Brien, Kelsey J. Ridley, Manjula R. Canagaratna, John T. Jayne, Philip L. Croteau, Douglas R. Worsnop, Sri Hapsari Budisulistiorini, Jason D. Surratt, Christopher L. Follett, Daniel J. Repeta, and Jesse H. Kroll
Atmos. Meas. Tech., 12, 1659–1671, https://doi.org/10.5194/amt-12-1659-2019, https://doi.org/10.5194/amt-12-1659-2019, 2019
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Analysis of the elemental composition of organic mixtures can provide insights into the sources and aging of environmental samples. Here we describe a method that allows characterization of this type of material using micrograms of material by a combination of a small-volume ultrasonic nebulizer and an aerosol mass spectrometer. This technique enables rapid analysis of complex organic mixtures using approximately an order of magnitude less sample than standard analyses.
Yang Chen, Mi Tian, Ru-Jin Huang, Guangming Shi, Huanbo Wang, Chao Peng, Junji Cao, Qiyuan Wang, Shumin Zhang, Dongmei Guo, Leiming Zhang, and Fumo Yang
Atmos. Chem. Phys., 19, 3245–3255, https://doi.org/10.5194/acp-19-3245-2019, https://doi.org/10.5194/acp-19-3245-2019, 2019
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Amine-containing particles were characterized in an urban area of Chongqing during both summer and winter using a single-particle aerosol mass spectrometer (SPAMS). Amines were observed to internally mix with elemental carbon (EC), organic carbon (OC), sulfate, and nitrate. Diethylamine (DEA) was the most abundant in both number and peak area among amine-containing particles. Vegetation and traffic were the primary sources of particulate amines.
Thomas J. Bannan, Michael Le Breton, Michael Priestley, Stephen D. Worrall, Asan Bacak, Nicholas A. Marsden, Archit Mehra, Julia Hammes, Mattias Hallquist, M. Rami Alfarra, Ulrich K. Krieger, Jonathan P. Reid, John Jayne, Wade Robinson, Gordon McFiggans, Hugh Coe, Carl J. Percival, and Dave Topping
Atmos. Meas. Tech., 12, 1429–1439, https://doi.org/10.5194/amt-12-1429-2019, https://doi.org/10.5194/amt-12-1429-2019, 2019
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The Filter Inlet for Gases and AEROsols (FIGAERO) is an inlet designed to be coupled with a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) and provides simultaneous molecular information relating to both the gas- and particle-phase samples. This method has been used to extract vapour pressures of compounds whilst giving quantitative concentrations in the particle phase. Here we detail an ideal set of benchmark compounds for characterization of the FIGAERO.
Li Xing, Jiarui Wu, Miriam Elser, Shengrui Tong, Suixin Liu, Xia Li, Lang Liu, Junji Cao, Jiamao Zhou, Imad El-Haddad, Rujin Huang, Maofa Ge, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 19, 2343–2359, https://doi.org/10.5194/acp-19-2343-2019, https://doi.org/10.5194/acp-19-2343-2019, 2019
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We used the WRF-CHEM model to simulate wintertime secondary organic aerosol (SOA) concentrations over Beijing–Tianjin–Hebei (BTH), China. Heterogeneous HONO sources increased the near-surface SOA by 46.3 % in BTH. Direct emissions of glyoxal and methylglyoxal from residential sources contributed 25.5 % to the total SOA mass. Our study highlights the importance of heterogeneous HONO sources and primary residential emissions of glyoxal and methylglyoxal to SOA formation in winter over BTH.
Mingjin Tang, Wenjun Gu, Qingxin Ma, Yong Jie Li, Cheng Zhong, Sheng Li, Xin Yin, Ru-Jin Huang, Hong He, and Xinming Wang
Atmos. Chem. Phys., 19, 2247–2258, https://doi.org/10.5194/acp-19-2247-2019, https://doi.org/10.5194/acp-19-2247-2019, 2019
Liya Guo, Wenjun Gu, Chao Peng, Weigang Wang, Yong Jie Li, Taomou Zong, Yujing Tang, Zhijun Wu, Qinhao Lin, Maofa Ge, Guohua Zhang, Min Hu, Xinhui Bi, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 19, 2115–2133, https://doi.org/10.5194/acp-19-2115-2019, https://doi.org/10.5194/acp-19-2115-2019, 2019
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In this work, hygroscopic properties of eight Ca- and Mg-containing salts were systematically investigated using two complementary techniques. The results largely improve our knowledge of the physicochemical properties of mineral dust and sea salt aerosols.
Qiyuan Wang, Suixin Liu, Nan Li, Wenting Dai, Yunfei Wu, Jie Tian, Yaqing Zhou, Meng Wang, Steven Sai Hang Ho, Yang Chen, Renjian Zhang, Shuyu Zhao, Chongshu Zhu, Yongming Han, Xuexi Tie, and Junji Cao
Atmos. Chem. Phys., 19, 1881–1899, https://doi.org/10.5194/acp-19-1881-2019, https://doi.org/10.5194/acp-19-1881-2019, 2019
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Andrew T. Lambe, Jordan E. Krechmer, Zhe Peng, Jason R. Casar, Anthony J. Carrasquillo, Jonathan D. Raff, Jose L. Jimenez, and Douglas R. Worsnop
Atmos. Meas. Tech., 12, 299–311, https://doi.org/10.5194/amt-12-299-2019, https://doi.org/10.5194/amt-12-299-2019, 2019
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This paper is an evaluation of methods used to generate OH radicals under conditions with high concentrations of NO and NO2 to simulate oxidation chemistry in polluted urban atmospheres over equivalent atmospheric timescales of ~ 1 day.
Nivedita K. Kumar, Joel C. Corbin, Emily A. Bruns, Dario Massabó, Jay G. Slowik, Luka Drinovec, Griša Močnik, Paolo Prati, Athanasia Vlachou, Urs Baltensperger, Martin Gysel, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 17843–17861, https://doi.org/10.5194/acp-18-17843-2018, https://doi.org/10.5194/acp-18-17843-2018, 2018
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It is clear that considerable uncertainties still exist in understanding the magnitude of aerosol absorption on a global scale and its contribution to global warming. This manuscript provides a comprehensive assessment of the optical absorption by organic aerosols (brown carbon) from residential wood combustion as a function of atmospheric aging.
Liqing Hao, Olga Garmash, Mikael Ehn, Pasi Miettinen, Paola Massoli, Santtu Mikkonen, Tuija Jokinen, Pontus Roldin, Pasi Aalto, Taina Yli-Juuti, Jorma Joutsensaari, Tuukka Petäjä, Markku Kulmala, Kari E. J. Lehtinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 18, 17705–17716, https://doi.org/10.5194/acp-18-17705-2018, https://doi.org/10.5194/acp-18-17705-2018, 2018
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An aerosol mass spectrometer was used to characterize aerosol chemical composition during new particle formation periods. The time profiles of mass concentrations and chemical composition of observed aerosol particles are subjected to joint effects of boundary layer dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During the nighttime, the increase in organic aerosol mass correlated well with the increase in condensed highly oxygenated organic molecules' mass.
Qiaozhi Zha, Chao Yan, Heikki Junninen, Matthieu Riva, Nina Sarnela, Juho Aalto, Lauriane Quéléver, Simon Schallhart, Lubna Dada, Liine Heikkinen, Otso Peräkylä, Jun Zou, Clémence Rose, Yonghong Wang, Ivan Mammarella, Gabriel Katul, Timo Vesala, Douglas R. Worsnop, Markku Kulmala, Tuukka Petäjä, Federico Bianchi, and Mikael Ehn
Atmos. Chem. Phys., 18, 17437–17450, https://doi.org/10.5194/acp-18-17437-2018, https://doi.org/10.5194/acp-18-17437-2018, 2018
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Vertical measurements of highly oxygenated molecules (HOMs) below and above the forest canopy were performed for the first time in a boreal forest during September 2016. Our results highlight that near-ground HOM measurements may only be representative of a small fraction of the entire nocturnal boundary layer, which may sequentially influence the growth of newly formed particles and SOA formation close to ground surface, where the majority of measurements are conducted.