Articles | Volume 16, issue 18
Atmos. Chem. Phys., 16, 11563–11580, 2016
https://doi.org/10.5194/acp-16-11563-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Special issue: Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5)...
Atmos. Chem. Phys., 16, 11563–11580, 2016
https://doi.org/10.5194/acp-16-11563-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article 19 Sep 2016
Research article | 19 Sep 2016
Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA)
Weiwei Hu et al.
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A tunnel test was initiated to measure the vehicular IVOCs emissions under real-world driving conditions. Higher SOA formations estimated from vehicular IVOCs than that from traditional VOCs emphasized the greater importance of IVOCs in modulating urban SOA. The results also revealed that non-road diesel-fueled engines greatly contributed to IVOCs in China.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Ye Kuang, Shan Huang, Biao Xue, Biao Luo, Qicong Song, Wei Chen, Weiwei Hu, Wei Li, Pusheng Zhao, Mingfu Cai, Yuwen Peng, Jipeng Qi, Tiange Li, Duohong Chen, Dingli Yue, Bin Yuan, and Min Shao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-3, https://doi.org/10.5194/acp-2021-3, 2021
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We found that organic aerosol factors with identified sources perform much better than oxidation level parameters in characterizing variations in organic aerosol hygroscopicity, and secondary aerosol formations associated with different sources have distinct effects on organic aerosol hygroscopicity. It reveals that source-oriented organic aerosol hygroscopicity investigations might come up to more appropriate parameterization approaches in chemical and climate models.
Caihong Wu, Chaomin Wang, Sihang Wang, Wenjie Wang, Bin Yuan, Jipeng Qi, Baolin Wang, Hongli Wang, Chen Wang, Wei Song, Xinming Wang, Weiwei Hu, Shengrong Lou, Chenshuo Ye, Yuwen Peng, Zelong Wang, Yibo Huangfu, Yan Xie, Manni Zhu, Junyu Zheng, Xuemei Wang, Bin Jiang, Zhanyi Zhang, and Min Shao
Atmos. Chem. Phys., 20, 14769–14785, https://doi.org/10.5194/acp-20-14769-2020, https://doi.org/10.5194/acp-20-14769-2020, 2020
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Based on measurements from an online mass spectrometer, we quantify volatile organic compound (VOC) concentrations from numerous ions of the mass spectrometer, using information from laboratory-obtained calibration results. We find that most VOC concentrations are from oxygenated VOCs (OVOCs). We further show that these OVOCs also contribute significantly to OH reactivity. Our results suggest the important role of OVOCs in VOC emissions and chemistry in urban air.
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. Discuss., https://doi.org/10.5194/acp-2020-1187, https://doi.org/10.5194/acp-2020-1187, 2020
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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.
Chaomin Wang, Bin Yuan, Caihong Wu, Sihang Wang, Jipeng Qi, Baolin Wang, Zelong Wang, Weiwei Hu, Wei Chen, Chenshuo Ye, Wenjie Wang, Yele Sun, Chen Wang, Shan Huang, Wei Song, Xinming Wang, Suxia Yang, Shenyang Zhang, Wanyun Xu, Nan Ma, Zhanyi Zhang, Bin Jiang, Hang Su, Yafang Cheng, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 20, 14123–14138, https://doi.org/10.5194/acp-20-14123-2020, https://doi.org/10.5194/acp-20-14123-2020, 2020
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We utilized a novel online mass spectrometry method to measure the total concentration of higher alkanes at each carbon number at two different sites in China, allowing us to take into account SOA contributions from all isomers for higher alkanes. We found that higher alkanes account for significant fractions of SOA formation at the two sites. The contributions are comparable to or even higher than single-ring aromatics, the most-recognized SOA precursors in urban air.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Hongyu Guo, Duseong S. Jo, Anne V. Handschy, Demetrios Pagonis, Jason C. Schroder, Melinda K. Schueneman, Michael J. Cubison, Jack E. Dibb, Alma Hodzic, Weiwei Hu, Brett B. Palm, and Jose L. Jimenez
Atmos. Meas. Tech., 13, 6193–6213, https://doi.org/10.5194/amt-13-6193-2020, https://doi.org/10.5194/amt-13-6193-2020, 2020
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Collecting particulate matter, or aerosols, onto filters to be analyzed offline is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
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
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. Discuss., https://doi.org/10.5194/acp-2020-914, https://doi.org/10.5194/acp-2020-914, 2020
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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 are predictable and explained by key emissions. These results are used to estimate the premature mortality associated to SOA in urban regions.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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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.
Junchen Guo, Shengzhen Zhou, Mingfu Cai, Jun Zhao, Wei Song, Weixiong Zhao, Weiwei Hu, Yele Sun, Yao He, Chengqiang Yang, Xuezhe Xu, Zhisheng Zhang, Peng Cheng, Qi Fan, Jian Hang, Shaojia Fan, Xinming Wang, and Xuemei Wang
Atmos. Chem. Phys., 20, 7595–7615, https://doi.org/10.5194/acp-20-7595-2020, https://doi.org/10.5194/acp-20-7595-2020, 2020
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We characterized non-refractory submicron particulate matter (PM1.0) during winter in Guangzhou, south China. Chemical composition and key sources of ambient PM1.0 are revealed, highlighting the significant role of SOA. The relationship with SOA and peroxy radicals indicated gas-phase oxidation contributed predominantly to SOA formation during non-pollution periods, while heterogeneous/multiphase reactions played more important roles in SOA formation during pollution periods.
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.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Eloise A. Marais, Zhe Peng, Benjamin A. Nault, Weiwei Hu, Pedro Campuzano-Jost, and Jose L. Jimenez
Geosci. Model Dev., 12, 2983–3000, https://doi.org/10.5194/gmd-12-2983-2019, https://doi.org/10.5194/gmd-12-2983-2019, 2019
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We developed a parameterization method for IEPOX-SOA based on the detailed chemical mechanism. Our parameterizations were tested using a box model and 3-D chemical transport model, which accurately captured the spatiotemporal distribution and response to changes in emissions compared to the explicit full chemistry, while being more computationally efficient. The method developed in this study can be applied to global climate models for long-term studies with a lower computational cost.
Shino Toma, Steve Bertman, Christopher Groff, Fulizi Xiong, Paul B. Shepson, Paul Romer, Kaitlin Duffey, Paul Wooldridge, Ronald Cohen, Karsten Baumann, Eric Edgerton, Abigail R. Koss, Joost de Gouw, Allen Goldstein, Weiwei Hu, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 1867–1880, https://doi.org/10.5194/acp-19-1867-2019, https://doi.org/10.5194/acp-19-1867-2019, 2019
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Acyl peroxy nitrates (APN) were measured near the ground in Alabama using GC in summer 2013 to study biosphere–atmosphere interactions. APN were lower than measured in the SE USA over the past 2 decades. Historical data showed APN in 2013 was limited by NOx and production was dominated by biogenic precursors more than in the past. Isoprene-derived MPAN correlated with isoprene hydroxynitrates as NOx-dependent products. MPAN varied with aerosol growth, but not with N-containing particles.
Juhi Nagori, Ruud H. H. Janssen, Juliane L. Fry, Maarten Krol, Jose L. Jimenez, Weiwei Hu, and Jordi Vilà-Guerau de Arellano
Atmos. Chem. Phys., 19, 701–729, https://doi.org/10.5194/acp-19-701-2019, https://doi.org/10.5194/acp-19-701-2019, 2019
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Secondary organic aerosol (SOA) is produced through a complex interaction of sunlight, volatile organic compounds emitted from trees, anthropogenic emissions, and atmospheric chemistry. We are able to successfully model the formation and diurnal evolution of SOA using a model that takes into consideration the surface and boundary layer dynamics (1–2 km from the surface) and photochemistry above the southeastern US with data collected during the SOAS campaign to constrain the model.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Joel Brito, Samara Carbone, Igor O. Ribeiro, Glauber G. Cirino, Yingjun Liu, Ryan Thalman, Arthur Sedlacek, Aaron Funk, Courtney Schumacher, John E. Shilling, Johannes Schneider, Paulo Artaxo, Allen H. Goldstein, Rodrigo A. F. Souza, Jian Wang, Karena A. McKinney, Henrique Barbosa, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 18, 12185–12206, https://doi.org/10.5194/acp-18-12185-2018, https://doi.org/10.5194/acp-18-12185-2018, 2018
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This study aimed at understanding and quantifying the changes in mass concentration and composition of submicron airborne particulate matter (PM) in Amazonia due to urban pollution. Downwind of Manaus, PM concentrations increased by up to 200 % under polluted compared with background conditions. The observed changes included contributions from both primary and secondary processes. The differences in organic PM composition suggested a shift in the pathways of secondary production with pollution.
Lindsay D. Yee, Gabriel Isaacman-VanWertz, Rebecca A. Wernis, Meng Meng, Ventura Rivera, Nathan M. Kreisberg, Susanne V. Hering, Mads S. Bering, Marianne Glasius, Mary Alice Upshur, Ariana Gray Bé, Regan J. Thomson, Franz M. Geiger, John H. Offenberg, Michael Lewandowski, Ivan Kourtchev, Markus Kalberer, Suzane de Sá, Scot T. Martin, M. Lizabeth Alexander, Brett B. Palm, Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Jose L. Jimenez, Yingjun Liu, Karena A. McKinney, Paulo Artaxo, Juarez Viegas, Antonio Manzi, Maria B. Oliveira, Rodrigo de Souza, Luiz A. T. Machado, Karla Longo, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 10433–10457, https://doi.org/10.5194/acp-18-10433-2018, https://doi.org/10.5194/acp-18-10433-2018, 2018
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Biogenic volatile organic compounds react in the atmosphere to form secondary organic aerosol, yet the chemical pathways remain unclear. We collected filter samples and deployed a semi-volatile thermal desorption aerosol gas chromatograph in the central Amazon. We measured 30 sesquiterpenes and 4 diterpenes and find them to be important for reactive ozone loss. We estimate that sesquiterpene oxidation contributes at least 0.4–5 % (median 1 %) of observed submicron organic aerosol mass.
Wei Hu, Min Hu, Wei-Wei Hu, Jing Zheng, Chen Chen, Yusheng Wu, and Song Guo
Atmos. Chem. Phys., 17, 9979–10000, https://doi.org/10.5194/acp-17-9979-2017, https://doi.org/10.5194/acp-17-9979-2017, 2017
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Seasonal changes in chemical compositions, sources, and evolution for submicron aerosols in the megacity Beijing were investigated based on high-resolution AMS measurements. Carbonaceous fraction (OA+BC) constituted over 50 % of PM1 in autumn due to primary emissions, while SNA contributed 60 % to PM1 in other seasons. Secondary components (OOA+SNA) contributed ~ 60–80 % to PM1, suggesting that secondary formation played an important role in PM pollution. OA was in a relatively high oxidation state.
Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Philip Croteau, Manjula R. Canagaratna, John T. Jayne, Douglas R. Worsnop, and Jose L. Jimenez
Atmos. Meas. Tech., 10, 2897–2921, https://doi.org/10.5194/amt-10-2897-2017, https://doi.org/10.5194/amt-10-2897-2017, 2017
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Aerosol mass spectrometers (AMS) from ARI are used widely to measure the non-refractory species in PM1. Recently, a new capture vapourizer (CV) has been designed to reduce the need for a bounce-related CE correction in the commonly used standard vapourizer (SV) installed in AMS. To test the CV, the fragments, CE and size distributions of four pure inorganic species in the CV-AMS are investigated in various laboratory experiments. Results from the co-located SV-AMS are also shown as a comparison.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Matthew K. Newburn, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Ryan Thalman, Joel Brito, Samara Carbone, Paulo Artaxo, Allen H. Goldstein, Antonio O. Manzi, Rodrigo A. F. Souza, Fan Mei, John E. Shilling, Stephen R. Springston, Jian Wang, Jason D. Surratt, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 17, 6611–6629, https://doi.org/10.5194/acp-17-6611-2017, https://doi.org/10.5194/acp-17-6611-2017, 2017
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Wei Hu, Min Hu, Wei-Wei Hu, Hongya Niu, Jing Zheng, Yusheng Wu, Wentai Chen, Chen Chen, Lingyu Li, Min Shao, Shaodong Xie, and Yuanhang Zhang
Atmos. Chem. Phys., 16, 13213–13230, https://doi.org/10.5194/acp-16-13213-2016, https://doi.org/10.5194/acp-16-13213-2016, 2016
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An Aerodyne high-resolution time-of-flight AMS was deployed at a suburban site in the Sichuan Basin, southwestern China, under high emission intensity, and unique geographical and adverse meteorological conditions. OA was the most abundant component (36 %) in PM1, characterized by a relatively high oxidation state. The contributions of BBOA and BC to PM1 were high in primary emission episodes, highlighting the critical influence of biomass burning.
Aki Pajunoja, Weiwei Hu, Yu J. Leong, Nathan F. Taylor, Pasi Miettinen, Brett B. Palm, Santtu Mikkonen, Don R. Collins, Jose L. Jimenez, and Annele Virtanen
Atmos. Chem. Phys., 16, 11163–11176, https://doi.org/10.5194/acp-16-11163-2016, https://doi.org/10.5194/acp-16-11163-2016, 2016
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The phase state of ambient particles was inferred from bounce measurements conducted at a rural site in central Alabama during the SOAS campaign. The organic-dominated ambient particles are mostly in the liquid phase at summertime conditions but they turn semisolid when dried in the measurement setup. Bounce humidograms reveal that the hygroscopicity and oxidation of the particles decreases the liquefying RH. The effect of oxidation is emphasized by oxidation flow reactor measurements.
Amber M. Ortega, Patrick L. Hayes, Zhe Peng, Brett B. Palm, Weiwei Hu, Douglas A. Day, Rui Li, Michael J. Cubison, William H. Brune, Martin Graus, Carsten Warneke, Jessica B. Gilman, William C. Kuster, Joost de Gouw, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 7411–7433, https://doi.org/10.5194/acp-16-7411-2016, https://doi.org/10.5194/acp-16-7411-2016, 2016
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An oxidation flow reactor (OFR) was deployed to study secondary organic aerosol (SOA) formation and aging of urban emissions at a wide range of OH exposures during the CalNex campaign in Pasadena, CA, in 2010. Results include linking SOA formation to short-lived reactive compounds, similar elemental composition of reactor-aged emissions to atmospheric aging, changes in OA mass due to condensation of oxidized gas-phase species and heterogeneous oxidation of particle-phase species.
Zhe Peng, Douglas A. Day, Amber M. Ortega, Brett B. Palm, Weiwei Hu, Harald Stark, Rui Li, Kostas Tsigaridis, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 4283–4305, https://doi.org/10.5194/acp-16-4283-2016, https://doi.org/10.5194/acp-16-4283-2016, 2016
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Oxidation flow reactors (OFRs) are promising tools of studying atmospheric oxidation processes. Elevated concentrations of both OH and non-OH oxidants in OFRs leave room for speculation that non-OH chemistry can play a major role. Through systematic modeling, we find conditions where non-OH VOC fate is significant and show that, in most field studies of SOA using OFRs, non-OH VOC fate in OFRs was insignificant. We also provide guidelines helping OFR users avoid significant non-OH VOC oxidation.
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
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. Discuss., https://doi.org/10.5194/amt-2021-22, https://doi.org/10.5194/amt-2021-22, 2021
Preprint under review for AMT
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The extractive electrospray ionization mass spectrometry (EESI-MS) has been deployed for high throughput online detection of analyte particles with minimal fragmentations for decades. Our studies elucidate the extraction mechanism between analyte particles of different properties and charged electrospray droplets at different sizes. The results show that the extraction is a complete coalesce but is limited by the coalesce efficiency at different sizes, affecting the quantification accuracy.
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 André S. H. Prévôt
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-197, https://doi.org/10.5194/acp-2021-197, 2021
Preprint under review for ACP
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Krakow 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 data elucidate key emission sources that influence the PM1 concentrations in Krakow.
Hui Wang, Qizhong Wu, Alex B. Guenther, Xiaochun Yang, Lanning Wang, Tang Xiao, Jie Li, Jinming Feng, Qi Xu, and Huaqiong Cheng
Atmos. Chem. Phys., 21, 4825–4848, https://doi.org/10.5194/acp-21-4825-2021, https://doi.org/10.5194/acp-21-4825-2021, 2021
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We assessed the influence of the greening trend on BVOC emission in China. The comparison among different scenarios showed that vegetation changes resulting from land cover management are the main driver of BVOC emission change in China. Climate variability contributed significantly to interannual variations but not much to the long-term trend during the study period.
Hua Fang, Xiaoqing Huang, Yanli Zhang, Chenglei Pei, Zuzhao Huang, Yujun Wang, Yanning Chen, Jianhong Yan, Jianqiang Zeng, Shaoxuan Xiao, Shilu Luo, Sheng Li, Jun Wang, Ming Zhu, Xuewei Fu, Zhenfeng Wu, Runqi Zhang, Wei Song, Guohua Zhang, Weiwei Hu, Mingjin Tang, Xiang Ding, Xinhui Bi, and Xinming Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-189, https://doi.org/10.5194/acp-2021-189, 2021
Preprint under review for ACP
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A tunnel test was initiated to measure the vehicular IVOCs emissions under real-world driving conditions. Higher SOA formations estimated from vehicular IVOCs than that from traditional VOCs emphasized the greater importance of IVOCs in modulating urban SOA. The results also revealed that non-road diesel-fueled engines greatly contributed to IVOCs in China.
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 %.
Melinda K. Schueneman, Benjamin A. Nault, Pedro Campuzano-Jost, Duseong S. Jo, Douglas A. Day, Jason C. Schroder, Brett B. Palm, Alma Hodzic, Jack E. Dibb, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 2237–2260, https://doi.org/10.5194/amt-14-2237-2021, https://doi.org/10.5194/amt-14-2237-2021, 2021
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This work focuses on two important properties of the aerosol, acidity, and sulfate composition, which is important for our understanding of aerosol health and environmental impacts. We explore different methods to understand the composition of the aerosol with measurements from a specific instrument and apply those methods to a large dataset. These measurements are confounded by other factors, making it challenging to predict aerosol sulfate composition; pH estimations, however, show promise.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-167, https://doi.org/10.5194/acp-2021-167, 2021
Preprint under review for ACP
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected over the oceans from nearly Pole to Pole during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigate their impact on the variability of tropospheric N2O.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
Changmin Cho, Andreas Hofzumahaus, Hendrik Fuchs, Hans-Peter Dorn, Marvin Glowania, Frank Holland, Franz Rohrer, Vaishali Vardhan, Astrid Kiendler-Scharr, Andreas Wahner, and Anna Novelli
Atmos. Meas. Tech., 14, 1851–1877, https://doi.org/10.5194/amt-14-1851-2021, https://doi.org/10.5194/amt-14-1851-2021, 2021
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This study describes the implementation and characterization of the chemical modulation reactor (CMR) used in the laser-induced fluorescence instrument of the Forschungszentrum Jülich. The CMR allows for interference-free OH radical measurement in ambient air. During a field campaign in a rural environment, the observed interference was mostly below the detection limit of the instrument and fully explained by the known ozone interference.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-173, https://doi.org/10.5194/acp-2021-173, 2021
Preprint under review for ACP
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere, and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
Richard H. Moore, Elizabeth B. Wiggins, Adam T. Ahern, Stephen Zimmerman, Lauren Montgomery, Pedro Campuzano Jost, Claire E. Robinson, Luke D. Ziemba, Edward L. Winstead, Bruce E. Anderson, Charles A. Brock, Matthew D. Brown, Gao Chen, Ewan C. Crosbie, Hongyu Guo, Jose L. Jimenez, Carolyn E. Jordan, Ming Lyu, Benjamin A. Nault, Nicholas E. Rothfuss, Kevin J. Sanchez, Melinda Schueneman, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Nicholas L. Wagner, and Jian Wang
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-21, https://doi.org/10.5194/amt-2021-21, 2021
Preprint under review for AMT
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Atmospheric particles are everywhere and exist in a range of sizes from a few nanometers to hundreds of microns. Because particle size determines the behavior of chemical and physical processes, accurately measuring particle sizes is an important and integral part of atmospheric field measurements! Here, we discuss the performance of two, commonly-used particle sizers and how changes in particle composition and optical properties may result in sizing uncertainties, which we quantify.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-118, https://doi.org/10.5194/acp-2021-118, 2021
Preprint under review for ACP
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We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the low-NO photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
Ye Kuang, Shan Huang, Biao Xue, Biao Luo, Qicong Song, Wei Chen, Weiwei Hu, Wei Li, Pusheng Zhao, Mingfu Cai, Yuwen Peng, Jipeng Qi, Tiange Li, Duohong Chen, Dingli Yue, Bin Yuan, and Min Shao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-3, https://doi.org/10.5194/acp-2021-3, 2021
Preprint under review for ACP
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We found that organic aerosol factors with identified sources perform much better than oxidation level parameters in characterizing variations in organic aerosol hygroscopicity, and secondary aerosol formations associated with different sources have distinct effects on organic aerosol hygroscopicity. It reveals that source-oriented organic aerosol hygroscopicity investigations might come up to more appropriate parameterization approaches in chemical and climate models.
Marvin Glowania, Franz Rohrer, Hans-Peter Dorn, Andreas Hofzumahaus, Frank Holland, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-10, https://doi.org/10.5194/amt-2021-10, 2021
Preprint under review for AMT
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Three instruments using different techniques measuring gaseous formaldehyde concentrations were compared in experiments in the atmospheric simulation chamber SAPHIR at Forschungszentrum Jülich. Results demonstrate the need to correct the baseline in the measurements of instruments using the Hantzsch reaction or making use of cavity ring-down spectroscopy. After application of corrections all three methods give accurate and precice measurements within their specifications.
Beata Opacka, Jean-François Müller, Trissevgeni Stavrakou, Maite Bauwens, Katerina Sindelarova, Jana Markova, and Alex B. Guenther
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-95, https://doi.org/10.5194/acp-2021-95, 2021
Preprint under review for ACP
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Isoprene is primarily emitted from plants and about 80 % of its global emissions occur in the Tropics. Current isoprene inventories are usually based on modelled vegetation maps. But high pressure on land use over the last decades lead to severe losses, especially in tropical forests, that are not considered by models. We provide a study on the present-day impact of spaceborne land cover changes on isoprene emissions and the first inventory based on high-resolution Landsat tree cover dataset.
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.
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.
Juliana Gil-Loaiza, Joseph R. Roscioli, Joanne H. Shorter, Till H. M. Volkmann, Wei-Ren Ng, Jordan E. Krechmer, and Laura K. Meredith
Biogeosciences Discuss., https://doi.org/10.5194/bg-2020-401, https://doi.org/10.5194/bg-2020-401, 2020
Revised manuscript under review for BG
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We evaluated a new diffusive soil probe integrated with high-resolution gas analyzers to measure soil gases in real-time at a centimeter-scale. Using columns with simple silica and soil, we captured changes in carbon dioxide (CO2), volatile organic compounds (VOCs), and nitrous oxide (N2O) with its isotopes to distinguish potential nutrient sources and microbial metabolism. This approach will advance the use of soil gases as important signals to understand and monitor soil fertility and health.
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. Discuss., https://doi.org/10.5194/acp-2020-1293, https://doi.org/10.5194/acp-2020-1293, 2020
Preprint under review for ACP
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This study provides a holistic approach to study the spectrally-resolved light absorption by atmospheric brown carbon (BrC) and black carbon, using long time series of biomass burning-influenced 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.
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. Discuss., https://doi.org/10.5194/acp-2020-1263, https://doi.org/10.5194/acp-2020-1263, 2020
Preprint under review for ACP
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We used a recently developed state-of-the-art rolling mechanism for the first time at a rural site, southern alpine valley (Magadino) to get a more realistic and detailed information of the organic aerosol sources. This work highlights the strength of this novel source apportionment technique by comparing with the results derived from conventional seasonal PMF. Overall, this detailed interpretation of chemical speciation monitor (ACSM) data could be a role model for similar analysis.
Huan Song, Xiaorui Chen, Keding Lu, Qi Zou, Zhaofeng Tan, Hendrik Fuchs, Alfred Wiedensohler, Daniel R. Moon, Dwayne E. Heard, María-Teresa Baeza-Romero, Mei Zheng, Andreas Wahner, Astrid Kiendler-Scharr, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 15835–15850, https://doi.org/10.5194/acp-20-15835-2020, https://doi.org/10.5194/acp-20-15835-2020, 2020
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Accurate calculation of the HO2 uptake coefficient is one of the key parameters to quantify the co-reduction of both aerosol and ozone pollution. We modelled various lab measurements of γHO2 based on a gas-liquid phase kinetic model and developed a state-of-the-art parameterized equation. Based on a dataset from a comprehensive field campaign in the North China Plain, we proposed that the determination of the heterogeneous uptake process for HO2 should be included in future field campaigns.
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.
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. Discuss., https://doi.org/10.5194/acp-2020-1165, https://doi.org/10.5194/acp-2020-1165, 2020
Revised manuscript accepted for ACP
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Carbonaceous aerosol sources and trends were studied at the Birkenes Observatory, a site representative of the Northern European region. A large decrease in EC (−3.9 % to −4.2 % yr−1) (2001–2018) and a smaller decline in levoglucosan (−2.8 % yr−1) (2008–2018), suggest that OC / EC from traffic/industry is decreasing, while abatement of OC / EC from biomass burning is less successful. PMF apportioned 72 % of EC to fossil fuel sources and 53 % (PM2.5) and 78 % (PM10-2.5) of OC to biogenic sources.
Caihong Wu, Chaomin Wang, Sihang Wang, Wenjie Wang, Bin Yuan, Jipeng Qi, Baolin Wang, Hongli Wang, Chen Wang, Wei Song, Xinming Wang, Weiwei Hu, Shengrong Lou, Chenshuo Ye, Yuwen Peng, Zelong Wang, Yibo Huangfu, Yan Xie, Manni Zhu, Junyu Zheng, Xuemei Wang, Bin Jiang, Zhanyi Zhang, and Min Shao
Atmos. Chem. Phys., 20, 14769–14785, https://doi.org/10.5194/acp-20-14769-2020, https://doi.org/10.5194/acp-20-14769-2020, 2020
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Based on measurements from an online mass spectrometer, we quantify volatile organic compound (VOC) concentrations from numerous ions of the mass spectrometer, using information from laboratory-obtained calibration results. We find that most VOC concentrations are from oxygenated VOCs (OVOCs). We further show that these OVOCs also contribute significantly to OH reactivity. Our results suggest the important role of OVOCs in VOC emissions and chemistry in urban air.
Rongrong Wu, Luc Vereecken, Epameinondas Tsiligiannis, Sungah Kang, Sascha R. Albrecht, Luisa Hantschke, Defeng Zhao, Anna Novelli, Hendrik Fuchs, Ralf Tillmann, Thorsten Hohaus, Philip T. M. Carlsson, Justin Shenolikar, François Bernard, John N. Crowley, Juliane L. Fry, Bellamy Brownwood, Joel A. Thornton, Steven S. Brown, Astrid Kiendler-Scharr, Andreas Wahner, Matthias Hallquist, and Thomas F. Mentel
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1180, https://doi.org/10.5194/acp-2020-1180, 2020
Preprint under review for ACP
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Isoprene is the biogenic volatile organic compound with the largest emissions rates. The nighttime reaction of isoprene with the NO3 radical has a large potential to contribute to SOA. We classified isoprene nitrates into generations and proposed formation pathways. Considering the potential functionalization of the isoprene nitrates we propose that mainly isoprene dimers contribute to SOA formation from the isoprene NO3 reactions with at least a 5 % mass yield.
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. Discuss., https://doi.org/10.5194/acp-2020-1187, https://doi.org/10.5194/acp-2020-1187, 2020
Preprint under review for ACP
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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.
Chaomin Wang, Bin Yuan, Caihong Wu, Sihang Wang, Jipeng Qi, Baolin Wang, Zelong Wang, Weiwei Hu, Wei Chen, Chenshuo Ye, Wenjie Wang, Yele Sun, Chen Wang, Shan Huang, Wei Song, Xinming Wang, Suxia Yang, Shenyang Zhang, Wanyun Xu, Nan Ma, Zhanyi Zhang, Bin Jiang, Hang Su, Yafang Cheng, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 20, 14123–14138, https://doi.org/10.5194/acp-20-14123-2020, https://doi.org/10.5194/acp-20-14123-2020, 2020
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We utilized a novel online mass spectrometry method to measure the total concentration of higher alkanes at each carbon number at two different sites in China, allowing us to take into account SOA contributions from all isomers for higher alkanes. We found that higher alkanes account for significant fractions of SOA formation at the two sites. The contributions are comparable to or even higher than single-ring aromatics, the most-recognized SOA precursors in urban air.
Junfeng Wang, Jianhuai Ye, Dantong Liu, Yangzhou Wu, Jian Zhao, Weiqi Xu, Conghui Xie, Fuzhen Shen, Jie Zhang, Paul E. Ohno, Yiming Qin, Xiuyong Zhao, Scot T. Martin, Alex K. Y. Lee, Pingqing Fu, Daniel J. Jacob, Qi Zhang, Yele Sun, Mindong Chen, and Xinlei Ge
Atmos. Chem. Phys., 20, 14091–14102, https://doi.org/10.5194/acp-20-14091-2020, https://doi.org/10.5194/acp-20-14091-2020, 2020
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We compared the organics in total submicron matter and those coated on BC cores during summertime in Beijing and found large differences between them. Traffic-related OA was associated significantly with BC, while cooking-related OA did not coat BC. In addition, a factor likely originated from primary biomass burning OA was only identified in BC-containing particles. Such a unique BBOA requires further field and laboratory studies to verify its presence and elucidate its properties and impacts.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Hongyu Guo, Duseong S. Jo, Anne V. Handschy, Demetrios Pagonis, Jason C. Schroder, Melinda K. Schueneman, Michael J. Cubison, Jack E. Dibb, Alma Hodzic, Weiwei Hu, Brett B. Palm, and Jose L. Jimenez
Atmos. Meas. Tech., 13, 6193–6213, https://doi.org/10.5194/amt-13-6193-2020, https://doi.org/10.5194/amt-13-6193-2020, 2020
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Collecting particulate matter, or aerosols, onto filters to be analyzed offline is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
Clara Betancourt, Christoph Küppers, Uta Sager, Andrea B. Hoyer, Heinz Kaminski, Gerhard Rapp, Astrid C. John, Miriam Küpper, Ulrich Quass, Thomas Kuhlbusch, Jochen Rudolph, Astrid Kiendler-Scharr, and Iulia Gensch
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1133, https://doi.org/10.5194/acp-2020-1133, 2020
Revised manuscript accepted for ACP
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For the first time, we included stable isotopes into the Lagrangian Particle Dispersion Model FLEXPART to investigate firewood home heating aerosol. This is an innovative source apportionment methodology since comparison of stable isotope ratio model predictions with observations deliver quantitative understanding of atmospheric processes. For this study, the home heating aerosol in residential areas was not of remote origin and thus, mitigation could be achieved by reducing local emissions.
Defeng Zhao, Iida Pullinen, Hendrik Fuchs, Stephanie Schrade, Rongrong Wu, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Yindong Guo, Astrid Kiendler-Scharr, Andreas Wahner, Sungah Kang, Luc Vereecken, and Thomas F. Mentel
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1178, https://doi.org/10.5194/acp-2020-1178, 2020
Preprint under review for ACP
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The reaction of isoprene, a biogenic volatile organic compound with the globally largest emission rates, with NO3, an nighttime oxidant influenced heavily by anthrogogenic emissions, forms a large number of highly oxygenated organic molecules (HOM). These HOM are formed via one or multiple oxidation steps, followed by autoxidation. Their total yield is much higher than that in the daytime oxidation of isoprene. They may play an important role in nighttime organic aerosol formation and growth.
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. Discuss., https://doi.org/10.5194/acp-2020-1018, https://doi.org/10.5194/acp-2020-1018, 2020
Revised manuscript accepted for ACP
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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.
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
Michael Rolletter, Marion Blocquet, Martin Kaminski, Birger Bohn, Hans-Peter Dorn, Andreas Hofzumahaus, Frank Holland, Xin Li, Franz Rohrer, Ralf Tillmann, Robert Wegener, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 20, 13701–13719, https://doi.org/10.5194/acp-20-13701-2020, https://doi.org/10.5194/acp-20-13701-2020, 2020
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The photooxidation of pinonaldehyde is investigated in a chamber study under natural sunlight and low NO conditions with and without an added hydroxyl radical (OH) scavenger. The experimentally determined pinonaldehyde photolysis frequency is faster by a factor of 3.5 than currently used parameterizations in atmospheric models. Yields of degradation products are measured in the presence and absence of OH. Measurements are compared to current atmospheric models and a theory-based mechanism.
Jake P. Rowe, Andrew T. Lambe, and William H. Brune
Atmos. Chem. Phys., 20, 13417–13424, https://doi.org/10.5194/acp-20-13417-2020, https://doi.org/10.5194/acp-20-13417-2020, 2020
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We conducted a series of experiments in which the 185 to 254 nm photon flux ratio (I185 : I254) emitted by low-pressure mercury lamps installed in an oxidation flow reactor (OFR) was systematically varied using multiple novel lamp configurations. Integrated OH exposure values achieved for each lamp type were obtained as a function of OFR operating conditions. A photochemical box model was used to develop a generalized OH exposure estimation equation as a function of [H2O], [O3], and OH reactivity.
Roger Seco, Thomas Holst, Mikkel Sillesen Matzen, Andreas Westergaard-Nielsen, Tao Li, Tihomir Simin, Joachim Jansen, Patrick Crill, Thomas Friborg, Janne Rinne, and Riikka Rinnan
Atmos. Chem. Phys., 20, 13399–13416, https://doi.org/10.5194/acp-20-13399-2020, https://doi.org/10.5194/acp-20-13399-2020, 2020
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Northern ecosystems exchange climate-relevant trace gases with the atmosphere, including volatile organic compounds (VOCs). We measured VOC fluxes from a subarctic permafrost-free fen and its adjacent lake in northern Sweden. The graminoid-dominated fen emitted mainly isoprene during the peak of the growing season, with a pronounced response to increasing temperatures stronger than assumed by biogenic emission models. The lake was a sink of acetone and acetaldehyde during both periods measured.
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. Discuss., https://doi.org/10.5194/acp-2020-914, https://doi.org/10.5194/acp-2020-914, 2020
Preprint under review for ACP
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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 are predictable and explained by key emissions. These results are used to estimate the premature mortality associated to SOA in urban regions.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Chen Dayan, Erick Fredj, Pawel K. Misztal, Maor Gabay, Alex B. Guenther, and Eran Tas
Atmos. Chem. Phys., 20, 12741–12759, https://doi.org/10.5194/acp-20-12741-2020, https://doi.org/10.5194/acp-20-12741-2020, 2020
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We studied the emission of biogenic volatile organic compounds from both marine and terrestrial ecosystems in the Eastern Mediterranean Basin, a global warming hot spot. We focused on isoprene and dimethyl sulfide (DMS), which are well recognized for their effect on climate and strong impact on photochemical pollution by the former. We found high emissions of isoprene and a strong decadal decrease in the emission of DMS which can both be attributed to the strong increase in seawater temperature.
Chinmoy Sarkar, Gracie Wong, Anne Mielnik, Alex B. Guenther, Taehyung Lee, Taehyun Park, Jihee Ban, Seokwon Kang, Jin-Soo Park, Joonyoung Ahn, Danbi Kim, Hyunjae Kim, Jinsoo Choi, Beom-Keon Seo, Jong-Ho Kim, Jeong-Ho Kim, Soo Bog Park, and Saewung Kim
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1103, https://doi.org/10.5194/acp-2020-1103, 2020
Preprint under review for ACP
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We present experimental proofs illustrating emission of ketene in an industrial facility in South Korea. It has been rarely reported the emission of such a compound but our experimental data shows that the emission rate is substantial. It potentially has tremendous implication in regional air quality and public health as it is highly reactive and toxic at the sometime.
Aikaterini Bougiatioti, Athanasios Nenes, Jack J. Lin, Charles A. Brock, Joost A. de Gouw, Jin Liao, Ann M. Middlebrook, and André Welti
Atmos. Chem. Phys., 20, 12163–12176, https://doi.org/10.5194/acp-20-12163-2020, https://doi.org/10.5194/acp-20-12163-2020, 2020
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The number concentration of droplets in clouds in the summertime in the southeastern United States is influenced by aerosol variations but limited by the strong competition for supersaturated water vapor. Concurrent variations in vertical velocity magnify the response of cloud droplet number to aerosol increases by up to a factor of 5. Omitting the covariance of vertical velocity with aerosol number may therefore bias estimates of the cloud albedo effect from aerosols.
Kouji Adachi, Naga Oshima, Zhaoheng Gong, Suzane de Sá, Adam P. Bateman, Scot T. Martin, Joel F. de Brito, Paulo Artaxo, Glauber G. Cirino, Arthur J. Sedlacek III, and Peter R. Buseck
Atmos. Chem. Phys., 20, 11923–11939, https://doi.org/10.5194/acp-20-11923-2020, https://doi.org/10.5194/acp-20-11923-2020, 2020
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Occurrences, size distributions, and number fractions of individual aerosol particles from the Amazon basin during the GoAmazon2014/5 campaign were analyzed using transmission electron microscopy. Aerosol particles from natural sources (e.g., mineral dust, primary biological aerosols, and sea salts) during the wet season originated from the Amazon forest and long-range transports (the Saharan desert and the Atlantic Ocean). They commonly mix at an individual particle scale during transport.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-973, https://doi.org/10.5194/acp-2020-973, 2020
Preprint under review for ACP
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction (RF) of •OH among detected radicals, but negatively correlated with the RF of C-centered radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
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.
Young-Chul Song, Ariana G. Bé, Scot T. Martin, Franz M. Geiger, Allan K. Bertram, Regan J. Thomson, and Mijung Song
Atmos. Chem. Phys., 20, 11263–11273, https://doi.org/10.5194/acp-20-11263-2020, https://doi.org/10.5194/acp-20-11263-2020, 2020
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We report the liquid–liquid phase separation (LLPS) of organic aerosol consisting of α-pinene- and β-caryophyllene-derived ozonolysis products and commercial organic compounds. As compositional complexity increased from one to two organic species, LLPS occurred over a wider range of average O : C values (increasing from 0.44 to 0.67). These results provide further evidence that LLPS is likely frequent in organic aerosol particles in the troposphere, even in the absence of inorganic salt.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-924, https://doi.org/10.5194/acp-2020-924, 2020
Revised manuscript accepted for ACP
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Functional group composition 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.
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.
Yutong Liang, Coty N. Jen, Robert J. Weber, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-910, https://doi.org/10.5194/acp-2020-910, 2020
Revised manuscript accepted for ACP
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This article reports the molecular composition of smoke particles people in SF Bay Area were exposed to during northern California wildfires Oct. 2017. Major components include sugars, acids, aromatics and terpenoids. These observations can be used to better understand health impacts of smoke exposure. Tracer compounds indicate which fuels burned, including diterpenoids for softwood and syringyls for hardwood. Statistical analysis reveals a group of secondary compounds formed in daytime aging.
Iida Pullinen, Sebastian Schmitt, Sungah Kang, Mehrnaz Sarrafzadeh, Patrick Schlag, Stefanie Andres, Einhard Kleist, Thomas F. Mentel, Franz Rohrer, Monika Springer, Ralf Tillmann, Jürgen Wildt, Cheng Wu, Defeng Zhao, Andreas Wahner, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 20, 10125–10147, https://doi.org/10.5194/acp-20-10125-2020, https://doi.org/10.5194/acp-20-10125-2020, 2020
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Biogenic and anthropogenic air masses mix in the atmosphere, bringing plant-emitted monoterpenes and traffic-related nitrogen oxides together. There is debate whether the presence of nitrogen oxides reduces or increases secondary aerosol formation. This is important as secondary aerosols have cooling effects in the climate system but also constitute a health risk in populated areas. We show that the presence of NOx alone should not much affect the mass yields of secondary organic aerosols.
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, Andre Stephan Henry Prevot, and Jay Gates Slowik
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-835, https://doi.org/10.5194/acp-2020-835, 2020
Preprint under review for ACP
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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 fall 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, (2) under high NOx and RH conditions, aqueous phase chemistry can be a major contributor to SOA formation.
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.
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. Discuss., https://doi.org/10.5194/amt-2020-264, https://doi.org/10.5194/amt-2020-264, 2020
Revised manuscript under review for AMT
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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.
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.
James M. Roberts, Chelsea E. Stockwell, Robert J. Yokelson, Joost de Gouw, Yong Liu, Vanessa Selimovic, Abigail R. Koss, Kanako Sekimoto, Matthew M. Coggon, Bin Yuan, Kyle J. Zarzana, Steven S. Brown, Cristina Santin, Stefan H. Doerr, and Carsten Warneke
Atmos. Chem. Phys., 20, 8807–8826, https://doi.org/10.5194/acp-20-8807-2020, https://doi.org/10.5194/acp-20-8807-2020, 2020
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We measured total reactive nitrogen, Nr, in lab fires from western North American fuels, along with measurements of individual nitrogen compounds. We measured the amount of N that gets converted to inactive compounds (avg. 70 %), and the amount that is accounted for by individual species (85 % of remaining N). We provide guidelines for how the reactive nitrogen is distributed among individual compounds such as NOx and ammonia. This will help estimates and predictions of wildfire emissions.
Christopher D. Cappa, Christopher Y. Lim, David H. Hagan, Matthew Coggon, Abigail Koss, Kanako Sekimoto, Joost de Gouw, Timothy B. Onasch, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 8511–8532, https://doi.org/10.5194/acp-20-8511-2020, https://doi.org/10.5194/acp-20-8511-2020, 2020
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Smoke from combustion of a wide range of biomass fuels (e.g., leaves, twigs, logs, peat, and dung) was photochemically aged in a small chamber for up to 8 d of equivalent atmospheric aging. Upon aging, the particle chemical composition and ability to absorb sunlight changed owing to reactions in both the gas and particulate phases. We developed a model to explain the observations and used this to derive insights into the aging of smoke in the atmosphere.
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.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Revised manuscript has not been submitted
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Yunle Chen, Masayuki Takeuchi, Theodora Nah, Lu Xu, Manjula R. Canagaratna, Harald Stark, Karsten Baumann, Francesco Canonaco, André S. H. Prévôt, L. Gregory Huey, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 20, 8421–8440, https://doi.org/10.5194/acp-20-8421-2020, https://doi.org/10.5194/acp-20-8421-2020, 2020
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Two online mass spectrometry instruments, an aerosol mass spectrometer and a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols, were deployed at Yorkville, GA, for a comprehensive characterization of organic aerosol. We observed notable secondary organic aerosol formation from isoprene and monoterpenes via different pathways during both day and night, and a series of highly oxidized acid-like compounds was found to be closely related to aged SOA.
Ryan Schmedding, Quazi Z. Rasool, Yue Zhang, Havala O. T. Pye, Haofei Zhang, Yuzhi Chen, Jason D. Surratt, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Allen H. Goldstein, and William Vizuete
Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, https://doi.org/10.5194/acp-20-8201-2020, 2020
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Accurate model prediction of aerosol concentrations is a known challenge. It is assumed in many modeling systems that aerosols are in a homogeneously mixed phase state. It has been observed that aerosols do phase separate and can form a highly viscous organic shell with an aqueous core impacting the formation processes of aerosols. This work is a model implementation to determine an aerosol's phase state using glass transition temperature and aerosol composition.
Ying Li, Douglas A. Day, Harald Stark, Jose L. Jimenez, and Manabu Shiraiwa
Atmos. Chem. Phys., 20, 8103–8122, https://doi.org/10.5194/acp-20-8103-2020, https://doi.org/10.5194/acp-20-8103-2020, 2020
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Viscosity is an important property of organic aerosols, but viscosity measurements of ambient organic aerosols are scarce. We developed a method to predict glass transition temperatures using volatility and the atomic oxygen-to-carbon ratio. The method was applied to field observations of volatility distributions to predict viscosity of ambient organic aerosols, yielding consistent results with ambient particle phase-state measurements and global simulations.
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.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Junchen Guo, Shengzhen Zhou, Mingfu Cai, Jun Zhao, Wei Song, Weixiong Zhao, Weiwei Hu, Yele Sun, Yao He, Chengqiang Yang, Xuezhe Xu, Zhisheng Zhang, Peng Cheng, Qi Fan, Jian Hang, Shaojia Fan, Xinming Wang, and Xuemei Wang
Atmos. Chem. Phys., 20, 7595–7615, https://doi.org/10.5194/acp-20-7595-2020, https://doi.org/10.5194/acp-20-7595-2020, 2020
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We characterized non-refractory submicron particulate matter (PM1.0) during winter in Guangzhou, south China. Chemical composition and key sources of ambient PM1.0 are revealed, highlighting the significant role of SOA. The relationship with SOA and peroxy radicals indicated gas-phase oxidation contributed predominantly to SOA formation during non-pollution periods, while heterogeneous/multiphase reactions played more important roles in SOA formation during pollution periods.
Evelyn Freney, Karine Sellegri, Alessia Nicosia, Jonathan T. Trueblood, Matteo Rinaldi, Leah R. Williams, 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, Hilka Timmonen, and Cécile Guieu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-406, https://doi.org/10.5194/acp-2020-406, 2020
Revised manuscript accepted for ACP
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In this work, we present observations of the organic aerosol content in primary sea spray aerosols (SSA) continuously generated along a five-weeks 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.
Chinmoy Sarkar, Alex B. Guenther, Jeong-Hoo Park, Roger Seco, Eliane Alves, Sarah Batalha, Raoni Santana, Saewung Kim, James Smith, Julio Tóta, and Oscar Vega
Atmos. Chem. Phys., 20, 7179–7191, https://doi.org/10.5194/acp-20-7179-2020, https://doi.org/10.5194/acp-20-7179-2020, 2020
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Biogenic volatile organic compounds (BVOCs) are important components of the atmosphere due to their contribution to atmospheric chemistry and biogeochemical cycles. In this study, we report major BVOCs, e.g. isoprene and total monoterpene flux measurements with a proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) using the eddy covariance (EC) method at a primary rainforest in eastern Amazonia. We used the measured data to evaluate the MEGAN2.1 model for the emission site.
Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Douglas A. Day, Jason C. Schroder, Jack E. Dibb, Maximilian Dollner, Bernadett Weinzierl, and Jose L. Jimenez
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-224, https://doi.org/10.5194/amt-2020-224, 2020
Revised manuscript accepted for AMT
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We utilize a set of high-quality datasets collected during the NASA ATom aircraft mission to investigate the impact of differences in observable particle sizes across aerosol instruments, in aerosol measurement comparisons. Very good agreement was found between chemically and physically derived submicron aerosol volume. Results support a lack of significant unknown biases in the response of Aerodyne Aerosol Mass Spectrometer (AMS) when sampling remote aerosols across the globe.
Pablo E. Saide, Meng Gao, Zifeng Lu, Daniel L. Goldberg, David G. Streets, Jung-Hun Woo, Andreas Beyersdorf, Chelsea A. Corr, Kenneth L. Thornhill, Bruce Anderson, Johnathan W. Hair, Amin R. Nehrir, Glenn S. Diskin, Jose L. Jimenez, Benjamin A. Nault, Pedro Campuzano-Jost, Jack Dibb, Eric Heim, Kara D. Lamb, Joshua P. Schwarz, Anne E. Perring, Jhoon Kim, Myungje Choi, Brent Holben, Gabriele Pfister, Alma Hodzic, Gregory R. Carmichael, Louisa Emmons, and James H. Crawford
Atmos. Chem. Phys., 20, 6455–6478, https://doi.org/10.5194/acp-20-6455-2020, https://doi.org/10.5194/acp-20-6455-2020, 2020
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Air quality forecasts over the Korean Peninsula captured aerosol optical depth but largely overpredicted surface PM during a Chinese haze transport event. Model deficiency was related to the calculation of optical properties. In order to improve it, aerosol size representation needs to be refined in the calculations, and the representation of aerosol properties, such as size distribution, chemical composition, refractive index, hygroscopicity parameter, and density, needs to be improved.
Sam J. Silva, Colette L. Heald, and Alex B. Guenther
Geosci. Model Dev., 13, 2569–2585, https://doi.org/10.5194/gmd-13-2569-2020, https://doi.org/10.5194/gmd-13-2569-2020, 2020
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Simulating the influence of the biosphere on atmospheric chemistry has traditionally been computationally intensive. We describe a surrogate canopy physics model parameterized using a statistical learning technique and specifically designed for use in large-scale chemical transport models. Our surrogate model reproduces a more detailed model to within 10 % without a large computational demand, improving the process representation of biosphere–atmosphere exchange.
Camille Mouchel-Vallon, Julia Lee-Taylor, Alma Hodzic, Paulo Artaxo, Bernard Aumont, Marie Camredon, David Gurarie, Jose-Luis Jimenez, Donald H. Lenschow, Scot T. Martin, Janaina Nascimento, John J. Orlando, Brett B. Palm, John E. Shilling, Manish Shrivastava, and Sasha Madronich
Atmos. Chem. Phys., 20, 5995–6014, https://doi.org/10.5194/acp-20-5995-2020, https://doi.org/10.5194/acp-20-5995-2020, 2020
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The GoAmazon 2014/5 field campaign took place near the city of Manaus, Brazil, isolated in the Amazon rainforest, to study the impacts of urban pollution on natural air masses. We simulated this campaign with an extremely detailed organic chemistry model to understand how the city would affect the growth and composition of natural aerosol particles. Discrepancies between the model and the measurements indicate that the chemistry of naturally emitted organic compounds is still poorly understood.
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.
Andrew T. Lambe, Ezra C. Wood, Jordan E. Krechmer, Francesca Majluf, Leah R. Williams, Philip L. Croteau, Manuela Cirtog, Anaïs Féron, Jean-Eudes Petit, Alexandre Albinet, Jose L. Jimenez, and Zhe Peng
Atmos. Meas. Tech., 13, 2397–2411, https://doi.org/10.5194/amt-13-2397-2020, https://doi.org/10.5194/amt-13-2397-2020, 2020
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We present a new method to continuously generate N2O5 in the gas phase that is injected into a reactor where it decomposes to generate nitrate radicals (NO3). To assess the applicability of the method towards different chemical systems, we present experimental and model characterization of the integrated NO3 exposure and other metrics as a function of operating conditions. We demonstrate the method by characterizing secondary organic aerosol particles generated from the β-pinene + NO3 reaction.
Alma Hodzic, Pedro Campuzano-Jost, Huisheng Bian, Mian Chin, Peter R. Colarco, Douglas A. Day, Karl D. Froyd, Bernd Heinold, Duseong S. Jo, Joseph M. Katich, John K. Kodros, Benjamin A. Nault, Jeffrey R. Pierce, Eric Ray, Jacob Schacht, Gregory P. Schill, Jason C. Schroder, Joshua P. Schwarz, Donna T. Sueper, Ina Tegen, Simone Tilmes, Kostas Tsigaridis, Pengfei Yu, and Jose L. Jimenez
Atmos. Chem. Phys., 20, 4607–4635, https://doi.org/10.5194/acp-20-4607-2020, https://doi.org/10.5194/acp-20-4607-2020, 2020
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Organic aerosol (OA) is a key source of uncertainty in aerosol climate effects. We present the first pole-to-pole OA characterization during the NASA Atmospheric Tomography aircraft mission. OA has a strong seasonal and zonal variability, with the highest levels in summer and over fire-influenced regions and the lowest ones in the southern high latitudes. We show that global models predict the OA distribution well but not the relative contribution of OA emissions vs. chemical production.
Alexander B. Thames, William H. Brune, David O. Miller, Hannah M. Allen, Eric C. Apel, Donald R. Blake, T. Paul Bui, Roisin Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, Joshua P. DiGangi, James W. Elkins, Samuel R. Hall, Thomas F. Hanisco, Reem A. Hannun, Eric Hintsa, Rebecca S. Hornbrook, Michelle J. Kim, Kathryn McKain, Fred L. Moore, Julie M. Nicely, Jeffrey Peischl, Thomas B. Ryerson, Jason M. St. Clair, Colm Sweeney, Alex Teng, Chelsea R. Thompson, Kirk Ullmann, Paul O. Wennberg, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 4013–4029, https://doi.org/10.5194/acp-20-4013-2020, https://doi.org/10.5194/acp-20-4013-2020, 2020
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Oceans and the atmosphere exchange volatile gases that react with the hydroxyl radical (OH). During a NASA airborne study, measurements of the total frequency of OH reactions, called the OH reactivity, were made in the marine boundary layer of the Atlantic and Pacific oceans. The measured OH reactivity often exceeded the OH reactivity calculated from measured chemical species. This missing OH reactivity appears to be from unmeasured volatile organic compounds coming out of the ocean.
Dianne Sanchez, Roger Seco, Dasa Gu, Alex Guenther, John Mak, Youngjae Lee, Danbi Kim, Joonyoung Ahn, Don Blake, Scott Herndon, Daun Jeong, John T. Sullivan, Thomas Mcgee, and Saewung Kim
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-174, https://doi.org/10.5194/acp-2020-174, 2020
Revised manuscript accepted for ACP
Anna Novelli, Luc Vereecken, Birger Bohn, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, David Reimer, Franz Rohrer, Simon Rosanka, Domenico Taraborrelli, Ralf Tillmann, Robert Wegener, Zhujun Yu, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 20, 3333–3355, https://doi.org/10.5194/acp-20-3333-2020, https://doi.org/10.5194/acp-20-3333-2020, 2020
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Experimental evidence from a simulation chamber study shows that the regeneration efficiency of the hydroxyl radical is maintained globally at values higher than 0.5 for a wide range of nitrogen oxide concentrations as a result of isomerizations of peroxy radicals originating from the OH oxidation of isoprene. The available models were tested, and suggestions on how to improve their ability to reproduce the measured radical and oxygenated volatile organic compound concentrations are provided.
Sidhant J. Pai, Colette L. Heald, Jeffrey R. Pierce, Salvatore C. Farina, Eloise A. Marais, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Ann M. Middlebrook, Hugh Coe, John E. Shilling, Roya Bahreini, Justin H. Dingle, and Kennedy Vu
Atmos. Chem. Phys., 20, 2637–2665, https://doi.org/10.5194/acp-20-2637-2020, https://doi.org/10.5194/acp-20-2637-2020, 2020
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Aerosols in the atmosphere have significant health and climate impacts. Organic aerosol (OA) accounts for a large fraction of the total aerosol burden, but models have historically struggled to accurately simulate it. This study compares two very different OA model schemes and evaluates them against a suite of globally distributed airborne measurements with the goal of providing insight into the strengths and weaknesses of each approach across different environments.
Yu Wang, Ying Chen, Zhijun Wu, Dongjie Shang, Yuxuan Bian, Zhuofei Du, Sebastian H. Schmitt, Rong Su, Georgios I. Gkatzelis, Patrick Schlag, Thorsten Hohaus, Aristeidis Voliotis, Keding Lu, Limin Zeng, Chunsheng Zhao, M. Rami Alfarra, Gordon McFiggans, Alfred Wiedensohler, Astrid Kiendler-Scharr, Yuanhang Zhang, and Min Hu
Atmos. Chem. Phys., 20, 2161–2175, https://doi.org/10.5194/acp-20-2161-2020, https://doi.org/10.5194/acp-20-2161-2020, 2020
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Severe haze events, with high particulate nitrate (pNO3−) burden, frequently prevail in Beijing. In this study, we demonstrate a mutual-promotion effect between aerosol water uptake and pNO3− formation backed up by theoretical calculations and field observations throughout a typical pNO3−-dominated haze event in Beijing wintertime. This self-amplified mutual-promotion effect between aerosol water content and particulate nitrate can rapidly deteriorate air quality and degrade visibility.
Therese S. Carter, Colette L. Heald, Jose L. Jimenez, Pedro Campuzano-Jost, Yutaka Kondo, Nobuhiro Moteki, Joshua P. Schwarz, Christine Wiedinmyer, Anton S. Darmenov, Arlindo M. da Silva, and Johannes W. Kaiser
Atmos. Chem. Phys., 20, 2073–2097, https://doi.org/10.5194/acp-20-2073-2020, https://doi.org/10.5194/acp-20-2073-2020, 2020
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Fires and the smoke they emit impact air quality, health, and climate, but the abundance and properties of smoke remain uncertain and poorly constrained. To explore this, we compare model simulations driven by four commonly-used fire emission inventories with surface, aloft, and satellite observations. We show that across inventories smoke emissions differ by factors of 4 to 7 over North America, challenging our ability to accurately characterize the impact of smoke on air quality and climate.
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.
Joseph R. Salazar, Benton T. Cartledge, John P. Haynes, Rachel York-Marini, Allen L. Robinson, Greg T. Drozd, Allen H. Goldstein, Sirine C. Fakra, and Brian J. Majestic
Atmos. Chem. Phys., 20, 1849–1860, https://doi.org/10.5194/acp-20-1849-2020, https://doi.org/10.5194/acp-20-1849-2020, 2020
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The solubility of atmospheric iron is important in human health and environmental chemistry. To understand the origin of water-soluble iron in urban areas, tailpipe emissions were collected from 32 low-emitting vehicles, from which iron solubility averaged 30 % (0–82 %), more than 10 times the average in the Earth's crust. Water-soluble iron was independent of almost all exhaust components and of the iron phase in the particles but was correlated with specific exhaust-derived organic compounds.
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.
Fan Mei, Jian Wang, Jennifer M. Comstock, Ralf Weigel, Martina Krämer, Christoph Mahnke, John E. Shilling, Johannes Schneider, Christiane Schulz, Charles N. Long, Manfred Wendisch, Luiz A. T. Machado, Beat Schmid, Trismono Krisna, Mikhail Pekour, John Hubbe, Andreas Giez, Bernadett Weinzierl, Martin Zoeger, Mira L. Pöhlker, Hans Schlager, Micael A. Cecchini, Meinrat O. Andreae, Scot T. Martin, Suzane S. de Sá, Jiwen Fan, Jason Tomlinson, Stephen Springston, Ulrich Pöschl, Paulo Artaxo, Christopher Pöhlker, Thomas Klimach, Andreas Minikin, Armin Afchine, and Stephan Borrmann
Atmos. Meas. Tech., 13, 661–684, https://doi.org/10.5194/amt-13-661-2020, https://doi.org/10.5194/amt-13-661-2020, 2020
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In 2014, the US DOE G1 aircraft and the German HALO aircraft overflew the Amazon basin to study how aerosols influence cloud cycles under a clean condition and around a tropical megacity. This paper describes how to meaningfully compare similar measurements from two research aircraft and identify the potential measurement issue. We also discuss the uncertainty range for each measurement for further usage in model evaluation and satellite data validation.
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.
Olga Garmash, Matti P. Rissanen, Iida Pullinen, Sebastian Schmitt, Oskari Kausiala, Ralf Tillmann, Defeng Zhao, Carl Percival, Thomas J. Bannan, Michael Priestley, Åsa M. Hallquist, Einhard Kleist, Astrid Kiendler-Scharr, Mattias Hallquist, Torsten Berndt, Gordon McFiggans, Jürgen Wildt, Thomas F. Mentel, and Mikael Ehn
Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, https://doi.org/10.5194/acp-20-515-2020, 2020
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Highly oxygenated organic molecules (HOMs) facilitate aerosol formation in the atmosphere. Using NO3− chemical ionization mass spectrometry we investigated HOM composition and yield in oxidation of aromatic compounds at different reactant concentrations, in the presence of NOx and seed aerosol. Higher OH concentrations increased HOM yield, suggesting multiple oxidation steps, and affected HOM composition, potentially explaining in part discrepancies in published secondary organic aerosol yields.
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
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, https://doi.org/10.5194/acp-19-14875-2019, 2019
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Wildfire emissions significantly contribute to adverse air quality; however, the chemical processes that lead to hazardous pollutants, such as ozone, are not fully understood. In this study, we describe laboratory experiments where we simulate the atmospheric chemistry of smoke emitted from a range of biomass fuels. We show that certain understudied compounds, such as furans and phenolic compounds, are significant contributors to pollutants formed as a result of typical atmospheric oxidation.
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.
Jiajue Chai, David J. Miller, Eric Scheuer, Jack Dibb, Vanessa Selimovic, Robert Yokelson, Kyle J. Zarzana, Steven S. Brown, Abigail R. Koss, Carsten Warneke, and Meredith Hastings
Atmos. Meas. Tech., 12, 6303–6317, https://doi.org/10.5194/amt-12-6303-2019, https://doi.org/10.5194/amt-12-6303-2019, 2019
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Isotopic analysis offers a potential tool to distinguish between sources and interpret transformation pathways of atmospheric species. We applied recently developed techniques in our lab to characterize the isotopic composition of reactive nitrogen species (NOx, HONO, HNO3, pNO3-) in fresh biomass burning emissions. Intercomparison with other techniques confirms the suitability of our methods, allowing for future applications of our techniques in a variety of environments.
Rupert Holzinger, W. Joe F. Acton, William J. Bloss, Martin Breitenlechner, Leigh R. Crilley, Sébastien Dusanter, Marc Gonin, Valerie Gros, Frank N. Keutsch, Astrid Kiendler-Scharr, Louisa J. Kramer, Jordan E. Krechmer, Baptiste Languille, Nadine Locoge, Felipe Lopez-Hilfiker, Dušan Materić, Sergi Moreno, Eiko Nemitz, Lauriane L. J. Quéléver, Roland Sarda Esteve, Stéphane Sauvage, Simon Schallhart, Roberto Sommariva, Ralf Tillmann, Sergej Wedel, David R. Worton, Kangming Xu, and Alexander Zaytsev
Atmos. Meas. Tech., 12, 6193–6208, https://doi.org/10.5194/amt-12-6193-2019, https://doi.org/10.5194/amt-12-6193-2019, 2019
Karl D. Froyd, Daniel M. Murphy, Charles A. Brock, Pedro Campuzano-Jost, Jack E. Dibb, Jose-Luis Jimenez, Agnieszka Kupc, Ann M. Middlebrook, Gregory P. Schill, Kenneth L. Thornhill, Christina J. Williamson, James C. Wilson, and Luke D. Ziemba
Atmos. Meas. Tech., 12, 6209–6239, https://doi.org/10.5194/amt-12-6209-2019, https://doi.org/10.5194/amt-12-6209-2019, 2019
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Single-particle mass spectrometer (SPMS) instruments characterize the composition of individual aerosol particles in real time. We present a new method that combines SPMS composition with independently measured particle size distributions to determine absolute number, surface area, volume, and mass concentrations of mineral dust, biomass burning, sea salt, and other climate-relevant atmospheric particle types, with a fast time response applicable to aircraft sampling.
Brett B. Palm, Xiaoxi Liu, Jose L. Jimenez, and Joel A. Thornton
Atmos. Meas. Tech., 12, 5829–5844, https://doi.org/10.5194/amt-12-5829-2019, https://doi.org/10.5194/amt-12-5829-2019, 2019
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We introduce a coaxial, low-pressure ion–molecule reaction (IMR) region for iodide-adduct chemical ionization mass spectrometry, designed to decrease the effects of IMR wall interactions with organic/inorganic gases. This IMR has 3–10 times shorter delay times than previous IMRs. We introduce a conceptual framework for understanding and subtracting the background signal due to analyte molecules interacting with IMR walls. This framework can be applied to other tubing and instrument systems.
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.
Hayley S. Glicker, Michael J. Lawler, John Ortega, Suzane S. de Sá, Scot T. Martin, Paulo Artaxo, Oscar Vega Bustillos, Rodrigo de Souza, Julio Tota, Annmarie Carlton, and James N. Smith
Atmos. Chem. Phys., 19, 13053–13066, https://doi.org/10.5194/acp-19-13053-2019, https://doi.org/10.5194/acp-19-13053-2019, 2019
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An understanding of the chemical composition of the smallest particles in the air over the Amazon Basin provides insights into the natural and human-caused influences on particle production in this sensitive region. We present measurements of the composition of sub-100 nm diameter particles performed during the wet season and identify unique constituents that point to both natural and human-caused sources and processes.
Daun Jeong, Roger Seco, Dasa Gu, Youngro Lee, Benjamin A. Nault, Christoph J. Knote, Tom Mcgee, John T. Sullivan, Jose L. Jimenez, Pedro Campuzano-Jost, Donald R. Blake, Dianne Sanchez, Alex B. Guenther, David Tanner, L. Gregory Huey, Russell Long, Bruce E. Anderson, Samuel R. Hall, Kirk Ullmann, Hye-jung Shin, Scott C. Herndon, Youngjae Lee, Danbi Kim, Joonyoung Ahn, and Saewung Kim
Atmos. Chem. Phys., 19, 12779–12795, https://doi.org/10.5194/acp-19-12779-2019, https://doi.org/10.5194/acp-19-12779-2019, 2019
Christopher Y. Lim, David H. Hagan, Matthew M. Coggon, Abigail R. Koss, Kanako Sekimoto, Joost de Gouw, Carsten Warneke, Christopher D. Cappa, and Jesse H. Kroll
Atmos. Chem. Phys., 19, 12797–12809, https://doi.org/10.5194/acp-19-12797-2019, https://doi.org/10.5194/acp-19-12797-2019, 2019
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Wildfires are a large source of gases and particles to the atmosphere, both of which impact human health and climate. The amount and composition of particles from wildfires can change with time in the atmosphere; however, the impact of aging is not well understood. In a series of controlled laboratory experiments, we show that the particles are oxidized and a significant fraction of the gas-phase carbon (24 %–56 %) is converted to particle mass over the course of several days in the atmosphere.
Michael Rolletter, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Hans-Peter Dorn, Xin Li, Anna Lutz, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 19, 11635–11649, https://doi.org/10.5194/acp-19-11635-2019, https://doi.org/10.5194/acp-19-11635-2019, 2019
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Here we present a study of the photooxidation of alpha-pinene, the most abundant monoterpene, by hydroxyl radicals (OH) conducted in the simulation chamber SAPHIR under low NOx and atmospheric alpha-pinene concentrations. Yields of the main degradation products acetone, formaldehyde, and pinonaldehyde were determined and the HOx (OH + HO2) radical budget was investigated. Measurements were used to test current atmospheric models and a theory-based mechanism.
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.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
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Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Xin Chen, Dylan B. Millet, Hanwant B. Singh, Armin Wisthaler, Eric C. Apel, Elliot L. Atlas, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, John D. Crounse, Joost A. de Gouw, Frank M. Flocke, Alan Fried, Brian G. Heikes, Rebecca S. Hornbrook, Tomas Mikoviny, Kyung-Eun Min, Markus Müller, J. Andrew Neuman, Daniel W. O'Sullivan, Jeff Peischl, Gabriele G. Pfister, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Stephen R. Shertz, Chelsea R. Thompson, Victoria Treadaway, Patrick R. Veres, James Walega, Carsten Warneke, Rebecca A. Washenfelder, Petter Weibring, and Bin Yuan
Atmos. Chem. Phys., 19, 9097–9123, https://doi.org/10.5194/acp-19-9097-2019, https://doi.org/10.5194/acp-19-9097-2019, 2019
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Volatile organic compounds (VOCs) affect air quality and modify the lifetimes of other pollutants. We combine a high-resolution 3-D atmospheric model with an ensemble of aircraft observations to perform an integrated analysis of the VOC budget over North America. We find that biogenic emissions provide the main source of VOC reactivity even in most major cities. Our findings point to key gaps in current models related to oxygenated VOCs and to the distribution of VOCs in the free troposphere.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Eloise A. Marais, Zhe Peng, Benjamin A. Nault, Weiwei Hu, Pedro Campuzano-Jost, and Jose L. Jimenez
Geosci. Model Dev., 12, 2983–3000, https://doi.org/10.5194/gmd-12-2983-2019, https://doi.org/10.5194/gmd-12-2983-2019, 2019
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We developed a parameterization method for IEPOX-SOA based on the detailed chemical mechanism. Our parameterizations were tested using a box model and 3-D chemical transport model, which accurately captured the spatiotemporal distribution and response to changes in emissions compared to the explicit full chemistry, while being more computationally efficient. The method developed in this study can be applied to global climate models for long-term studies with a lower computational cost.
Benjamin L. Deming, Demetrios Pagonis, Xiaoxi Liu, Douglas A. Day, Ranajit Talukdar, Jordan E. Krechmer, Joost A. de Gouw, Jose L. Jimenez, and Paul J. Ziemann
Atmos. Meas. Tech., 12, 3453–3461, https://doi.org/10.5194/amt-12-3453-2019, https://doi.org/10.5194/amt-12-3453-2019, 2019
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Losses or measurement delays of gas-phase compounds sampled through tubing are important to atmospheric science. Here we characterize 14 tubing materials by measuring the effects on step changes in organic compound concentration. We find that polymeric tubings exhibit absorptive partitioning behaviour while glass and metal tubings show adsorptive partitioning. Adsorptive materials impart complex humidity, concentration, and VOC–VOC interaction dependencies that absorptive tubings do not.
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.
Suzane S. de Sá, Luciana V. Rizzo, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Lindsay D. Yee, Rebecca Wernis, Gabriel Isaacman-VanWertz, Joel Brito, Samara Carbone, Yingjun J. Liu, Arthur Sedlacek, Stephen Springston, Allen H. Goldstein, Henrique M. J. Barbosa, M. Lizabeth Alexander, Paulo Artaxo, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 19, 7973–8001, https://doi.org/10.5194/acp-19-7973-2019, https://doi.org/10.5194/acp-19-7973-2019, 2019
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This study investigates the impacts of urban and fire emissions on the concentration, composition, and optical properties of submicron particulate matter (PM1) in central Amazonia during the dry season. Biomass-burning and urban emissions appeared to contribute at least 80 % of brown carbon absorption while accounting for 30 % to 40 % of the organic PM1 mass concentration. Only a fraction of the 9-fold increase in mass concentration relative to the wet season was due to biomass burning.
Karena A. McKinney, Daniel Wang, Jianhuai Ye, Jean-Baptiste de Fouchier, Patricia C. Guimarães, Carla E. Batista, Rodrigo A. F. Souza, Eliane G. Alves, Dasa Gu, Alex B. Guenther, and Scot T. Martin
Atmos. Meas. Tech., 12, 3123–3135, https://doi.org/10.5194/amt-12-3123-2019, https://doi.org/10.5194/amt-12-3123-2019, 2019
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Volatile organic compound (VOC) emissions influence air quality and particulate distributions, particularly in major source regions such as the Amazon. A sampler for collecting VOCs from an unmanned aerial vehicle (UAV) is described. Field tests of its performance and an initial example data set collected in the Amazon are also presented. The low cost, ease of use, and maneuverability of UAVs give this method the potential to significantly advance knowledge of the spatial distribution of VOCs.
Xiaoxi Liu, Benjamin Deming, Demetrios Pagonis, Douglas A. Day, Brett B. Palm, Ranajit Talukdar, James M. Roberts, Patrick R. Veres, Jordan E. Krechmer, Joel A. Thornton, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 12, 3137–3149, https://doi.org/10.5194/amt-12-3137-2019, https://doi.org/10.5194/amt-12-3137-2019, 2019
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Delays or losses of gases in sampling tubing and instrumental surfaces due to surface interactions can lead to inaccurate quantification. By sampling with several chemical ionization mass spectrometers and six tubing materials, we quantify delays of semivolatile organic compounds and small polar gases. Delay times generally increase with decreasing volatility or increasing polarity and also depend on materials. The method and results will inform inlet material selection and instrumental design.
Moshe Shechner, Alex Guenther, Robert Rhew, Asher Wishkerman, Qian Li, Donald Blake, Gil Lerner, and Eran Tas
Atmos. Chem. Phys., 19, 7667–7690, https://doi.org/10.5194/acp-19-7667-2019, https://doi.org/10.5194/acp-19-7667-2019, 2019
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Along with other recent studies, our findings point to strong emission of a suite of volatile halogenated organic compounds (VHOCs) from saline soils and salt lakes. Some emitted VHOCs were not known to be emitted from terrestrial sources, and our observations point to apparent new common controls for the emission of several VHOCs. These findings are an important milestone toward a more complete understanding of the effect of VHOCs on atmospheric ozone concentrations and oxidation capacity.
Charles A. Brock, Christina Williamson, Agnieszka Kupc, Karl D. Froyd, Frank Erdesz, Nicholas Wagner, Matthews Richardson, Joshua P. Schwarz, Ru-Shan Gao, Joseph M. Katich, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Jose L. Jimenez, Bernadett Weinzierl, Maximilian Dollner, ThaoPaul Bui, and Daniel M. Murphy
Atmos. Meas. Tech., 12, 3081–3099, https://doi.org/10.5194/amt-12-3081-2019, https://doi.org/10.5194/amt-12-3081-2019, 2019
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From 2016 to 2018 a NASA aircraft profiled the atmosphere from 180 m to ~12 km from the Arctic to the Antarctic over both the Pacific and Atlantic oceans. This program, ATom, sought to sample atmospheric chemical composition to compare with global climate models. We describe the how measurements of particulate matter were made during ATom, and show that the instrument performance was excellent. Data from this project can be used with confidence to evaluate models and compare with satellites.
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.
Zhaofeng Tan, Keding Lu, Andreas Hofzumahaus, Hendrik Fuchs, Birger Bohn, Frank Holland, Yuhan Liu, Franz Rohrer, Min Shao, Kang Sun, Yusheng Wu, Limin Zeng, Yinsong Zhang, Qi Zou, Astrid Kiendler-Scharr, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 19, 7129–7150, https://doi.org/10.5194/acp-19-7129-2019, https://doi.org/10.5194/acp-19-7129-2019, 2019
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Atmospheric OH, HO2, and RO2 radicals; OH reactivity; and trace gases measured in the Pearl River Delta in autumn 2014 are used for radical budget analyses. The RO2 budget suggests that unexplained OH reactivity is due to unmeasured volatile organic compounds. The OH budget points to a missing OH source and that of RO2 to a missing RO2 sink at low NO. This could indicate a common, unknown process that converts RO2 to OH without the involvement of NO, which would reduce ozone production by 30 %.
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.
John T. Sullivan, Thomas J. McGee, Ryan M. Stauffer, Anne M. Thompson, Andrew Weinheimer, Christoph Knote, Scott Janz, Armin Wisthaler, Russell Long, James Szykman, Jinsoo Park, Youngjae Lee, Saewung Kim, Daun Jeong, Dianne Sanchez, Laurence Twigg, Grant Sumnicht, Travis Knepp, and Jason R. Schroeder
Atmos. Chem. Phys., 19, 5051–5067, https://doi.org/10.5194/acp-19-5051-2019, https://doi.org/10.5194/acp-19-5051-2019, 2019
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During the May–June 2016 International Cooperative Air Quality Field Study in Korea (KORUS-AQ), pollution reached the remote Taehwa Research Forest (TRF) site. Two case studies are examined and observations clearly identify TRF and the surrounding rural areas as long-term receptor sites for severe urban pollution events. In summary, domestic emissions may be causing more pollution than by transboundary pathways, which have been historically believed to be the major source of air pollution.
Ali Akherati, Christopher D. Cappa, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, Stephen M. Griffith, Sebastien Dusanter, Philip S. Stevens, and Shantanu H. Jathar
Atmos. Chem. Phys., 19, 4561–4594, https://doi.org/10.5194/acp-19-4561-2019, https://doi.org/10.5194/acp-19-4561-2019, 2019
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Unburned and partially burned organic compounds emitted from fossil fuel and biomass combustion can react in the atmosphere in the presence of sunlight to form particles. In this work, we use an air pollution model to examine the influence of these organic compounds released by motor vehicles and fires on fine particle pollution in southern California.
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.
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.
Alexander Zaytsev, Martin Breitenlechner, Abigail R. Koss, Christopher Y. Lim, James C. Rowe, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 1861–1870, https://doi.org/10.5194/amt-12-1861-2019, https://doi.org/10.5194/amt-12-1861-2019, 2019
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We present the development of a chemical ionization mass spectrometer which can be operated with either ammonium (NH4+) or hydronium (H3O+) as the reagent ion. We describe a mass spectrometric voltage scanning procedure based on collision-induced dissociation that allows us to determine the stability of detected ammonium–organic ions and hence constrain the sensitivity of the instrument to a wide range of organic compounds that cannot be calibrated directly.
Anna L. Hodshire, Pedro Campuzano-Jost, John K. Kodros, Betty Croft, Benjamin A. Nault, Jason C. Schroder, Jose L. Jimenez, and Jeffrey R. Pierce
Atmos. Chem. Phys., 19, 3137–3160, https://doi.org/10.5194/acp-19-3137-2019, https://doi.org/10.5194/acp-19-3137-2019, 2019
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A global chemical-transport model is used to determine the impact of methanesulfonic acid (MSA) on the aerosol size distribution and associated radiative effects, testing varying assumptions of MSA’s effective volatility and nucleating ability. We find that MSA mass best matches the ATom airborne measurements when volatility varies as a function of temperature, relative humidity, and available gas-phase bases, and the MSA radiative forcing is on the order of -50 mW m-2 over the Southern Ocean.
Jin Liao, Thomas F. Hanisco, Glenn M. Wolfe, Jason St. Clair, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Alan Fried, Eloise A. Marais, Gonzalo Gonzalez Abad, Kelly Chance, Hiren T. Jethva, Thomas B. Ryerson, Carsten Warneke, and Armin Wisthaler
Atmos. Chem. Phys., 19, 2765–2785, https://doi.org/10.5194/acp-19-2765-2019, https://doi.org/10.5194/acp-19-2765-2019, 2019
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Organic aerosol (OA) intimately links natural and anthropogenic emissions with air quality and climate. Direct OA measurements from space are currently not possible. This paper describes a new method to estimate OA by combining satellite HCHO and in situ OA and HCHO. The OA estimate is validated with the ground network. This new method has a potential for mapping observation-based global OA estimate.
Erik Ahlberg, Axel Eriksson, William H. Brune, Pontus Roldin, and Birgitta Svenningsson
Atmos. Chem. Phys., 19, 2701–2712, https://doi.org/10.5194/acp-19-2701-2019, https://doi.org/10.5194/acp-19-2701-2019, 2019
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The effects of wet or dry salt seed particle concentration (ammonium nitrate and ammonium sulphate) on secondary organic aerosol mass yields from a mixture of m-xylene and α-pinene were examined in an oxidation flow reactor. The experiments confirmed that increasing the condensation sink significantly increases the particle mass yields in oxidation flow reactors. Further, wet seed particles increased the particle mass yield by 60 % more than dry particles.
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.
Ru-Jin Huang, Yichen Wang, Junji Cao, Chunshui Lin, Jing Duan, Qi Chen, Yongjie Li, Yifang Gu, Jin Yan, Wei Xu, Roman Fröhlich, Francesco Canonaco, Carlo Bozzetti, Jurgita Ovadnevaite, Darius Ceburnis, Manjula R. Canagaratna, John Jayne, Douglas R. Worsnop, Imad El-Haddad, André S. H. Prévôt, and Colin D. O'Dowd
Atmos. Chem. Phys., 19, 2283–2298, https://doi.org/10.5194/acp-19-2283-2019, https://doi.org/10.5194/acp-19-2283-2019, 2019
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We found that in wintertime Shijiazhuang fine PM was mostly from primary emissions without sufficient atmospheric aging. In addition, secondary inorganic and organic aerosol dominated in pollution events under high-RH conditions, likely due to enhanced aqueous-phase chemistry, whereas primary organic aerosol dominated in pollution events under low-RH and stagnant conditions. Our results also highlighted the importance of meteorological conditions for PM pollution in this highly polluted city.
Shino Toma, Steve Bertman, Christopher Groff, Fulizi Xiong, Paul B. Shepson, Paul Romer, Kaitlin Duffey, Paul Wooldridge, Ronald Cohen, Karsten Baumann, Eric Edgerton, Abigail R. Koss, Joost de Gouw, Allen Goldstein, Weiwei Hu, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 1867–1880, https://doi.org/10.5194/acp-19-1867-2019, https://doi.org/10.5194/acp-19-1867-2019, 2019
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Acyl peroxy nitrates (APN) were measured near the ground in Alabama using GC in summer 2013 to study biosphere–atmosphere interactions. APN were lower than measured in the SE USA over the past 2 decades. Historical data showed APN in 2013 was limited by NOx and production was dominated by biogenic precursors more than in the past. Isoprene-derived MPAN correlated with isoprene hydroxynitrates as NOx-dependent products. MPAN varied with aerosol growth, but not with N-containing particles.
Nathan J. Janechek, Rachel F. Marek, Nathan Bryngelson, Ashish Singh, Robert L. Bullard, William H. Brune, and Charles O. Stanier
Atmos. Chem. Phys., 19, 1649–1664, https://doi.org/10.5194/acp-19-1649-2019, https://doi.org/10.5194/acp-19-1649-2019, 2019
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Cyclic volatile methyl siloxanes (cVMSs) are widely used chemicals in personal care products which can undergo oxidation to generate secondary organic aerosol. In this work, cVMS oxidation aerosols were generated using a photochemical chamber and the physical properties characterized. The aerosol yield, volatility, hygroscopicity, morphology, elemental composition, and proposed parameters for treatment as secondary organic aerosol in atmospheric models are provided.
Dagny A. Ullmann, Mallory L. Hinks, Adrian M. Maclean, Christopher L. Butenhoff, James W. Grayson, Kelley Barsanti, Jose L. Jimenez, Sergey A. Nizkorodov, Saeid Kamal, and Allan K. Bertram
Atmos. Chem. Phys., 19, 1491–1503, https://doi.org/10.5194/acp-19-1491-2019, https://doi.org/10.5194/acp-19-1491-2019, 2019
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We measured the viscosity and diffusion of organic molecules in secondary organic aerosol (SOA) generated from the ozonolysis of limonene. The results suggest that the mixing times of large organics in the SOA studied are short (< 1 h) for conditions found in the planetary boundary layer. The results also show that the Stokes–Einstein equation gives accurate predictions of diffusion coefficients of large organics within the studied SOA up to a viscosity of 102 to 104 Pa s.
Coty N. Jen, Lindsay E. Hatch, Vanessa Selimovic, Robert J. Yokelson, Robert Weber, Arantza E. Fernandez, Nathan M. Kreisberg, Kelley C. Barsanti, and Allen H. Goldstein
Atmos. Chem. Phys., 19, 1013–1026, https://doi.org/10.5194/acp-19-1013-2019, https://doi.org/10.5194/acp-19-1013-2019, 2019
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Wildfires in the western US are occurring more frequently and burning larger land areas. Smoke from these fires will play a greater role in regional air quality and atmospheric chemistry than in the past. To help fire and climate modelers and atmospheric experimentalists better understand how smoke impacts the environment, we have separated, identified, classified, and quantified the thousands of organic compounds found in smoke and related their amounts emitted to fire conditions.
Zhe Peng, Julia Lee-Taylor, John J. Orlando, Geoffrey S. Tyndall, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 813–834, https://doi.org/10.5194/acp-19-813-2019, https://doi.org/10.5194/acp-19-813-2019, 2019
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The use of oxidation flow reactors (OFRs) has been rapidly increasing. We investigate organic peroxy radical (RO2) chemistry in OFRs by kinetic modeling. It is found that, at low NO, UV intensity should be limited to avoid high radical levels leading to significant reaction of RO2 with OH and negligible RO2 isomerization, both of which are atmospherically irrelevant. We also develop two RO2 fate estimators (for general use and for OFRs) to aid experiment design and interpretation.
Juhi Nagori, Ruud H. H. Janssen, Juliane L. Fry, Maarten Krol, Jose L. Jimenez, Weiwei Hu, and Jordi Vilà-Guerau de Arellano
Atmos. Chem. Phys., 19, 701–729, https://doi.org/10.5194/acp-19-701-2019, https://doi.org/10.5194/acp-19-701-2019, 2019
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Secondary organic aerosol (SOA) is produced through a complex interaction of sunlight, volatile organic compounds emitted from trees, anthropogenic emissions, and atmospheric chemistry. We are able to successfully model the formation and diurnal evolution of SOA using a model that takes into consideration the surface and boundary layer dynamics (1–2 km from the surface) and photochemistry above the southeastern US with data collected during the SOAS campaign to constrain the model.
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.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Bruce Anderson, Andreas J. Beyersdorf, Donald R. Blake, William H. Brune, Yonghoon Choi, Chelsea A. Corr, Joost A. de Gouw, Jack Dibb, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, L. Gregory Huey, Michelle J. Kim, Christoph J. Knote, Kara D. Lamb, Taehyoung Lee, Taehyun Park, Sally E. Pusede, Eric Scheuer, Kenneth L. Thornhill, Jung-Hun Woo, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 17769–17800, https://doi.org/10.5194/acp-18-17769-2018, https://doi.org/10.5194/acp-18-17769-2018, 2018
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Aerosol impacts visibility and human health in large cities. Sources of aerosols are still highly uncertain, especially for cities surrounded by numerous other cities. We use observations collected during the Korea–United States Air Quality study to determine sources of organic aerosol (OA). We find that secondary OA (SOA) is rapidly produced over Seoul, South Korea, and that the sources of the SOA originate from short-lived hydrocarbons, which originate from local emissions.
Lindsay E. Hatch, Albert Rivas-Ubach, Coty N. Jen, Mary Lipton, Allen H. Goldstein, and Kelley C. Barsanti
Atmos. Chem. Phys., 18, 17801–17817, https://doi.org/10.5194/acp-18-17801-2018, https://doi.org/10.5194/acp-18-17801-2018, 2018
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We demonstrate the use of solid-phase extraction (SPE) disks for the untargeted analysis of gas-phase intermediate volatility and semi-volatile organic compounds emitted from biomass burning. SPE and Teflon filter samples collected from laboratory fires were analyzed by two-dimensional gas chromatography, with distinct differences in the observed chromatographic profiles as a function of
fuel type. Fuel-dependent emissions and volatility differences among benzenediol isomers were captured.
Barbara Ervens, Armin Sorooshian, Abdulmonam M. Aldhaif, Taylor Shingler, Ewan Crosbie, Luke Ziemba, Pedro Campuzano-Jost, Jose L. Jimenez, and Armin Wisthaler
Atmos. Chem. Phys., 18, 16099–16119, https://doi.org/10.5194/acp-18-16099-2018, https://doi.org/10.5194/acp-18-16099-2018, 2018
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The paper presents a new framework that can be used to identify emission scenarios in which aerosol populations are most likely modified by chemical processes in clouds. We show that in neither very polluted nor in very clean air masses is this the case. Only if the ratio of possible aerosol mass precursors (sulfur dioxide, some organics) and preexisting aerosol mass is sufficiently high will aerosol particles show substantially modified physicochemical properties upon cloud processing.
Kyle J. Zarzana, Vanessa Selimovic, Abigail R. Koss, Kanako Sekimoto, Matthew M. Coggon, Bin Yuan, William P. Dubé, Robert J. Yokelson, Carsten Warneke, Joost A. de Gouw, James M. Roberts, and Steven S. Brown
Atmos. Chem. Phys., 18, 15451–15470, https://doi.org/10.5194/acp-18-15451-2018, https://doi.org/10.5194/acp-18-15451-2018, 2018
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Emissions of glyoxal and methylglyoxal from fuels common to the western United States were measured using cavity-enhanced spectroscopy, which provides a more selective measurement of those compounds than was previously available. Primary emissions of glyoxal were lower than previously reported and showed variability between the different fuel groups. However, emissions of glyoxal relative to formaldehyde were constant across almost all the fuel groups at 6 %–7 %.
Christiane Schulz, Johannes Schneider, Bruna Amorim Holanda, Oliver Appel, Anja Costa, Suzane S. de Sá, Volker Dreiling, Daniel Fütterer, Tina Jurkat-Witschas, Thomas Klimach, Christoph Knote, Martina Krämer, Scot T. Martin, Stephan Mertes, Mira L. Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Bernadett Weinzierl, Helmut Ziereis, Martin Zöger, Meinrat O. Andreae, Paulo Artaxo, Luiz A. T. Machado, Ulrich Pöschl, Manfred Wendisch, and Stephan Borrmann
Atmos. Chem. Phys., 18, 14979–15001, https://doi.org/10.5194/acp-18-14979-2018, https://doi.org/10.5194/acp-18-14979-2018, 2018
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Aerosol chemical composition measurements in the tropical upper troposphere over the Amazon region show that 78 % of the aerosol in the upper troposphere consists of organic matter. Up to 20 % of the organic aerosol can be attributed to isoprene epoxydiol secondary organic aerosol (IEPOX-SOA). Furthermore, organic nitrates were identified, suggesting a connection to the IEPOX-SOA formation.
Yingjie Zhang, Wei Du, Yuying Wang, Qingqing Wang, Haofei Wang, Haitao Zheng, Fang Zhang, Hongrong Shi, Yuxuan Bian, Yongxiang Han, Pingqing Fu, Francesco Canonaco, André S. H. Prévôt, Tong Zhu, Pucai Wang, Zhanqing Li, and Yele Sun
Atmos. Chem. Phys., 18, 14637–14651, https://doi.org/10.5194/acp-18-14637-2018, https://doi.org/10.5194/acp-18-14637-2018, 2018
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We have a comprehensive characterization of aerosol chemistry and particle growth events at a downwind site of a highly polluted city in the North China Plain. Aerosol particles at the urban downwind site were highly aged and mainly from secondary formation. New particle growth events were also frequently observed on both clean and polluted days. While both sulfate and SOA played important roles in particle growth during clean periods, SOA was more important than sulfate during polluted events.
William H. Brune, Xinrong Ren, Li Zhang, Jingqiu Mao, David O. Miller, Bruce E. Anderson, Donald R. Blake, Ronald C. Cohen, Glenn S. Diskin, Samuel R. Hall, Thomas F. Hanisco, L. Gregory Huey, Benjamin A. Nault, Jeff Peischl, Ilana Pollack, Thomas B. Ryerson, Taylor Shingler, Armin Sorooshian, Kirk Ullmann, Armin Wisthaler, and Paul J. Wooldridge
Atmos. Chem. Phys., 18, 14493–14510, https://doi.org/10.5194/acp-18-14493-2018, https://doi.org/10.5194/acp-18-14493-2018, 2018
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Thunderstorms pull in polluted air from near the ground, transport it up through clouds containing lightning, and deposit it at altitudes where airplanes fly. The resulting chemical mixture in this air reacts to form ozone and particles, which affect climate. In this study, aircraft observations of the reactive gases responsible for this chemistry generally agree with modeled values, even in ice clouds. Thus, atmospheric oxidation chemistry appears to be mostly understood for this environment.
Daniela Wimmer, Stephany Buenrostro Mazon, Hanna Elina Manninen, Juha Kangasluoma, Alessandro Franchin, Tuomo Nieminen, John Backman, Jian Wang, Chongai Kuang, Radovan Krejci, Joel Brito, Fernando Goncalves Morais, Scot Turnbull Martin, Paulo Artaxo, Markku Kulmala, Veli-Matti Kerminen, and Tuukka Petäjä
Atmos. Chem. Phys., 18, 13245–13264, https://doi.org/10.5194/acp-18-13245-2018, https://doi.org/10.5194/acp-18-13245-2018, 2018
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This work focuses on understanding the production of very small airborne particles in the undisturbed environment of the Amazon basin. Computer models have shown that up to 70 % of these tiny particles are responsible for cloud formation on a global scale. The processes behind the production of these very small particles have been studied intensely recently. Their appearance has been observed almost all over the world. We directly measure sub-3 nm aerosols for the first time in the Amazon basin.
Georgios I. Gkatzelis, Thorsten Hohaus, Ralf Tillmann, Iulia Gensch, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Zhujun Yu, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 18, 12969–12989, https://doi.org/10.5194/acp-18-12969-2018, https://doi.org/10.5194/acp-18-12969-2018, 2018
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Defining the fundamental parameters that distribute organic molecules between the gas and particle phases is essential to understand their impact on the atmosphere. In this work, gas to particle partitioning of major biogenic oxidation products from monoterpenes and real plant emissions was investigated. While measurement results and theoretical calculation for most semi-volatile compounds are in good agreement, significant deviations are found for intermediate volatile organic compounds.
Jason A. Ducker, Christopher D. Holmes, Trevor F. Keenan, Silvano Fares, Allen H. Goldstein, Ivan Mammarella, J. William Munger, and Jordan Schnell
Biogeosciences, 15, 5395–5413, https://doi.org/10.5194/bg-15-5395-2018, https://doi.org/10.5194/bg-15-5395-2018, 2018
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We have developed an accurate method (SynFlux) to estimate ozone deposition and stomatal uptake across 103 flux tower sites (43 US, 60 Europe), where ozone concentrations and fluxes have not been measured. In all, the SynFlux public dataset provides monthly values of ozone dry deposition for 926 site years across a wide array of ecosystems. The SynFlux dataset will promote further applications to ecosystem, air quality, or climate modeling across the geoscience community.
Fernando Santos, Karla Longo, Alex Guenther, Saewung Kim, Dasa Gu, Dave Oram, Grant Forster, James Lee, James Hopkins, Joel Brito, and Saulo Freitas
Atmos. Chem. Phys., 18, 12715–12734, https://doi.org/10.5194/acp-18-12715-2018, https://doi.org/10.5194/acp-18-12715-2018, 2018
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We investigated the impact of biomass burning on the chemical composition of trace gases in the Amazon. The findings corroborate the influence of biomass burning activity not only on direct emissions of particulate matter but also on the oxidative capacity to produce secondary organic aerosol. The scientists plan to use this information to improve the numerical model simulation with a better representativeness of the chemical processes, which can impact on global climate prediction.
Anna L. Hodshire, Brett B. Palm, M. Lizabeth Alexander, Qijing Bian, Pedro Campuzano-Jost, Eben S. Cross, Douglas A. Day, Suzane S. de Sá, Alex B. Guenther, Armin Hansel, James F. Hunter, Werner Jud, Thomas Karl, Saewung Kim, Jesse H. Kroll, Jeong-Hoo Park, Zhe Peng, Roger Seco, James N. Smith, Jose L. Jimenez, and Jeffrey R. Pierce
Atmos. Chem. Phys., 18, 12433–12460, https://doi.org/10.5194/acp-18-12433-2018, https://doi.org/10.5194/acp-18-12433-2018, 2018
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We investigate the nucleation and growth processes that shape the aerosol size distribution inside oxidation flow reactors (OFRs) that sampled ambient air from Colorado and the Amazon rainforest. Results indicate that organics are important for both nucleation and growth, vapor uptake was limited to accumulation-mode particles, fragmentation reactions were important to limit particle growth at higher OH exposures, and an H2SO4-organics nucleation mechanism captured new particle formation well.
Zhaofeng Tan, Franz Rohrer, Keding Lu, Xuefei Ma, Birger Bohn, Sebastian Broch, Huabin Dong, Hendrik Fuchs, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, Xin Li, Ying Liu, Yuhan Liu, Anna Novelli, Min Shao, Haichao Wang, Yusheng Wu, Limin Zeng, Min Hu, Astrid Kiendler-Scharr, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 18, 12391–12411, https://doi.org/10.5194/acp-18-12391-2018, https://doi.org/10.5194/acp-18-12391-2018, 2018
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We present the first wintertime OH, HO2, and RO2 measurements in Beijing, China. OH concentrations are nearly 2-fold larger than those observed in foreign cities during wintertime. The high OH and large OH reactivities indicate photochemical processes can be effective even during wintertime. A box model largely underestimated HO2 and RO2 concentrations during pollution episodes correlated with high NOx, indicating a deficit current chemistry in the high NOx regime.
Hongyu Guo, Rene Otjes, Patrick Schlag, Astrid Kiendler-Scharr, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 12241–12256, https://doi.org/10.5194/acp-18-12241-2018, https://doi.org/10.5194/acp-18-12241-2018, 2018
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Reduction in ammonia has been proposed as a way to lower fine particle mass and improve air quality, but gas-phase ammonia is linked to agricultural productivity. We assess the feasibility of ammonia control at a variety of locations through an aerosol thermodynamic analysis. We show that aerosol response to ammonia control is highly nonlinear and only becomes effective when ambient particle pH drops below approximately 3. Particle pH is a relevant aerosol air quality parameter.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Joel Brito, Samara Carbone, Igor O. Ribeiro, Glauber G. Cirino, Yingjun Liu, Ryan Thalman, Arthur Sedlacek, Aaron Funk, Courtney Schumacher, John E. Shilling, Johannes Schneider, Paulo Artaxo, Allen H. Goldstein, Rodrigo A. F. Souza, Jian Wang, Karena A. McKinney, Henrique Barbosa, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 18, 12185–12206, https://doi.org/10.5194/acp-18-12185-2018, https://doi.org/10.5194/acp-18-12185-2018, 2018
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This study aimed at understanding and quantifying the changes in mass concentration and composition of submicron airborne particulate matter (PM) in Amazonia due to urban pollution. Downwind of Manaus, PM concentrations increased by up to 200 % under polluted compared with background conditions. The observed changes included contributions from both primary and secondary processes. The differences in organic PM composition suggested a shift in the pathways of secondary production with pollution.
Xiao-Feng Huang, Bei-Bing Zou, Ling-Yan He, Min Hu, André S. H. Prévôt, and Yuan-Hang Zhang
Atmos. Chem. Phys., 18, 11563–11580, https://doi.org/10.5194/acp-18-11563-2018, https://doi.org/10.5194/acp-18-11563-2018, 2018
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A novel multilinear engine (ME-2) model was applied to the PM2.5 dataset observed in the Pearl River Delta (PRD) of China in 2015 and identified the sources of secondary sulfate (21 %), vehicle emissions (14 %), industrial emissions (13 %), secondary nitrate (11 %), biomass burning (11 %), secondary organic aerosol (7 %), coal burning (6 %), fugitive dust (5 %), ship emissions (3 %) and aged sea salt (2 %). The central PRD area was clearly identified as the key emission area in the PRD.
Juliane L. Fry, Steven S. Brown, Ann M. Middlebrook, Peter M. Edwards, Pedro Campuzano-Jost, Douglas A. Day, José L. Jimenez, Hannah M. Allen, Thomas B. Ryerson, Ilana Pollack, Martin Graus, Carsten Warneke, Joost A. de Gouw, Charles A. Brock, Jessica Gilman, Brian M. Lerner, William P. Dubé, Jin Liao, and André Welti
Atmos. Chem. Phys., 18, 11663–11682, https://doi.org/10.5194/acp-18-11663-2018, https://doi.org/10.5194/acp-18-11663-2018, 2018
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This paper uses measurements made during research aircraft flights through power plant smokestack emissions plumes as a natural laboratory in the field experiment. We investigated a specific source of airborne particulate matter from the combination of human-produced NOx pollutant emissions (the smokestack plumes) with isoprene emitted by naturally by trees in the southeastern United States. These field-based yields appear to be higher than those typically measured in chamber studies.
Anna Novelli, Martin Kaminski, Michael Rolletter, Ismail-Hakki Acir, Birger Bohn, Hans-Peter Dorn, Xin Li, Anna Lutz, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Frank Holland, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 18, 11409–11422, https://doi.org/10.5194/acp-18-11409-2018, https://doi.org/10.5194/acp-18-11409-2018, 2018
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The impact of photooxidation of 2-methyl-3-butene-2-ol (MBO) on the concentration of radical species was studied in the atmospheric simulation chamber SAPHIR. MBO is a volatile organic compound mainly emitted by ponderosa and lodgepole pines which are very abundant in forests in the central-west USA. A very good agreement between measured and modelled radical concentrations and products from the oxidation of MBO was observed in an environment with NO of ~ 200 pptv.
Amelie Bertrand, Giulia Stefenelli, Simone M. Pieber, Emily A. Bruns, Brice Temime-Roussel, Jay G. Slowik, Henri Wortham, André S. H. Prévôt, Imad El Haddad, and Nicolas Marchand
Atmos. Chem. Phys., 18, 10915–10930, https://doi.org/10.5194/acp-18-10915-2018, https://doi.org/10.5194/acp-18-10915-2018, 2018
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We model the evolution of several BBOA markers including levoglucosan during aging experiments conducted in an atmospheric Teflon chamber, in order to evaluate the influence of vapor wall loss on the determination of the rate constants of the compounds with hydroxyl radicals (OH).
John E. Shilling, Mikhail S. Pekour, Edward C. Fortner, Paulo Artaxo, Suzane de Sá, John M. Hubbe, Karla M. Longo, Luiz A. T. Machado, Scot T. Martin, Stephen R. Springston, Jason Tomlinson, and Jian Wang
Atmos. Chem. Phys., 18, 10773–10797, https://doi.org/10.5194/acp-18-10773-2018, https://doi.org/10.5194/acp-18-10773-2018, 2018
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We report aircraft observations of the evolution of organic aerosol in the Manaus urban plume as it ages. We observe dynamic changes in the organic aerosol. The mean carbon oxidation state of the OA increases from −0.6 to −0.45. Hydrocarbon-like organic aerosol (HOA) mass is lost and is balanced out by formation of oxygenated organic aerosol (OOA). Because HOA loss is balanced by OOA formation, we observe little change in the net Δorg / ΔCO values with aging.
Eleni Karnezi, Benjamin N. Murphy, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Florian Rubach, Astrid Kiendler-Scharr, Thomas F. Mentel, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 10759–10772, https://doi.org/10.5194/acp-18-10759-2018, https://doi.org/10.5194/acp-18-10759-2018, 2018
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Different parameterizations of the organic aerosol (OA) formation and evolution are evaluated using ground and airborne measurements collected in the 2012 PEGASOS field campaign in the Po Valley (Italy). Total OA concentration and O : C ratios were reproduced within experimental error by a number of schemes. Anthropogenic secondary OA (SOA) contributed 15–25 % of the total OA, 20–35 % of SOA from intermediate volatility compounds oxidation, and 15–45 % of biogenic SOA depending on the scheme.
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
Lindsay D. Yee, Gabriel Isaacman-VanWertz, Rebecca A. Wernis, Meng Meng, Ventura Rivera, Nathan M. Kreisberg, Susanne V. Hering, Mads S. Bering, Marianne Glasius, Mary Alice Upshur, Ariana Gray Bé, Regan J. Thomson, Franz M. Geiger, John H. Offenberg, Michael Lewandowski, Ivan Kourtchev, Markus Kalberer, Suzane de Sá, Scot T. Martin, M. Lizabeth Alexander, Brett B. Palm, Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Jose L. Jimenez, Yingjun Liu, Karena A. McKinney, Paulo Artaxo, Juarez Viegas, Antonio Manzi, Maria B. Oliveira, Rodrigo de Souza, Luiz A. T. Machado, Karla Longo, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 10433–10457, https://doi.org/10.5194/acp-18-10433-2018, https://doi.org/10.5194/acp-18-10433-2018, 2018
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Biogenic volatile organic compounds react in the atmosphere to form secondary organic aerosol, yet the chemical pathways remain unclear. We collected filter samples and deployed a semi-volatile thermal desorption aerosol gas chromatograph in the central Amazon. We measured 30 sesquiterpenes and 4 diterpenes and find them to be important for reactive ozone loss. We estimate that sesquiterpene oxidation contributes at least 0.4–5 % (median 1 %) of observed submicron organic aerosol mass.
Mira L. Pöhlker, Florian Ditas, Jorge Saturno, Thomas Klimach, Isabella Hrabě de Angelis, Alessandro C. Araùjo, Joel Brito, Samara Carbone, Yafang Cheng, Xuguang Chi, Reiner Ditz, Sachin S. Gunthe, Bruna A. Holanda, Konrad Kandler, Jürgen Kesselmeier, Tobias Könemann, Ovid O. Krüger, Jošt V. Lavrič, Scot T. Martin, Eugene Mikhailov, Daniel Moran-Zuloaga, Luciana V. Rizzo, Diana Rose, Hang Su, Ryan Thalman, David Walter, Jian Wang, Stefan Wolff, Henrique M. J. Barbosa, Paulo Artaxo, Meinrat O. Andreae, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Chem. Phys., 18, 10289–10331, https://doi.org/10.5194/acp-18-10289-2018, https://doi.org/10.5194/acp-18-10289-2018, 2018
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This paper presents the aerosol and cloud condensation nuclei (CCN) variability for characteristic atmospheric states – such as biomass burning, long-range transport, and pristine rain forest conditions – in the vulnerable and climate-relevant Amazon Basin. It summarizes the key properties of aerosol and CCN and, thus, provides a basis for an in-depth analysis of aerosol–cloud interactions in the Amazon region.
Daniel Moran-Zuloaga, Florian Ditas, David Walter, Jorge Saturno, Joel Brito, Samara Carbone, Xuguang Chi, Isabella Hrabě de Angelis, Holger Baars, Ricardo H. M. Godoi, Birgit Heese, Bruna A. Holanda, Jošt V. Lavrič, Scot T. Martin, Jing Ming, Mira L. Pöhlker, Nina Ruckteschler, Hang Su, Yaqiang Wang, Qiaoqiao Wang, Zhibin Wang, Bettina Weber, Stefan Wolff, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Chem. Phys., 18, 10055–10088, https://doi.org/10.5194/acp-18-10055-2018, https://doi.org/10.5194/acp-18-10055-2018, 2018
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This study presents multiple years of aerosol coarse mode observations at the remote ATTO site in the Amazon Basin. The results are discussed in light of the frequent and episodic long-range transport of Saharan dust plumes in the early wet season as well as the persistent background bioaerosol cycling in the rain forest ecosystem. This work provides a solid basis for future studies on the dynamic coarse mode aerosol cycling and its biogeochemical relevance in the Amazon.
Simone M. Pieber, Nivedita K. Kumar, Felix Klein, Pierre Comte, Deepika Bhattu, Josef Dommen, Emily A. Bruns, Doǧuşhan Kılıç, Imad El Haddad, Alejandro Keller, Jan Czerwinski, Norbert Heeb, Urs Baltensperger, Jay G. Slowik, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 9929–9954, https://doi.org/10.5194/acp-18-9929-2018, https://doi.org/10.5194/acp-18-9929-2018, 2018
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We studied primary emissions and secondary organic aerosol (SOA) from gasoline direct injection (GDI) vehicles including GDIs retrofitted with gasoline particle filters (GPF). GPF retrofitting significantly decreased the primary particulate matter, particularly through removal of refractory black carbon and, to a lesser extent, of non-refractory organic particulates. SOA experiments were conducted in a batch and flow reactor. GPF retrofitting did not significantly affect precursors or yields.
Emmanouil Oikonomakis, Sebnem Aksoyoglu, Martin Wild, Giancarlo Ciarelli, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Chem. Phys., 18, 9741–9765, https://doi.org/10.5194/acp-18-9741-2018, https://doi.org/10.5194/acp-18-9741-2018, 2018
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We report a model sensitivity study on the impact of aerosol–radiation interaction (ARI) changes in Europe between 1990 and 2010 on summer surface ozone via effects on photolysis rates and biogenic emissions. The overall impact of ARI changes on ozone was relatively small when compared to the total ozone concentrations, but it was more important when compared to the order of magnitude of ozone trends, indicating a potential partial damping of the effects of ozone precursor emissions' reduction.
Kanako Sekimoto, Abigail R. Koss, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Carsten Warneke, Robert J. Yokelson, James M. Roberts, and Joost de Gouw
Atmos. Chem. Phys., 18, 9263–9281, https://doi.org/10.5194/acp-18-9263-2018, https://doi.org/10.5194/acp-18-9263-2018, 2018
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We found that on average 85 % of the VOC emissions from biomass burning across various fuels representative of the western US (including various coniferous and chaparral fuels) can be explained using only two emission profiles: (i) a high-temperature pyrolysis profile and (ii) a low-temperature pyrolysis profile. The high-temperature profile is quantitatively similar between different fuel types (r2 > 0.84), and likewise for the low-temperature profile.
Eliane G. Alves, Julio Tóta, Andrew Turnipseed, Alex B. Guenther, José Oscar W. Vega Bustillos, Raoni A. Santana, Glauber G. Cirino, Julia V. Tavares, Aline P. Lopes, Bruce W. Nelson, Rodrigo A. de Souza, Dasa Gu, Trissevgeni Stavrakou, David K. Adams, Jin Wu, Scott Saleska, and Antonio O. Manzi
Biogeosciences, 15, 4019–4032, https://doi.org/10.5194/bg-15-4019-2018, https://doi.org/10.5194/bg-15-4019-2018, 2018
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This study shows that leaf quantity and leaf age have an important effect on seasonal changes in isoprene emissions and that these could play an even more important role in regulating ecosystem isoprene fluxes than light and temperature at seasonal timescales in tropical forests. These results bring novelty and new insight for future research because in the past leaf phenology was not considered as an important factor that controls biological processes in the tropics.
Chunxiang Ye, Xianliang Zhou, Dennis Pu, Jochen Stutz, James Festa, Max Spolaor, Catalina Tsai, Christopher Cantrell, Roy L. Mauldin III, Andrew Weinheimer, Rebecca S. Hornbrook, Eric C. Apel, Alex Guenther, Lisa Kaser, Bin Yuan, Thomas Karl, Julie Haggerty, Samuel Hall, Kirk Ullmann, James Smith, and John Ortega
Atmos. Chem. Phys., 18, 9107–9120, https://doi.org/10.5194/acp-18-9107-2018, https://doi.org/10.5194/acp-18-9107-2018, 2018
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Substantial levels of HONO existed during the day throughout the troposphere over the southeastern US during NOMADSS 2013. Particulate nitrate photolysis appeared to be the major volume HONO source, while NOx was an important HONO precursor only in industrial and urban plumes. HONO was not a significant OH radical precursor in the rural troposphere away from the ground surface; however, its production from particulate nitrate photolysis was an important renoxification pathway.
Maite Bauwens, Trissevgeni Stavrakou, Jean-François Müller, Bert Van Schaeybroeck, Lesley De Cruz, Rozemien De Troch, Olivier Giot, Rafiq Hamdi, Piet Termonia, Quentin Laffineur, Crist Amelynck, Niels Schoon, Bernard Heinesch, Thomas Holst, Almut Arneth, Reinhart Ceulemans, Arturo Sanchez-Lorenzo, and Alex Guenther
Biogeosciences, 15, 3673–3690, https://doi.org/10.5194/bg-15-3673-2018, https://doi.org/10.5194/bg-15-3673-2018, 2018
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Biogenic isoprene fluxes are simulated over Europe with the MEGAN–MOHYCAN model for the recent past and end-of-century climate at high spatiotemporal resolution (0.1°, 3 min). Due to climate change, fluxes increased by 40 % over 1979–2014. Climate scenarios for 2070–2099 suggest an increase by 83 % due to climate, and an even stronger increase when the potential impact of CO2 fertilization is considered (up to 141 %). Accounting for CO2 inhibition cancels out a large part of these increases.
Yele Sun, Weiqi Xu, Qi Zhang, Qi Jiang, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Jie Li, John Jayne, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 18, 8469–8489, https://doi.org/10.5194/acp-18-8469-2018, https://doi.org/10.5194/acp-18-8469-2018, 2018
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We present a 2–year analysis of organic aerosol (OA) from highly time–resolved measurements by an aerosol chemical speciation monitor in the megacity of Beijing. The sources of OA were analyzed with the advanced factor analysis of a multilinear engine (ME-2). Our results showed very different seasonal patterns, relative humidity and temperature dependence, and sources regions among different OA factors. The sources and processes of OA factors, and their roles in haze pollution are elucidated.
Hendrik Fuchs, Sascha Albrecht, Ismail–Hakki Acir, Birger Bohn, Martin Breitenlechner, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, Martin Kaminski, Frank N. Keutsch, Anna Novelli, David Reimer, Franz Rohrer, Ralf Tillmann, Luc Vereecken, Robert Wegener, Alexander Zaytsev, Astrid Kiendler-Scharr, and Andreas Wahner
Atmos. Chem. Phys., 18, 8001–8016, https://doi.org/10.5194/acp-18-8001-2018, https://doi.org/10.5194/acp-18-8001-2018, 2018
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The photooxidation of methyl vinyl ketone MVK, one of the most important products of isoprene that is emitted by plants, was investigated in the atmospheric simulation chamber SAPHIR for conditions found in forested areas. The comparison of measured trace gas time series with model calculations shows a gap in the understanding of radical chemistry in the MVK oxidation scheme. The possibility of unimolecular isomerization reactions were investigated by means of quantum-chemical calculations.
Si-Wan Kim, Vijay Natraj, Seoyoung Lee, Hyeong-Ahn Kwon, Rokjin Park, Joost de Gouw, Gregory Frost, Jhoon Kim, Jochen Stutz, Michael Trainer, Catalina Tsai, and Carsten Warneke
Atmos. Chem. Phys., 18, 7639–7655, https://doi.org/10.5194/acp-18-7639-2018, https://doi.org/10.5194/acp-18-7639-2018, 2018
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Formaldehyde (HCHO) is a hazardous air pollutant and is associated with tropospheric ozone production. HCHO has been monitored from space. In this study, to acquire high-quality satellite-based HCHO observations, we utilize fine-resolution atmospheric chemistry model results as an input to the computer code for satellite retrievals over the Los Angeles Basin. Our study indicates that the use of fine-resolution profile shapes helps to identify HCHO plumes from space.
Amelie Bertrand, Giulia Stefenelli, Coty N. Jen, Simone M. Pieber, Emily A. Bruns, Haiyan Ni, Brice Temime-Roussel, Jay G. Slowik, Allen H. Goldstein, Imad El Haddad, Urs Baltensperger, André S. H. Prévôt, Henri Wortham, and Nicolas Marchand
Atmos. Chem. Phys., 18, 7607–7624, https://doi.org/10.5194/acp-18-7607-2018, https://doi.org/10.5194/acp-18-7607-2018, 2018
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A thermal desorption aerosol gas chromatograph coupled to an aerosol mass spectrometer (TAG–AMS) is connected to an atmospheric chamber. The setup serves the quantitative study of the impact of combustion conditions and atmospheric aging on the chemical fingerprint at the molecular level of biomass burning organic aerosol.
Nan Li, Qingyang He, Jim Greenberg, Alex Guenther, Jingyi Li, Junji Cao, Jun Wang, Hong Liao, Qiyuan Wang, and Qiang Zhang
Atmos. Chem. Phys., 18, 7489–7507, https://doi.org/10.5194/acp-18-7489-2018, https://doi.org/10.5194/acp-18-7489-2018, 2018
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O3 pollution has been increasing in most Chinese cities in recent years. Our study reveals that the synergistic impact of individual source contributions to O3 formation should be considered in the formation of air pollution control strategies, especially for big cities in the vicinity of forests.
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.
Arineh Cholakian, Matthias Beekmann, Augustin Colette, Isabelle Coll, Guillaume Siour, Jean Sciare, Nicolas Marchand, Florian Couvidat, Jorge Pey, Valerie Gros, Stéphane Sauvage, Vincent Michoud, Karine Sellegri, Aurélie Colomb, Karine Sartelet, Helen Langley DeWitt, Miriam Elser, André S. H. Prévot, Sonke Szidat, and François Dulac
Atmos. Chem. Phys., 18, 7287–7312, https://doi.org/10.5194/acp-18-7287-2018, https://doi.org/10.5194/acp-18-7287-2018, 2018
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In this work, four schemes for the simulation of organic aerosols in the western Mediterranean basin are added to the CHIMERE chemistry–transport model; the resulting simulations are then compared to measurements obtained from ChArMEx. It is concluded that the scheme taking into account the fragmentation and the formation of nonvolatile organic aerosols corresponds better to measurements; the major source of this aerosol in the western Mediterranean is found to be of biogenic origin.
Mingjin Wang, Tong Zhu, Defeng Zhao, Florian Rubach, Andreas Wahner, Astrid Kiendler-Scharr, and Thomas F. Mentel
Atmos. Chem. Phys., 18, 7345–7359, https://doi.org/10.5194/acp-18-7345-2018, https://doi.org/10.5194/acp-18-7345-2018, 2018
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Organic coatings modify hygroscopicity and CCN activation of mineral dust perticles. Small amounts of oleic acid coating (volume fraction (vf) ≤ 4.1 %) decreased the CCN activity of CaCO3 particles, while more oleic acid coating (vf ≥ 14.8 %) increased the CCN activity of CaCO3 particles, while malonic acid coating (vf = 0.4−42 %) even in smallest amounts increased the CCN activity of CaCO3 particles. Our laboratory results should also hold under conditions of the atmosphere.
Jun Zhou, Peter Zotter, Emily A. Bruns, Giulia Stefenelli, Deepika Bhattu, Samuel Brown, Amelie Bertrand, Nicolas Marchand, Houssni Lamkaddam, Jay G. Slowik, André S. H. Prévôt, Urs Baltensperger, Thomas Nussbaumer, Imad El-Haddad, and Josef Dommen
Atmos. Chem. Phys., 18, 6985–7000, https://doi.org/10.5194/acp-18-6985-2018, https://doi.org/10.5194/acp-18-6985-2018, 2018
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We thoroughly studied the reactive oxygen species (ROS) generation potential of particulate wood combustion emissions, from different combustion technologies, fuel types, operation methods, combustion regimes and phases. ROS from automatically operated combustion devices under optimal conditions were much lower than those from manually operated appliances. We examined the impact of atmospheric aging on ROS content in SOA and determined the controlling parameters, by using an online ROS analyzer.
Eunha Kang, Meehye Lee, William H. Brune, Taehyoung Lee, Taehyun Park, Joonyoung Ahn, and Xiaona Shang
Atmos. Chem. Phys., 18, 6661–6677, https://doi.org/10.5194/acp-18-6661-2018, https://doi.org/10.5194/acp-18-6661-2018, 2018
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A potential aerosol mass (PAM) reactor expedites slow atmospheric oxidation reactions and enables the observation of chemical aging processes and the determination of the aerosol-forming power of an air mass. A PAM reactor was deployed at Baengnyeong Island in the Yellow Sea. Experimental results confirm the key role of SO2 in generating secondary aerosols in northeast Asia, and the contribution of organics to secondary aerosols is more variable during transport in the atmosphere.
Luiz A. T. Machado, Alan J. P. Calheiros, Thiago Biscaro, Scott Giangrande, Maria A. F. Silva Dias, Micael A. Cecchini, Rachel Albrecht, Meinrat O. Andreae, Wagner F. Araujo, Paulo Artaxo, Stephan Borrmann, Ramon Braga, Casey Burleyson, Cristiano W. Eichholz, Jiwen Fan, Zhe Feng, Gilberto F. Fisch, Michael P. Jensen, Scot T. Martin, Ulrich Pöschl, Christopher Pöhlker, Mira L. Pöhlker, Jean-François Ribaud, Daniel Rosenfeld, Jaci M. B. Saraiva, Courtney Schumacher, Ryan Thalman, David Walter, and Manfred Wendisch
Atmos. Chem. Phys., 18, 6461–6482, https://doi.org/10.5194/acp-18-6461-2018, https://doi.org/10.5194/acp-18-6461-2018, 2018
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This overview discuss the main precipitation processes and their sensitivities to environmental conditions in the Central Amazon Basin. It presents a review of the knowledge acquired about cloud processes and rainfall formation in Amazonas. In addition, this study provides a characterization of the seasonal variation and rainfall sensitivities to topography, surface cover, and aerosol concentration. Airplane measurements were evaluated to characterize and contrast cloud microphysical properties.
Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Benjamin Chazeau, Gary A. Salazar, Soenke Szidat, Jean-Luc Jaffrezo, Christoph Hueglin, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 6187–6206, https://doi.org/10.5194/acp-18-6187-2018, https://doi.org/10.5194/acp-18-6187-2018, 2018
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Carbonaceous aerosols are related to adverse human health effects, which depend on the aerosol chemical composition and size. Here, we combine aerosol mass spectrometry and radiocarbon measurements of size-resolved samples collected over a long term to identify the origins of primary and secondary carbonaceous aerosols in the fine and coarse modes.
Adan S. S. Medeiros, Igor O. Ribeiro, Marcos V. B. Morais, Rita V. Andreoli, Jorge A. Martins, Leila D. Martins, Carla E. Batista, Patrícia C. Guimarães, Scot T. Martin, and Rodrigo A. F. Souza
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-347, https://doi.org/10.5194/acp-2018-347, 2018
Revised manuscript not accepted
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The study evaluates the river breezes influence on pollutant plume dispersion or canalization in central amazon, using atmospheric chemistry modelling. Manaus, a 2 million people city, is considered herein for be a major city surrounded by pristine forest and large rivers. The main conclusion is that Manaus pollution plume dispersion could at times be partially canalized leading to significant changes of surface river concentration, even most of Manaus plume following prevailing trade winds.
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.
Wei Zhou, Qingqing Wang, Xiujuan Zhao, Weiqi Xu, Chen Chen, Wei Du, Jian Zhao, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 18, 3951–3968, https://doi.org/10.5194/acp-18-3951-2018, https://doi.org/10.5194/acp-18-3951-2018, 2018
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We present a 3-month analysis of submicron aerosols that were measured at 260 m on a meteorological tower in Beijing, China. The sources of organic aerosol (OA) were analyzed by using a multi-linear engine (ME-2). Our results showed significant changes in both primary and secondary OA composition from the non-heating season to the heating season. We also observed a considerable contribution (10–13%) of cooking OA at 260 m and very different OA composition between ground level and 260 m.
Georgios I. Gkatzelis, Ralf Tillmann, Thorsten Hohaus, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Meas. Tech., 11, 1481–1500, https://doi.org/10.5194/amt-11-1481-2018, https://doi.org/10.5194/amt-11-1481-2018, 2018
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This manuscript presents an intercomparison of state-of-the-art online and in situ particle sampling techniques connected to proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS). Collection and vaporization of aerosol combined with soft ionization mass spectrometry offers the advantage of detailed chemical characterization of SOA species. The benefits of these techniques are highlighted through their consistency in providing the chemical composition of biogenic SOA.
Abigail R. Koss, Kanako Sekimoto, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Jose L. Jimenez, Jordan Krechmer, James M. Roberts, Carsten Warneke, Robert J. Yokelson, and Joost de Gouw
Atmos. Chem. Phys., 18, 3299–3319, https://doi.org/10.5194/acp-18-3299-2018, https://doi.org/10.5194/acp-18-3299-2018, 2018
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Non-methane organic gases (NMOGs) were detected by proton-transfer-reaction mass spectrometry (PTR-ToF) during an extensive laboratory characterization of wildfire emissions. Identifications for PTR-ToF ion masses are proposed and supported by a combination of techniques. Overall excellent agreement with other instrumentation is shown. Scalable emission factors and ratios are reported for many newly reported reactive species. An analysis of chemical characteristics is presented.
Vanessa Selimovic, Robert J. Yokelson, Carsten Warneke, James M. Roberts, Joost de Gouw, James Reardon, and David W. T. Griffith
Atmos. Chem. Phys., 18, 2929–2948, https://doi.org/10.5194/acp-18-2929-2018, https://doi.org/10.5194/acp-18-2929-2018, 2018
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We burned fuels representing western US wildfires in large-scale laboratory simulations to generate relevant emissions as confirmed by lab–field comparison. We report emission factors (EFs) for light scattering and absorption and BC along with SSA at 870 and 401 nm and AAE. We report EF for 22 trace gases that are major inorganic and organic emissions from flaming and smoldering. We report trace gas EF for species rarely (NH3) or not yet measured (e.g., HONO, acetic acid) for real US wildfires.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Qiao Zhu, Xiao-Feng Huang, Li-Ming Cao, Lin-Tong Wei, Bin Zhang, Ling-Yan He, Miriam Elser, Francesco Canonaco, Jay G. Slowik, Carlo Bozzetti, Imad El-Haddad, and André S. H. Prévôt
Atmos. Meas. Tech., 11, 1049–1060, https://doi.org/10.5194/amt-11-1049-2018, https://doi.org/10.5194/amt-11-1049-2018, 2018
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Organic aerosol constitutes one of the major components of atmospheric particulate matter globally and is emitted from various sources. Therefore, identifying and quantifying the sources of organic aerosol accurately is a key task in the field. In this study, we applied a rather novel procedure for an improved source apportionment method (ME-2) to resolve the
less meaningful or mixed factorsproblems for organic aerosol using the traditional method (PMF).
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Eric Edgerton, Karsten Baumann, Philip A. Feiner, David O. Miller, William H. Brune, Abigail R. Koss, Joost A. de Gouw, Pawel K. Misztal, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 2601–2614, https://doi.org/10.5194/acp-18-2601-2018, https://doi.org/10.5194/acp-18-2601-2018, 2018
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Observations of increased ozone on hotter days are widely reported, but the mechanisms driving this relationship remain uncertain. We use measurements from the rural southeastern United States to study how temperature affects ozone production. We find that changing NOx emissions, most likely from soil microbes, can be a major driver of increased ozone with temperature in the continental background. These findings suggest that ozone will increase with temperature under a wide range of conditions.
Kenneth E. Christian, William H. Brune, Jingqiu Mao, and Xinrong Ren
Atmos. Chem. Phys., 18, 2443–2460, https://doi.org/10.5194/acp-18-2443-2018, https://doi.org/10.5194/acp-18-2443-2018, 2018
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We applied a global sensitivity analysis to the GEOS-Chem chemical transport model analyzing some well-studied tropospheric oxidants for a time period corresponding to an aircraft field campaign. We find modeled results generally agree with measurements when uncertainties in both the model and measurements are taken into account. While model results were largely sensitive to emissions, chemical reaction rates also represented a large source of uncertainty.
Claire F. Fortenberry, Michael J. Walker, Yaping Zhang, Dhruv Mitroo, William H. Brune, and Brent J. Williams
Atmos. Chem. Phys., 18, 2199–2224, https://doi.org/10.5194/acp-18-2199-2018, https://doi.org/10.5194/acp-18-2199-2018, 2018
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In these laboratory studies, two types of biomass burning organic aerosol (BBOA) were generated in a combustion chamber and treated in a flow reactor to mimic atmospheric oxidation. Complementary bulk and molecular chemical measurements show that while many species deplete with oxidation, oxidized BBOA markers are enhanced. The results provide insight into the complex chemical evolution of BBOA over nearly 10 days of atmospheric photochemistry, informing future laboratory and field studies.
Kaspar R. Daellenbach, Imad El-Haddad, Lassi Karvonen, Athanasia Vlachou, Joel C. Corbin, Jay G. Slowik, Maarten F. Heringa, Emily A. Bruns, Samuel M. Luedin, Jean-Luc Jaffrezo, Sönke Szidat, Andrea Piazzalunga, Raquel Gonzalez, Paola Fermo, Valentin Pflueger, Guido Vogel, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 2155–2174, https://doi.org/10.5194/acp-18-2155-2018, https://doi.org/10.5194/acp-18-2155-2018, 2018
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A novel offline LDI-MS method was developed to analyse particulate matter (PM) collected at multiple sites in central Europe during the entire year of 2013. PM sources were identified by positive matrix factorization. Wood burning emissions were separated according to the burning conditions; inefficient burns had a larger impact on air quality in southern Alpine valleys than in northern Switzerland. Moreover, primary tailpipe exhaust was distinguished from aged/secondary traffic emissions.
Emmanouil Oikonomakis, Sebnem Aksoyoglu, Giancarlo Ciarelli, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Chem. Phys., 18, 2175–2198, https://doi.org/10.5194/acp-18-2175-2018, https://doi.org/10.5194/acp-18-2175-2018, 2018
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We report a modeling study investigating the uncertainties in ozone production in Europe. Using various methods for different emission and meteorological scenarios, we searched for the possible reasons for underestimation of high ozone levels in Europe by models. Our results suggest that emissions, especially NOx, might be too low in the European inventories. Improvement of the modeled ozone production will contribute to more consistent and effective ozone mitigation strategies for the future.
Catalina Tsai, Max Spolaor, Santo Fedele Colosimo, Olga Pikelnaya, Ross Cheung, Eric Williams, Jessica B. Gilman, Brian M. Lerner, Robert J. Zamora, Carsten Warneke, James M. Roberts, Ravan Ahmadov, Joost de Gouw, Timothy Bates, Patricia K. Quinn, and Jochen Stutz
Atmos. Chem. Phys., 18, 1977–1996, https://doi.org/10.5194/acp-18-1977-2018, https://doi.org/10.5194/acp-18-1977-2018, 2018
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Nitrous acid (HONO) photolysis is an important source of hydroxyl radicals (OH). Vertical HONO fluxes, observed in the snow-free, wintertime Uintah Basin, Utah, USA, show that chemical formation of HONO on the ground closes the HONO budget. Under high NOx conditions, HONO formation is most likely due to photo-enhanced conversion of NO2 on the ground. Under moderate to low NO2 conditions, photolysis of HNO3 on the ground seems to be the most likely source of HONO.
Defeng Zhao, Sebastian H. Schmitt, Mingjin Wang, Ismail-Hakki Acir, Ralf Tillmann, Zhaofeng Tan, Anna Novelli, Hendrik Fuchs, Iida Pullinen, Robert Wegener, Franz Rohrer, Jürgen Wildt, Astrid Kiendler-Scharr, Andreas Wahner, and Thomas F. Mentel
Atmos. Chem. Phys., 18, 1611–1628, https://doi.org/10.5194/acp-18-1611-2018, https://doi.org/10.5194/acp-18-1611-2018, 2018
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Air pollutants emitted by human activities such as NOx and SO2 can influence the abundance of secondary organic aerosol (SOA) from biogenic volatile organic compounds (VOCs). We found that NOx suppressed new particle formation and SOA mass formation. When both SO2 and NOx are present, the suppressing effect of NOx on SOA mass formation was counteracted by SO2. High NOx changed SOA chemical composition, forming more organic nitrate, because NOx changed radical chemistry during VOC oxidation.
Xuan Wang, Colette L. Heald, Jiumeng Liu, Rodney J. Weber, Pedro Campuzano-Jost, Jose L. Jimenez, Joshua P. Schwarz, and Anne E. Perring
Atmos. Chem. Phys., 18, 635–653, https://doi.org/10.5194/acp-18-635-2018, https://doi.org/10.5194/acp-18-635-2018, 2018
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Brown carbon (BrC) contributes significantly to uncertainty in estimating the global direct radiative effect (DRE) of aerosols. We develop a global model simulation of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental United States. We suggest that BrC DRE has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.
Brett B. Palm, Suzane S. de Sá, Douglas A. Day, Pedro Campuzano-Jost, Weiwei Hu, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Joel Brito, Florian Wurm, Paulo Artaxo, Ryan Thalman, Jian Wang, Lindsay D. Yee, Rebecca Wernis, Gabriel Isaacman-VanWertz, Allen H. Goldstein, Yingjun Liu, Stephen R. Springston, Rodrigo Souza, Matt K. Newburn, M. Lizabeth Alexander, Scot T. Martin, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 467–493, https://doi.org/10.5194/acp-18-467-2018, https://doi.org/10.5194/acp-18-467-2018, 2018
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Ambient air was oxidized by OH or O3 in an oxidation flow reactor during both wet and dry seasons in the GoAmazon2014/5 campaign to study secondary organic aerosol (SOA) formation. We investigated how much biogenic, urban, and biomass burning sources contributed to the ambient concentrations of SOA precursor gases and how their contributions changed diurnally and seasonally. SOA yields and hygroscopicity of organic aerosol in the oxidation flow reactor were also studied.
Havala O. T. Pye, Andreas Zuend, Juliane L. Fry, Gabriel Isaacman-VanWertz, Shannon L. Capps, K. Wyat Appel, Hosein Foroutan, Lu Xu, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 357–370, https://doi.org/10.5194/acp-18-357-2018, <