Articles | Volume 21, issue 24
https://doi.org/10.5194/acp-21-18247-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-18247-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
16 Dec 2021
Research article |
| 16 Dec 2021
| 16 Dec 2021
Modeling secondary organic aerosol formation from volatile chemical products
Elyse A. Pennington
Oak Ridge Institute for Science and Education, Office of Research and Development, US Environmental Protection Agency, Research
Triangle Park, NC 27711, USA
Division of Chemistry and Chemical Engineering, California Institute of
Technology, Pasadena, CA 91125, USA
Karl M. Seltzer
Oak Ridge Institute for Science and Education, Office of Research and Development, US Environmental Protection Agency, Research
Triangle Park, NC 27711, USA
Benjamin N. Murphy
Office of Research and Development, US Environmental Protection
Agency, Research Triangle Park, NC 27711, USA
Momei Qin
Oak Ridge Institute for Science and Education, Office of Research and Development, US Environmental Protection Agency, Research
Triangle Park, NC 27711, USA
Jiangsu Key Laboratory of Atmospheric Environment Monitoring and
Pollution Control, Collaborative Innovation Center of Atmospheric
Environment and Equipment Technology, School of Environmental Science and
Engineering, Nanjing University of Information Science & Technology,
Nanjing, China
John H. Seinfeld
Division of Chemistry and Chemical Engineering, California Institute of
Technology, Pasadena, CA 91125, USA
Office of Research and Development, US Environmental Protection
Agency, Research Triangle Park, NC 27711, USA
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Hejun Hu, Haichao Wang, Keding Lu, Jie Wang, Zelong Zheng, Xuezhen Xu, Tianyu Zhai, Xiaorui Chen, Xiao Lu, Wenxing Fu, Xin Li, Limin Zeng, Min Hu, Yuanhang Zhang, and Shaojia Fan
Atmos. Chem. Phys., 23, 8211–8223, https://doi.org/10.5194/acp-23-8211-2023, https://doi.org/10.5194/acp-23-8211-2023, 2023
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Nitrate radical chemistry is critical to the degradation of volatile organic compounds (VOCs) and secondary organic aerosol formation. This work investigated the level, seasonal variation, and trend of nitrate radical reactivity towards volatile organic compounds (kNO3) in Beijing. We show the key role of isoprene and styrene in regulating seasonal variation in kNO3 and rebuild a long-term record of kNO3 based on the reported VOC measurements.
Yuchen Wang, Xvli Guo, Yajie Huo, Mengying Li, Yuqing Pan, Shaocai Yu, Alexander Baklanov, Daniel Rosenfeld, John H. Seinfeld, and Pengfei Li
Atmos. Chem. Phys., 23, 5233–5249, https://doi.org/10.5194/acp-23-5233-2023, https://doi.org/10.5194/acp-23-5233-2023, 2023
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Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
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Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
Qian Shu, Sergey L. Napelenok, William T. Hutzell, Kirk R. Baker, Barron H. Henderson, Benjamin N. Murphy, and Christian Hogrefe
Geosci. Model Dev., 16, 2303–2322, https://doi.org/10.5194/gmd-16-2303-2023, https://doi.org/10.5194/gmd-16-2303-2023, 2023
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Source attribution methods are generally used to determine culpability of precursor emission sources to ambient pollutant concentrations. However, source attribution of secondarily formed pollutants such as ozone and its precursors cannot be explicitly measured, making evaluation of source apportionment methods challenging. In this study, multiple apportionment approach comparisons show common features but still reveal wide variations in predicted sector contribution and species dependency.
Forwood Wiser, Bryan K. Place, Siddhartha Sen, Havala O. T. Pye, Benjamin Yang, Daniel M. Westervelt, Daven K. Henze, Arlene M. Fiore, and V. Faye McNeill
Geosci. Model Dev., 16, 1801–1821, https://doi.org/10.5194/gmd-16-1801-2023, https://doi.org/10.5194/gmd-16-1801-2023, 2023
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Jingyu An, Cheng Huang, Dandan Huang, Momei Qin, Huan Liu, Rusha Yan, Liping Qiao, Min Zhou, Yingjie Li, Shuhui Zhu, Qian Wang, and Hongli Wang
Atmos. Chem. Phys., 23, 323–344, https://doi.org/10.5194/acp-23-323-2023, https://doi.org/10.5194/acp-23-323-2023, 2023
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Xun Li, Momei Qin, Lin Li, Kangjia Gong, Huizhong Shen, Jingyi Li, and Jianlin Hu
Atmos. Chem. Phys., 22, 14799–14811, https://doi.org/10.5194/acp-22-14799-2022, https://doi.org/10.5194/acp-22-14799-2022, 2022
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Photochemical indicators have been widely used to predict O3–NOx–VOC sensitivity with given thresholds. Here we assessed the effectiveness of four indicators with a case study in the Yangtze River Delta, China. The overall performance was good, while some indicators showed inconsistencies with the O3 isopleths. The methodology used to determine the thresholds may produce uncertainties. These results would improve our understanding of the use of photochemical indicators in policy implications.
Peeyush Khare, Jordan E. Krechmer, Jo E. Machesky, Tori Hass-Mitchell, Cong Cao, Junqi Wang, Francesca Majluf, Felipe Lopez-Hilfiker, Sonja Malek, Will Wang, Karl Seltzer, Havala O. T. Pye, Roisin Commane, Brian C. McDonald, Ricardo Toledo-Crow, John E. Mak, and Drew R. Gentner
Atmos. Chem. Phys., 22, 14377–14399, https://doi.org/10.5194/acp-22-14377-2022, https://doi.org/10.5194/acp-22-14377-2022, 2022
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Ammonium adduct chemical ionization is used to examine the atmospheric abundances of oxygenated volatile organic compounds associated with emissions from volatile chemical products, which are now key contributors of reactive precursors to ozone and secondary organic aerosols in urban areas. The application of this valuable measurement approach in densely populated New York City enables the evaluation of emissions inventories and thus the role these oxygenated compounds play in urban air quality.
Jinjin Sun, Momei Qin, Xiaodong Xie, Wenxing Fu, Yang Qin, Li Sheng, Lin Li, Jingyi Li, Ishaq Dimeji Sulaymon, Lei Jiang, Lin Huang, Xingna Yu, and Jianlin Hu
Atmos. Chem. Phys., 22, 12629–12646, https://doi.org/10.5194/acp-22-12629-2022, https://doi.org/10.5194/acp-22-12629-2022, 2022
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NO3- has become the dominant and the least reduced chemical component of fine particulate matter in China. NO3- formation is mostly in the NH3-rich regime in the Yangtze River Delta (YRD). OH + NO2 contributes 60 %–83 % of the TNO3 production rates, and the N2O5 heterogeneous pathway contributes 10 %–36 %. The N2O5 heterogeneous pathway becomes more important in cold seasons. Local emissions and regional transportation contribute 50 %–62 % and 38 %–50 % to YRD NO3- concentrations, respectively.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866, https://doi.org/10.5194/acp-22-11845-2022, https://doi.org/10.5194/acp-22-11845-2022, 2022
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This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Shenglun Wu, Hyung Joo Lee, Andrea Anderson, Shang Liu, Toshihiro Kuwayama, John H. Seinfeld, and Michael J. Kleeman
Atmos. Chem. Phys., 22, 4929–4949, https://doi.org/10.5194/acp-22-4929-2022, https://doi.org/10.5194/acp-22-4929-2022, 2022
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An ozone control experiment usually conducted in the laboratory was installed in a trailer and moved to the outdoor environment to directly confirm that we are controlling the right sources in order to lower ambient ozone concentrations. Adding small amounts of precursor oxides of nitrogen and volatile organic compounds to ambient air showed that the highest ozone concentrations are best controlled by reducing concentrations of oxides of nitrogen. The results confirm satellite measurements.
Sophia M. Charan, Yuanlong Huang, Reina S. Buenconsejo, Qi Li, David R. Cocker III, and John H. Seinfeld
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Linhui Jiang, Yan Xia, Lu Wang, Xue Chen, Jianjie Ye, Tangyan Hou, Liqiang Wang, Yibo Zhang, Mengying Li, Zhen Li, Zhe Song, Yaping Jiang, Weiping Liu, Pengfei Li, Daniel Rosenfeld, John H. Seinfeld, and Shaocai Yu
Atmos. Chem. Phys., 21, 16985–17002, https://doi.org/10.5194/acp-21-16985-2021, https://doi.org/10.5194/acp-21-16985-2021, 2021
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Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Weimeng Kong, Stavros Amanatidis, Huajun Mai, Changhyuk Kim, Benjamin C. Schulze, Yuanlong Huang, Gregory S. Lewis, Susanne V. Hering, John H. Seinfeld, and Richard C. Flagan
Atmos. Meas. Tech., 14, 5429–5445, https://doi.org/10.5194/amt-14-5429-2021, https://doi.org/10.5194/amt-14-5429-2021, 2021
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We present the design, modeling, and experimental characterization of the nano-scanning electrical mobility spectrometer (nSEMS), a recently developed instrument that probes particle physical properties in the 1.5–25 nm range. The nSEMS has proven to be extremely powerful in examining atmospheric nucleation and the subsequent growth of nanoparticles in the CERN CLOUD experiment, which provides a valuable asset to study atmospheric nanoparticles and to evaluate their impact on climate.
Xiaoyang Chen, Yang Zhang, Kai Wang, Daniel Tong, Pius Lee, Youhua Tang, Jianping Huang, Patrick C. Campbell, Jeff Mcqueen, Havala O. T. Pye, Benjamin N. Murphy, and Daiwen Kang
Geosci. Model Dev., 14, 3969–3993, https://doi.org/10.5194/gmd-14-3969-2021, https://doi.org/10.5194/gmd-14-3969-2021, 2021
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The continuously updated National Air Quality Forecast Capability (NAQFC) provides air quality forecasts. To support the development of the next-generation NAQFC, we evaluate a prototype of GFSv15-CMAQv5.0.2. The performance and the potential improvements for the system are discussed. This study can provide a scientific basis for further development of NAQFC and help it to provide more accurate air quality forecasts to the public over the contiguous United States.
Stavros Amanatidis, Yuanlong Huang, Buddhi Pushpawela, Benjamin C. Schulze, Christopher M. Kenseth, Ryan X. Ward, John H. Seinfeld, Susanne V. Hering, and Richard C. Flagan
Atmos. Meas. Tech., 14, 4507–4516, https://doi.org/10.5194/amt-14-4507-2021, https://doi.org/10.5194/amt-14-4507-2021, 2021
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We assess the performance of a highly portable mobility analyzer, the Spider DMA, in measuring ambient aerosol particle size distributions, with specific attention to its moderate sizing resolution (R=3). Long-term field testing showed excellent correlation with a conventional mobility analyzer (R=10) over the 17–500 nm range, suggesting that moderate resolution may be sufficient to obtain key properties of ambient size distributions, enabling smaller instruments and better counting statistics.
Benjamin N. Murphy, Christopher G. Nolte, Fahim Sidi, Jesse O. Bash, K. Wyat Appel, Carey Jang, Daiwen Kang, James Kelly, Rohit Mathur, Sergey Napelenok, George Pouliot, and Havala O. T. Pye
Geosci. Model Dev., 14, 3407–3420, https://doi.org/10.5194/gmd-14-3407-2021, https://doi.org/10.5194/gmd-14-3407-2021, 2021
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The algorithms for applying air pollution emission rates in the Community Multiscale Air Quality (CMAQ) model have been improved to better support users and developers. The new features accommodate emissions perturbation studies that are typical in atmospheric research and output a wealth of metadata for each model run so assumptions can be verified and documented. The new approach dramatically enhances the transparency and functionality of this critical aspect of atmospheric modeling.
K. Wyat Appel, Jesse O. Bash, Kathleen M. Fahey, Kristen M. Foley, Robert C. Gilliam, Christian Hogrefe, William T. Hutzell, Daiwen Kang, Rohit Mathur, Benjamin N. Murphy, Sergey L. Napelenok, Christopher G. Nolte, Jonathan E. Pleim, George A. Pouliot, Havala O. T. Pye, Limei Ran, Shawn J. Roselle, Golam Sarwar, Donna B. Schwede, Fahim I. Sidi, Tanya L. Spero, and David C. Wong
Geosci. Model Dev., 14, 2867–2897, https://doi.org/10.5194/gmd-14-2867-2021, https://doi.org/10.5194/gmd-14-2867-2021, 2021
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This paper details the scientific updates in the recently released CMAQ version 5.3 (and v5.3.1) and also includes operational and diagnostic evaluations of CMAQv5.3.1 against observations and the previous version of the CMAQ (v5.2.1). This work was done to improve the underlying science in CMAQ. This article is used to inform the CMAQ modeling community of the updates to the modeling system and the expected change in model performance from these updates (versus the previous model version).
Qian Shu, Benjamin Murphy, Jonathan E. Pleim, Donna Schwede, Barron H. Henderson, Havala O.T. Pye, Keith Wyat Appel, Tanvir R. Khan, and Judith A. Perlinger
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-129, https://doi.org/10.5194/gmd-2021-129, 2021
Preprint withdrawn
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We have bridged the gap between dry deposition measurement and modeling by rigorous use of box and regional transport models and field measurements, but more efforts are needed. This study highlights that deviation among deposition schemes is most pronounced for small and large particles. This study better links model predictions to available real-world observations and incrementally reduces uncertainties in the magnitude of loss processes important for the lifecycle of air pollutants.
Karl M. Seltzer, Elyse Pennington, Venkatesh Rao, Benjamin N. Murphy, Madeleine Strum, Kristin K. Isaacs, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 5079–5100, https://doi.org/10.5194/acp-21-5079-2021, https://doi.org/10.5194/acp-21-5079-2021, 2021
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Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon emissions. Here, we develop VCPy, a new framework to model organic emissions from VCPs throughout the United States. At the national-level, VCPy emissions are broadly consistent with the US EPA’s 2017 National Emission Inventory, however county-level and categorical estimates can differ substantially. An observational evaluation indicates high fidelity in the methods employed here.
Liqiang Wang, Shaocai Yu, Pengfei Li, Xue Chen, Zhen Li, Yibo Zhang, Mengying Li, Khalid Mehmood, Weiping Liu, Tianfeng Chai, Yannian Zhu, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 20, 14787–14800, https://doi.org/10.5194/acp-20-14787-2020, https://doi.org/10.5194/acp-20-14787-2020, 2020
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The Chinese government has made major strides in curbing anthropogenic emissions. In this study, we constrain a state-of-the-art CTM by a reliable data assimilation method with extensive chemical and meteorological observations. This comprehensive technical design provides a crucial advance in isolating the influences of emission changes and meteorological perturbations over the Yangtze River Delta (YRD) from 2016 to 2019, thus establishing the first map of the PM2.5 mitigation across the YRD.
Brigitte Rooney, Yuan Wang, Jonathan H. Jiang, Bin Zhao, Zhao-Cheng Zeng, and John H. Seinfeld
Atmos. Chem. Phys., 20, 14597–14616, https://doi.org/10.5194/acp-20-14597-2020, https://doi.org/10.5194/acp-20-14597-2020, 2020
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Wildfires have become increasingly prevalent. Intense smoke consisting of particulate matter (PM) leads to an increased risk of morbidity and mortality. The record-breaking Camp Fire ravaged Northern California for two weeks in 2018. Here, we employ a comprehensive chemical transport model along with ground-based and satellite observations to characterize the PM concentrations across Northern California and to investigate the pollution sensitivity predictions to key parameters of the model.
Sophia M. Charan, Reina S. Buenconsejo, and John H. Seinfeld
Atmos. Chem. Phys., 20, 13167–13190, https://doi.org/10.5194/acp-20-13167-2020, https://doi.org/10.5194/acp-20-13167-2020, 2020
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In urban areas, the emissions from volatile chemical products may be responsible for the formation of as much particulate matter as motor vehicles. Since exposure to particulate matter is a public health crisis, understanding its formation is critical. In this work, we investigate the secondary organic aerosol formation potential of benzyl alcohol, an important compound that is representative of some of these new emission sources, and find that more particulate matter forms than is expected.
Cited articles
Appel, K. W., Bash, J. O., Fahey, K. M., Foley, K. M., Gilliam, R. C., Hogrefe, C., Hutzell, W. T., Kang, D., Mathur, R., Murphy, B. N., Napelenok, S. L., Nolte, C. G., Pleim, J. E., Pouliot, G. A., Pye, H. O. T., Ran, L., Roselle, S. J., Sarwar, G., Schwede, D. B., Sidi, F. I., Spero, T. L., and Wong, D. C.: The Community Multiscale Air Quality (CMAQ) model versions 5.3 and 5.3.1: system updates and evaluation, Geosci. Model Dev., 14, 2867–2897, https://doi.org/10.5194/gmd-14-2867-2021, 2021.
Baker, K. R., Carlton, A. G., Kleindienst, T. E., Offenberg, J. H., Beaver, M. R., Gentner, D. R., Goldstein, A. H., Hayes, P. L., Jimenez, J. L., Gilman, J. B., de Gouw, J. A., Woody, M. C., Pye, H. O. T., Kelly, J. T., Lewandowski, M., Jaoui, M., Stevens, P. S., Brune, W. H., Lin, Y.-H., Rubitschun, C. L., and Surratt, J. D.: Gas and aerosol carbon in California: comparison of measurements and model predictions in Pasadena and Bakersfield, Atmos. Chem. Phys., 15, 5243–5258, https://doi.org/10.5194/acp-15-5243-2015, 2015.
Bash, J. O., Baker, K. R., and Beaver, M. R.: Evaluation of improved land use and canopy representation in BEIS v3.61 with biogenic VOC measurements in California, Geosci. Model Dev., 9, 2191–2207, https://doi.org/10.5194/gmd-9-2191-2016, 2016.
Binkowski, F. S. and Roselle, S. J.: Models-3 Community Multiscale Air Quality (CMAQ) model aerosol component 1. Model description, J. Geophys. Res.-Atmos., 108, 4183, https://doi.org/10.1029/2001JD001409, 2003.
CalNex measurement data: NOAA Earth System Research Laboratory, CalNex 2010 [data set], available at: https://www.esrl.noaa.gov/csd/groups/csd7/measurements/2010calnex/ (last access: 7 July 2021), 2012.
Cappa, C. D. and Wilson, K. R.: Multi-generation gas-phase oxidation, equilibrium partitioning, and the formation and evolution of secondary organic aerosol, Atmos. Chem. Phys., 12, 9505–9528, https://doi.org/10.5194/acp-12-9505-2012, 2012.
Charan, S. M., Buenconsejo, R. S., and Seinfeld, J. H.: Secondary organic aerosol yields from the oxidation of benzyl alcohol, Atmos. Chem. Phys., 20, 13167–13190, https://doi.org/10.5194/acp-20-13167-2020, 2020.
Charan, S. M., Huang, Y., Buenconsejo, R. S., Li, Q., Cocker III, D. R., and Seinfeld, J. H.: Secondary Organic Aerosol Formation from the Oxidation of Decamethylcyclopentasiloxane at Atmospherically Relevant OH Concentrations, Atmos. Chem. Phys. Discuss. [preprint], https://doi.org/10.5194/acp-2021-353, in review, 2021.
Coggon, M. M., McDonald, B. C., Vlasenko, A., Veres, P. R., Bernard, F.,
Koss, A. R., Yuan, B., Gilman, J. B., Peischl, J., Aikin, K. C., DuRant, J.,
Warneke, C., Li, S.-M., and de Gouw, J. A.: Diurnal Variability and Emission
Pattern of Decamethylcyclopentasiloxane (D5) from the Application of
Personal Care Products in Two North American Cities, Environ. Sci. Technol.,
52, 5610–5618, https://doi.org/10.1021/acs.est.8b00506, 2018.
Coggon, M. M., Gkatzelis, G. I., McDonald, B. C., Gilman, J. B., Schwantes,
R. H., Abuhassan, N., Aikin, K. C., Arend, M. F., Berkoff, T. A., Brown, S.
S., Campos, T. L., Dickerson, R. R., Gronoff, G., Hurley, J. F.,
Isaacman-VanWertz, G., Koss, A. R., Li, M., McKeen, S. A., Moshary, F.,
Peischl, J., Pospisilova, V., Ren, X., Wilson, A. Wu, Y., Trainer, M., and
Warneke, C.: Volatile chemical product emissions enhance ozone and modulate
urban chemistry, P. Natl. Acad. Sci. USA, 118, e2026653118,
https://doi.org/10.1073/pnas.2026653118, 2021.
Crounse, J. D., Nielsen, L. B., Jørgensen, S., Kjaergaard, H. G., and
Wennberg, P. O.: Autoxidation of Organic Compounds in the Atmosphere, J.
Phys. Chem. Lett., 4, 3513–3520, https://doi.org/10.1021/jz4019207,
2013.
Donahue, N. M., Epstein, S. A., Pandis, S. N., and Robinson, A. L.: A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics, Atmos. Chem. Phys., 11, 3303–3318, https://doi.org/10.5194/acp-11-3303-2011, 2011.
Ensberg, J. J., Hayes, P. L., Jimenez, J. L., Gilman, J. B., Kuster, W. C., de Gouw, J. A., Holloway, J. S., Gordon, T. D., Jathar, S., Robinson, A. L., and Seinfeld, J. H.: Emission factor ratios, SOA mass yields, and the impact of vehicular emissions on SOA formation, Atmos. Chem. Phys., 14, 2383–2397, https://doi.org/10.5194/acp-14-2383-2014, 2014.
Epstein, S. A., Riipinen, I., and Donahue, N. M.: A Semiempirical
Correlation between Enthalpy of Vaporization and Saturation Concentration
for Organic Aerosol, Environ. Sci. Technol., 44, 743–748,
https://doi.org/10.1021/es902497z, 2010.
Gkatzelis, G. I., Coggon, M. M., McDonald, B. C., Peischl, J., Aikin, K. C.,
Gilman, J. B., Trainer, M., and Warneke, C.: Identifying Volatile Chemical
Product Tracer Compounds in U.S. Cities, Environ. Sci. Technol., 55,
188–199, https://doi.org/10.1021/acs.est.0c05467, 2021.
Goldstein, A. H. and Galbally, I. E.: Known and Unexplored Organic
Constituents in the Earth's Atmosphere, Environ. Sci. Technol., 41,
1514–1521, https://doi.org/10.1021/es072476p, 2007.
Griffith, S. M., Hansen, R. F., Dusanter, S., Michoud, V., Gilman, J. B.,
Kuster, W. C., Veres, P. R., Graus, M., Gouw, J. A. de, Roberts, J., Young,
C., Washenfelder, R., Brown, S. S., Thalman, R., Waxman, E., Volkamer, R.,
Tsai, C., Stutz, J., Flynn, J. H., Grossberg, N., Lefer, B., Alvarez, S. L.,
Rappenglueck, B., Mielke, L. H., Osthoff, H. D., and Stevens, P. S.:
Measurements of hydroxyl and hydroperoxy radicals during CalNex-LA: Model
comparisons and radical budgets, J. Geophys. Res.-Atmos., 121,
4211–4232, https://doi.org/10.1002/2015JD024358, 2016.
Hayes, P. L., Ortega, A. M., Cubison, M. J., Froyd, K. D., Zhao, Y., Cliff,
S. S., Hu, W. W., Toohey, D. W., Flynn, J. H., Lefer, B. L., Grossberg, N.,
Alvarez, S., Rappenglück, B., Taylor, J. W., Allan, J. D., Holloway, J.
S., Gilman, J. B., Kuster, W. C., de Gouw, J. A., Massoli, P., Zhang, X.,
Liu, J., Weber, R. J., Corrigan, A. L., Russell, L. M., Isaacman, G., Worton,
D. R., Kreisberg, N. M., Goldstein, A. H., Thalman, R., Waxman, E. M., Volkamer, R., Lin, Y.H., Surratt, J. D., Kleindienst, T. E., Offenberg, J. H., Dusanter, S., Griffith, S., Stevens, P. S., Brioude, J., Angevine, W. M., and Jimenez, J. L.: Organic aerosol composition and sources in Pasadena, California, during the 2010 CalNex campaign, J. Geophys. Res.-Atmos., 118,
9233–9257, https://doi.org/10.1002/jgrd.50530, 2013.
Hayes, P. L., Carlton, A. G., Baker, K. R., Ahmadov, R., Washenfelder, R. A., Alvarez, S., Rappenglück, B., Gilman, J. B., Kuster, W. C., de Gouw, J. A., Zotter, P., Prévôt, A. S. H., Szidat, S., Kleindienst, T. E., Offenberg, J. H., Ma, P. K., and Jimenez, J. L.: Modeling the formation and aging of secondary organic aerosols in Los Angeles during CalNex 2010, Atmos. Chem. Phys., 15, 5773–5801, https://doi.org/10.5194/acp-15-5773-2015, 2015.
Hodzic, A., Aumont, B., Knote, C., Lee-Taylor, J., Madronich, S., and
Tyndall, G.: Volatility dependence of Henry's law constants of condensable
organics: Application to estimate depositional loss of secondary organic
aerosols, Geophys. Res. Lett., 41, 4795–4804,
https://doi.org/10.1002/2014GL060649, 2014.
Huffman, J. A., Docherty, K. S., Mohr, C., Cubison, M. J., Ulbrich, I. M.,
Ziemann, P. J., Onasch, T. B., and Jimenez, J. L.: Chemically-Resolved
Volatility Measurements of Organic Aerosol from Different Sources, Environ.
Sci. Technol., 43, 5351–5357, https://doi.org/10.1021/es803539d, 2009.
Hyslop, N. P.: Impaired visibility: The air pollution people see, Atmos.
Environ., 43, 182–195, https://doi.org/10.1016/j.atmosenv.2008.09.067,
2009.
Intergovernmental Panel on Climate Change: Anthropogenic and Natural
Radiative Forcing, in: Climate Change 2013 – The Physical Science Basis:
Working Group I Contribution to the Fifth Assessment Report of the
Intergovernmental Panel on Climate Change, Cambridge University Press,
659–740, https://doi.org/10.1017/CBO9781107415324.018, 2014.
Janechek, N. J., Hansen, K. M., and Stanier, C. O.: Comprehensive atmospheric modeling of reactive cyclic siloxanes and their oxidation products, Atmos. Chem. Phys., 17, 8357–8370, https://doi.org/10.5194/acp-17-8357-2017, 2017.
Janechek, N. J., Marek, R. F., Bryngelson, N., Singh, A., Bullard, R. L., Brune, W. H., and Stanier, C. O.: Physical properties of secondary photochemical aerosol from OH oxidation of a cyclic siloxane, Atmos. Chem. Phys., 19, 1649–1664, https://doi.org/10.5194/acp-19-1649-2019, 2019.
Jathar, S. H., Gordon, T. D., Hennigan, C. J., Pye, H. O. T., Pouliot, G.,
Adams, P. J., Donahue, N. M., and Robinson, A. L.: Unspeciated organic
emissions from combustion sources and their influence on the secondary
organic aerosol budget in the United States, P. Natl. Acad. Sci. USA,
111, 10473–10478, https://doi.org/10.1073/pnas.1323740111, 2014.
Jathar, S. H., Woody, M., Pye, H. O. T., Baker, K. R., and Robinson, A. L.: Chemical transport model simulations of organic aerosol in southern California: model evaluation and gasoline and diesel source contributions, Atmos. Chem. Phys., 17, 4305–4318, https://doi.org/10.5194/acp-17-4305-2017, 2017.
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang,
Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken,
A. C., Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L.,
Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun,
Y. L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara,
P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J.,
Dunlea, E. J., Huffman, J. A., Onasch, T. B., Alfarrap, M. R., Williams, P. I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina, K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A. M.,
Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb, C. E., Baltensperger,
U., and Worsnop, D. R.: Evolution of Organic Aerosols in the Atmosphere,
Science, 326, 1525–1529, https://doi.org/10.1126/science.1180353,
2009.
Kaiser, J., Wolfe, G. M., Bohn, B., Broch, S., Fuchs, H., Ganzeveld, L. N., Gomm, S., Häseler, R., Hofzumahaus, A., Holland, F., Jäger, J., Li, X., Lohse, I., Lu, K., Prévôt, A. S. H., Rohrer, F., Wegener, R., Wolf, R., Mentel, T. F., Kiendler-Scharr, A., Wahner, A., and Keutsch, F. N.: Evidence for an unidentified non-photochemical ground-level source of formaldehyde in the Po Valley with potential implications for ozone production, Atmos. Chem. Phys., 15, 1289–1298, https://doi.org/10.5194/acp-15-1289-2015, 2015.
Khare, P. and Gentner, D. R.: Considering the future of anthropogenic gas-phase organic compound emissions and the increasing influence of non-combustion sources on urban air quality, Atmos. Chem. Phys., 18, 5391–5413, https://doi.org/10.5194/acp-18-5391-2018, 2018.
Khare, P., Machesky, J., Soto, R., He, M., Presto, A. A., and Gentner, D. R.: Asphalt-related emissions are a major missing nontraditional source of
secondary organic aerosol precursors, Science Adv., 6, eabb9785,
https://doi.org/10.1126/sciadv.abb9785, 2020.
Levelt, P. F., Joiner, J., Tamminen, J., Veefkind, J. P., Bhartia, P. K., Stein Zweers, D. C., Duncan, B. N., Streets, D. G., Eskes, H., van der A, R., McLinden, C., Fioletov, V., Carn, S., de Laat, J., DeLand, M., Marchenko, S., McPeters, R., Ziemke, J., Fu, D., Liu, X., Pickering, K., Apituley, A., González Abad, G., Arola, A., Boersma, F., Chan Miller, C., Chance, K., de Graaf, M., Hakkarainen, J., Hassinen, S., Ialongo, I., Kleipool, Q., Krotkov, N., Li, C., Lamsal, L., Newman, P., Nowlan, C., Suleiman, R., Tilstra, L. G., Torres, O., Wang, H., and Wargan, K.: The Ozone Monitoring Instrument: overview of 14 years in space, Atmos. Chem. Phys., 18, 5699–5745, https://doi.org/10.5194/acp-18-5699-2018, 2018.
Li, L. and Cocker, D. R.: Molecular structure impacts on secondary organic
aerosol formation from glycol ethers, Atmos. Environ., 180, 206–215,
https://doi.org/10.1016/j.atmosenv.2017.12.025, 2018.
Li, W., Li, L., Chen, C., Kacarab, M., Peng, W., Price, D., Xu, J., and
Cocker, D. R.: Potential of select intermediate-volatility organic compounds
and consumer products for secondary organic aerosol and ozone formation
under relevant urban conditions, Atmos. Environ., 178, 109–117,
https://doi.org/10.1016/j.atmosenv.2017.12.019, 2018.
Li, Y., Rodier, C., Lea, J. D., Harvey, J., and Kleeman, M. J.: Improving
spatial surrogates for area source emissions inventories in California,
Atmos. Environ., 247, 117665, https://doi.org/10.1016/j.atmosenv.2020.117665, 2021.
Liao, J., Hanisco, T. F., Wolfe, G. M., St. Clair, J., Jimenez, J. L., Campuzano-Jost, P., Nault, B. A., Fried, A., Marais, E. A., Gonzalez Abad, G., Chance, K., Jethva, H. T., Ryerson, T. B., Warneke, C., and Wisthaler, A.: Towards a satellite formaldehyde – in situ hybrid estimate for organic aerosol abundance, Atmos. Chem. Phys., 19, 2765–2785, https://doi.org/10.5194/acp-19-2765-2019, 2019.
Lu, Q., Murphy, B. N., Qin, M., Adams, P. J., Zhao, Y., Pye, H. O. T., Efstathiou, C., Allen, C., and Robinson, A. L.: Simulation of organic aerosol formation during the CalNex study: updated mobile emissions and secondary organic aerosol parameterization for intermediate-volatility organic compounds, Atmos. Chem. Phys., 20, 4313–4332, https://doi.org/10.5194/acp-20-4313-2020, 2020.
Luecken, D. J., Napelenok, S. L., Strum, M., Scheffe, R., and Phillips, S.:
Sensitivity of Ambient Atmospheric Formaldehyde and Ozone to Precursor
Species and Source Types Across the United States, Environ. Sci. Technol.,
52, 4668–4675, https://doi.org/10.1021/acs.est.7b05509, 2018.
McDonald, B. C., Gouw, J. A. de, Gilman, J. B., Jathar, S. H., Akherati, A.,
Cappa, C. D., Jimenez, J. L., Lee-Taylor, J., Hayes, P. L., McKeen, S. A.,
Cui, Y. Y., Kim, S.-W., Gentner, D. R., Isaacman-VanWertz, G., Goldstein, A.
H., Harley, R. A., Frost, G. J., Roberts, J. M., Ryerson, T. B., and
Trainer, M.: Volatile chemical products emerging as largest petrochemical
source of urban organic emissions, Science, 359, 760–764,
https://doi.org/10.1126/science.aaq0524, 2018.
Milani, A., Al-Naiema, I. M., and Stone, E. A.: Detection of a secondary
organic aerosol tracer derived from personal care products, Atmos. Environ.,
246, 118078, https://doi.org/10.1016/j.atmosenv.2020.118078, 2021.
Murphy, B. N., Woody, M. C., Jimenez, J. L., Carlton, A. M. G., Hayes, P. L., Liu, S., Ng, N. L., Russell, L. M., Setyan, A., Xu, L., Young, J., Zaveri, R. A., Zhang, Q., and Pye, H. O. T.: Semivolatile POA and parameterized total combustion SOA in CMAQv5.2: impacts on source strength and partitioning, Atmos. Chem. Phys., 17, 11107–11133, https://doi.org/10.5194/acp-17-11107-2017, 2017.
Murphy, B. N., Nolte, C. G., Sidi, F., Bash, J. O., Appel, K. W., Jang, C., Kang, D., Kelly, J., Mathur, R., Napelenok, S., Pouliot, G., and Pye, H. O. T.: The Detailed Emissions Scaling, Isolation, and Diagnostic (DESID) module in the Community Multiscale Air Quality (CMAQ) modeling system version 5.3.2, Geosci. Model Dev., 14, 3407–3420, https://doi.org/10.5194/gmd-14-3407-2021, 2021.
Nussbaumer, C. M. and Cohen, R. C.: Impact of OA on the Temperature
Dependence of PM2.5 in the Los Angeles Basin, Environ. Sci. Technol.,
55, 3549–3558, https://doi.org/10.1021/acs.est.0c07144, 2021.
Pye, H. O. T., Pinder, R. W., Piletic, I. R., Xie, Y., Capps, S. L., Lin,
Y.-H., Surratt, J. D., Zhang, Z., Gold, A., Luecken, D. J., Hutzell, W. T.,
Jaoui, M., Offenberg, J. H., Kleindienst, T. E., Lewandowski, M., and Edney,
E. O.: Epoxide Pathways Improve Model Predictions of Isoprene Markers and
Reveal Key Role of Acidity in Aerosol Formation, Environ. Sci. Technol.,
47, 11056–11064, https://doi.org/10.1021/es402106h, 2013.
Pye, H. O. T., Murphy, B. N., Xu, L., Ng, N. L., Carlton, A. G., Guo, H., Weber, R., Vasilakos, P., Appel, K. W., Budisulistiorini, S. H., Surratt, J. D., Nenes, A., Hu, W., Jimenez, J. L., Isaacman-VanWertz, G., Misztal, P. K., and Goldstein, A. H.: On the implications of aerosol liquid water and phase separation for organic aerosol mass, Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, 2017.
Qin, M., Murphy, B. N., Isaacs, K. K., McDonald, B. C., Lu, Q., McKeen, S.
A., Koval, L., Robinson, A. L., Efstathiou, C., Allen, C., and Pye, H. O.
T.: Criteria pollutant impacts of volatile chemical products informed by
near-field modelling, Nat. Sustain., 4, 129–137,
https://doi.org/10.1038/s41893-020-00614-1, 2021.
Robinson, A. L., Donahue, N. M., Shrivastava, M. K., Weitkamp, E. A., Sage,
A. M., Grieshop, A. P., Lane, T. E., Pierce, J. R., and Pandis, S. N.:
Rethinking Organic Aerosols: Semivolatile Emissions and Photochemical Aging,
Science, 315, 1259–1262, https://doi.org/10.1126/science.1133061,
2007.
Ryerson, T. B., Andrews, A. E., Angevine, W. M., Bates, T. S., Brock, C. A.,
Cairns, B., Cohen, R. C., Cooper, O. R., de Gouw, J. A., Fehsenfeld, F. C.,
Ferrare, R. A., Fischer, M. L., Flagan, R. C., Goldstein, A. H., Hair, J.
W., Hardesty, R. M., Hostetler, C. A., Jimenez, J. L., Langford, A. O.,
McCauley, E., McKeen, S. A., Molina, L. T., Nenes, A., Oltmans, S. J., Parrish, D. D., Pederson, J. R., Pierce, R. B., Prather, K., Quinn, P. K., Seinfeld, J. H., Senff, C. J., Sorooshian, A., Stutz, J., Surratt, J. D., Trainer, M., Volkamer, R., Williams, E. J., and Wofsy, S. C.: The 2010 California Research at the Nexus of Air Quality and Climate Change (CalNex) field study, J. Geophys. Res.-Atmos., 118, 5830–5866, https://doi.org/10.1002/jgrd.50331, 2013.
Santoni, G. W., Daube, B. C., Kort, E. A., Jiménez, R., Park, S., Pittman, J. V., Gottlieb, E., Xiang, B., Zahniser, M. S., Nelson, D. D., McManus, J. B., Peischl, J., Ryerson, T. B., Holloway, J. S., Andrews, A. E., Sweeney, C., Hall, B., Hintsa, E. J., Moore, F. L., Elkins, J. W., Hurst, D. F., Stephens, B. B., Bent, J., and Wofsy, S. C.: Evaluation of the airborne quantum cascade laser spectrometer (QCLS) measurements of the carbon and greenhouse gas suite – CO2, CH4, N2O, and CO – during the CalNex and HIPPO campaigns, Atmos. Meas. Tech., 7, 1509–1526, https://doi.org/10.5194/amt-7-1509-2014, 2014.
Seinfeld, J. H. and Pandis, S. N.: From Air Pollution to Climate Change, 3rd edn., in: Atmospheric Chemistry and Physics, John Wiley & Sons, Inc., Hoboken, New Jersey,
2016.
Seltzer, K. M., Pennington, E., Rao, V., Murphy, B. N., Strum, M., Isaacs, K. K., and Pye, H. O. T.: Reactive organic carbon emissions from volatile chemical products, Atmos. Chem. Phys., 21, 5079–5100, https://doi.org/10.5194/acp-21-5079-2021, 2021.
Shah, R. U., Coggon, M. M., Gkatzelis, G. I., McDonald, B. C., Tasoglou, A.,
Huber, H., Gilman, J., Warneke, C., Robinson, A. L., and Presto, A. A.:
Urban Oxidation Flow Reactor Measurements Reveal Significant Secondary
Organic Aerosol Contributions from Volatile Emissions of Emerging
Importance, Environ. Sci. Technol., 54, 714–725, https://doi.org/10.1021/acs.est.9b06531, 2020a.
Shah, T., Shi, Y., Beardsley, R., and Yarwood, G.: Speciation Tool User's Guide Version 5.0, Ramboll US Corporation, Novato, California, 41 pp., 2020b.
Skamarock, W. C., Klemp, J. B., Dudhia, J., Gill, D. O., and Barker, D.: A Description of the Advanced Research WRF Version 3
(NCAR/TN-475+STR), University Corporation for Atmospheric Research, 113 pp.,
https://doi.org/10.5065/D68S4MVH, 2008.
U.S. EPA: Air Quality System (AQS), U.S. EPA [data set], available at:
https://www.epa.gov/aqs (last access: 4 February 2021), 2013.
U.S. EPA: National Emissions Inventory (NEI), U.S. EPA [code], available at:
https://www.epa.gov/air-emissions-inventories/national-emissions-inventory-nei (last access: 23 June 2021),
2015.
U.S. EPA: AE7I Species Table, U.S. EPA [code], available at:
https://github.com/USEPA/CMAQ/blob/72ec4e5681e1ed0b4917792a9a240b0302a303a7/CCTM/src/MECHS/mechanism_information/saprc07tic_ae7i_aq/AE7I_species_table.md (last access: 23 June 2021), 2016.
U.S. EPA: CMAQ, Zenodo [code], https://doi.org/10.5281/zenodo.4081737, 2020.
U.S. EPA: Reactive Organic Carbon Emissions from Volatile Chemical Products, U.S. EPA Office of Research and Development (ORD) [data set], https://doi.org/10.23719/1520157, 2021a.
U.S. EPA: Data for Modeling secondary organic aerosol formation from volatile chemical products, U.S. EPA Office of Research and Development (ORD) [data set], https://doi.org/10.23719/1522655, 2021b.
Wang, D.-G., Norwood, W., Alaee, M., Byer, J. D., and Brimble, S.: Review of
recent advances in research on the toxicity, detection, occurrence and fate
of cyclic volatile methyl siloxanes in the environment, Chemosphere, 93,
711–725, https://doi.org/10.1016/j.chemosphere.2012.10.041, 2013.
Wang, Y., Wang, H., Tan, Y., Liu, J., Wang, K., Ji, W., Sun, L., Yu, X.,
Zhao, J., Xu, B., and Xiong, J.: Measurement of the key parameters of VOC
emissions from wooden furniture, and the impact of temperature. Atmos.
Environ., 259, 118510, https://doi.org/10.1016/j.atmosenv.2021.118510, 2021.
Warneke, C., Veres, P., Holloway, J. S., Stutz, J., Tsai, C., Alvarez, S., Rappenglueck, B., Fehsenfeld, F. C., Graus, M., Gilman, J. B., and de Gouw, J. A.: Airborne formaldehyde measurements using PTR-MS: calibration, humidity dependence, inter-comparison and initial results, Atmos. Meas. Tech., 4, 2345–2358, https://doi.org/10.5194/amt-4-2345-2011, 2011.
Woody, M. C., Baker, K. R., Hayes, P. L., Jimenez, J. L., Koo, B., and Pye, H. O. T.: Understanding sources of organic aerosol during CalNex-2010 using the CMAQ-VBS, Atmos. Chem. Phys., 16, 4081–4100, https://doi.org/10.5194/acp-16-4081-2016, 2016.
Wu, Y. and Johnston, M. V.: Aerosol Formation from OH Oxidation of the
Volatile Cyclic Methyl Siloxane (cVMS) Decamethylcyclopentasiloxane,
Environ. Sci. Technol., 51, 4445–4451,
https://doi.org/10.1021/acs.est.7b00655, 2017.
Xie, Y., Paulot, F., Carter, W. P. L., Nolte, C. G., Luecken, D. J., Hutzell, W. T., Wennberg, P. O., Cohen, R. C., and Pinder, R. W.: Understanding the impact of recent advances in isoprene photooxidation on simulations of regional air quality, Atmos. Chem. Phys., 13, 8439–8455, https://doi.org/10.5194/acp-13-8439-2013, 2013.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H.,
Ulbrich, I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L.,
Dzepina, K., Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch,
T., Jayne, J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N.,
Kondo, Y., Schneider J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian,
K., Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J.,
Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.: Ubiquity and
dominance of oxygenated species in organic aerosols in
anthropogenically-influenced Northern Hemisphere midlatitudes, Geophys. Res.
Lett., 34, L13801, https://doi.org/10.1029/2007GL029979, 2007.
Zhao, Y., Hennigan, C. J., May, A. A., Tkacik, D. S., de Gouw, J. A.,
Gilman, J. B., Kuster, W. C., Borbon, A., and Robinson, A. L.:
Intermediate-Volatility Organic Compounds: A Large Source of Secondary
Organic Aerosol, Environ. Sci. Technol., 48, 13743–13750,
https://doi.org/10.1021/es5035188, 2014.
Zhao, Y., Nguyen, N. T., Presto, A. A., Hennigan, C. J., May, A. A., and
Robinson, A. L.: Intermediate Volatility Organic Compound Emissions from
On-Road Diesel Vehicles: Chemical Composition, Emission Factors, and
Estimated Secondary Organic Aerosol Production, Environ. Sci. Technol.,
49, 11516–11526, https://doi.org/10.1021/acs.est.5b02841, 2015.
Short summary
Volatile chemical products (VCPs) are commonly used consumer and industrial items that contribute to the formation of atmospheric aerosol. We implemented the emissions and chemistry of VCPs in a regional-scale model and compared predictions with measurements made in Los Angeles. Our results reduced model bias and suggest that VCPs may contribute up to half of anthropogenic secondary organic aerosol in Los Angeles and are an important source of human-influenced particular matter in urban areas.
Volatile chemical products (VCPs) are commonly used consumer and industrial items that...
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