Grantee Research Project Results
2017 Progress Report: Rethinking the Formation of Secondary Organic Aerosols (SOA) Under Changing Climate by Incorporating Mechanistic and Field Constraints
EPA Grant Number: R835877Title: Rethinking the Formation of Secondary Organic Aerosols (SOA) Under Changing Climate by Incorporating Mechanistic and Field Constraints
Investigators: Jimenez, Jose-Luis , Hodzic, Alma , Aumont, Bernard , Lamarque, Jean-Francois , Emmons, Louisa , Madronich, Sasha
Current Investigators: Jimenez, Jose-Luis , Emmons, Louisa , Hodzic, Alma , Aumont, Bernard , Lamarque, Jean-Francois , Madronich, Sasha
Institution: University of Colorado at Boulder , National Center for Atmospheric Research
EPA Project Officer: Keating, Terry
Project Period: January 1, 2016 through December 31, 2018 (Extended to October 15, 2020)
Project Period Covered by this Report: January 1, 2017 through December 31,2017
Project Amount: $469,808
RFA: Particulate Matter and Related Pollutants in a Changing World (2014) RFA Text | Recipients Lists
Research Category: Air , Climate Change
Objective:
The overall objective of this work is to evaluate the changes and impacts of secondary organic aerosols (SOA) under future climate scenarios, using more realistic formation mechanisms than have been used in past studies. This is important because SOA has important impacts on human health and radiative forcing, and at present it is unclear how those effects will change under future climate and emission conditions. SOA parameterizations will be made more realistic and traceable by constraining them with the semi-explicit and explicit models, and constraining them with oxidation flow reactor (OFR) and thermodenuder (TD) observations. Regional and global model results will be evaluated against observations from high quality airborne field campaigns (already collected at no cost to this project) and from ground sites and networks. The 3D models will then be used to project the changes and impacts of SOA under future climate scenarios.
Progress Summary:
There are three main objectives in this project: (1) develop and test updated SOA formation parameterizations; (2) calculate present SOA using 3D models and compare to observations; and (3) evaluate SOA using 3D models under future climate scenarios. Further details of the objectives are given in section 3 of the proposal. Work to date has focused on objectives 1 and 2, consistent with the timeline in the proposal. The results are described below and directly address the objectives of this proposal and will help improve SOA modeling under current and future climate scenarios. Therefore, these results contribute to EPA’s mission to protect human health and the environment through the improved understanding and ability to predict the behavior of aerosols in the atmosphere, which are known to have major effects on human health and climate.
Objective 1: Improve SOA mechanisms for use in global models by incorporating constraints
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The Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) box model has been used under multiple environmental conditions to study the SOA formation and properties from typical hydrocarbon precursors and (ii) to fit a Volatility Basis Set (VBS) type parameterization, which can be used in 3D models. The set of parent hydrocarbons includes n-alkanes and 1-alkenes with 10, 14, 18, 22, and 26 carbon atoms, α-pinene, β-pinene and limonene, benzene, toluene, o-xylene, m-xylene and p-xylene. Isoprene chemistry was not considered as GECKO does not treat the aqueous phase formation, and a different approach has been adapted to develop a parameterization for isoprene SOA (see below). Its evaluation shows that VBS-GECKO captures the dynamic of SOA formation for a large range of conditions within 20% of the explicit simulations. This VBS-GECKO is however computationally very demanding, and we are currently working on a reduced version of it. A paper detailing these results is undergoing peer-review.
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A parameterization method has been developed to simulate the SOA formed from isoprene-derived epoxydiols (IEPOX-SOA). Our parameterization enables the fast calculation of IEPOX-SOA mass, maintaining accuracy compared to full chemistry simulation results. It uses the chemical environment (e.g., OH, HO2, and NO) and aerosol properties (e.g., pH and surface area), to estimate the yield of this chemistry at different locations. This results in much better accuracy compared to the constant 3% yield from isoprene emissions used in most global modeling studies. A paper detailing these findings is in preparation.
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We are applying a simpler box model and the fully explicit GECKO-A box model to simulate in detail the chemistry within the oxidation flow reactors (OFR), including that of oxidized nitrogen species, peroxy radicals, and volatile organic compounds. The results show reasonable correspondence to simulated chemistry in a typical chamber and in the ambient atmosphere under a subset of explored physical conditions, which have been identified. We are preparing two papers detailing our findings.
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A new VBS parametrization is being developed for monoterpene-derived SOA. We have taken into account as many constraints as possible, including constraints from field measurements. These include SOA yields at OA concentrations of ~1–10 μg m-3 measured in traditional chamber experiments, new SOA yields at very low OA concentrations (from extremely low volatility species, or ELVOCs), OA volatility quantified in aircraft measurements under small temperature changes, and OA evaporation at higher temperatures in thermal denuder (TD) experiments. With these constraints considered, the new parametrization would be suitable for modeling monoterpene-derived SOA formation more robustly across a range of conditions, in pristine regions (where only low-volatility species contribute to OA growth), in colder regions (e.g., the arctic or the upper free troposphere), and in a warming climate. Aging of OA is currently being considered to improve the agreement with the TD experiment results and the modeled TD experiments using this VBS parametrization. VBS parameterizations for anthropogenic-derived and biomass burning SOA will be developed in similar manner.
Objective 2: Implement the new mechanisms in a global model and simulate present conditions
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Our group is performing high-resolution OA measurements (with separate funding) on the NASA ATOM campaigns, which are sampling the remote free troposphere over the Pacific and Atlantic over 4 seasons. Results from the measurements are being extensively compared to results from different global models, including the CAM-Chem model. These comparisons are allowing the identification of model shortcomings (e.g., in vertical transport, OA heterogeneous oxidation rates, and other processes). This year the focus will shift from using the default parameterizations in each model to using the new parameterizations derived in this work.
Future Activities:
Work will continue along several lines:
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Finalize the publication of the GECKO-based VBS parameterizations
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Finalizing the IEPOX-SOA parameterization and publish a paper describing it.
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Completing OFR/chamber/ambient simulations comparing the radical chemistry regimes of each with GECKO-A and submitting the paper describing them.
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Collaborating with colleagues at NCAR to simulate ambient and OFR chemistry during the BEACHON and GOAmazon campaigns.
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Submitting the OFR peroxy radical chemistry paper and writing a review that comprehensively analyzes the atmospheric relevance of OFR chemistry.
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Completing the new SOA parametrization development by incorporating all available constraints and writing the paper describing this.
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Implementing the improved mechanisms into the chemistry component (CAM-Chem) of community earth system model (CESM) to investigate the performance of the model in simulating current OA data, such as from ATOM and other campaigns, with both the default and the improved parameterizations.
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Once a global model and parameterization configuration with satisfactory performance has been identified, simulations under future climate and emission scenarios will be performed to investigate the changes in concentrations, budgets and climate impacts of SOA when using more realistic SOA parameterizations.
Journal Articles on this Report : 24 Displayed | Download in RIS Format
Other project views: | All 53 publications | 53 publications in selected types | All 53 journal articles |
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Cappa CD, Jathar SH, Kleeman MJ, Docherty KS, Jimenez JL, Seinfeld JH, Wexler AS. Simulating secondary organic aerosol in a regional air quality model using the statistical oxidation model – Part 2: assessing the influence of vapor wall losses. Atmospheric Chemistry and Physics 2016;16(5):3041-3059. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Ciarelli G, Aksoyoglu S, Crippa M, Jimenez J-L, Nemitz E, Sellegri K, Aijala M, Carbone S, Mohr C, O'Dowd C, Poulain L, Baltensperger U, Prevot ASH. Evaluation of European air quality modelled by CAMx including the volatility basis set scheme. Atmospheric Chemistry and Physics 2016;16(16):10313-10332. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Gentner DR, Jathar SH, Gordon TD, Bahreini R, Day DA, El Haddad I, Hayes PL, Pieber SM, Platt SM, de Gouw J, Goldstein AH, Harley RA, Jimenez JL, Prevot ASH, Robinson AL. Review of urban secondary organic aerosol formation from gasoline and diesel motor vehicle emissions. Environmental Science & Technology 2017;51(3):1074-1093. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Hodzic A, Kasibhatla PS, Jo DS, Cappa CD, Jimenez JL, Madronich S, Park RJ. Rethinking the global secondary organic aerosol (SOA) budget:stronger production, faster removal, shorter lifetime. Atmospheric Chemistry and Physics 2016;16(12):7917-7941. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Kiendler-Scharr A, Mensah AA, Friese E, Topping D, Nemitz E, Prevot ASH, Aijala M, Allan J, Canonaco F, Canagaratna M, Carbone S, Crippa M, Dall Osto M, Day DA, De Carlo P, Di Marco CF, Elbern H, Eriksson A, Freney E, Hao L, Herrmann H, Hildebrandt L, Hillamo R, Jimenez JL, Laaksonen A, McFiggans G, Mohr C, O'Dowd C, Otjes R, Ovadnevaite J, Pandis SN, Poulain L, Schlag P, Sellegri K, Swietlicki E, Tiitta P, Vermeulen A, Wahner A, Worsnop D, Wu H-C. Ubiquity of organic nitrates from nighttime chemistry in the European submicron aerosol. Geophysical Research Letters 2016;43(14):7735-7744. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Ma PK, Zhao Y, Robinson AL, Worton DR, Goldstein AH, Ortega AM, Jimenez JL, Zotter P, Prevot ASH, Szidat S, Hayes PL. Evaluating the impact of new observational constraints on P-S/IVOC emissions, multi-generation oxidation, and chamber wall losses on SOA modeling for Los Angeles, CA. Atmospheric Chemistry and Physics 2017;17(15):9237-9259. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Maclean AM, Butenhoff CL, Grayson JW, Barsanti K, Jimenez JL, Bertram AK. Mixing times of organic molecules within secondary organic aerosol particles: a global planetary boundary layer perspective. Atmospheric Chemistry and Physics 2017;17(21):13037-13048. |
R835877 (2017) R835877 (2018) R835877 (2019) |
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Mao J, Carlton A, Cohen RC, Brune WH, Brown SS, Wolfe GM, Jimenez JL, Pye HOT, Ng, NL, Xu L, McNeill VF, Tsigaridis K, McDonald BC, Warneke C, Guenther A, Alvarado MJ, de Gouw J, Mickley LJ, Leibensperger EM, Mathur R, Nolte CG, Portmann RW, Unger N, Tosca M, Horowitz LW. Southeast Atmosphere Studies: learning from model-observation syntheses. Atmospheric Chemistry and Physics 2018;18(4):2615-2651. |
R835877 (2017) R835877 (2018) R835877 (2019) |
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McDuffie EE, Fibiger DL, Dube WP, Lopez‐Hilfiker F, Lee BH, Thornton JA, Shah V, Jaegle L, Guo H, Weber RJ,Reeves JM, Weinheimer AJ, Schroder JC, Campuzano-Jost P, Jimenez JL, Dibb JE, Veres P, Ebben C, Sparks TL, Woolridge PJ, Cohen RC, Hornbrook RS, Apel EC, Campos T, Hall SR, Ullman K, Brown SS. Heterogeneous N2 O5 uptake during winter: aircraft measurements during the 2015 WINTER campaign and critical evaluation of current parameterizations. Journal of Geophysical Research: Atmospheres 2018;123(8):4345-4372. |
R835877 (2017) R835877 (2018) R835877 (2019) |
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Murphy BN, Woody MC, Jimenez JL, Carlton AMG, Hayes PL, Liu S, Ng NL, Russell LM, Setyan A, Xu L, Young J, Zaveri RA, Zhang Q, Pye HOT. Semivolatile POA and parameterized total combustion SOA in CMAQv5.2: impacts on source strength and partitioning. Atmospheric Chemistry and Physics 2017;17(18):11107-11133. |
R835877 (2017) R835877 (2018) R835877 (2019) R835403 (Final) |
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Ng NL, Brown SS, Archibald AT, Atlas E, Cohen RC, Crowley JN, Day DA, Donahue NM, Fry JL, Fuchs H, Griffin RJ, Guzman MI, Herrmann H, Hodzic A, Iinuma Y, Jimenez JL, Kiendler-Scharr A, Lee BH, Luecken DJ, Mao J, McLaren R, Mutzel A, Osthoff HD, Ouyang B, Picquet-Varrault B, Platt U, Pye HOT, Rudich Y, Schwantes RH, Shiraiwa M, Stutz J, Thornton JA, Tilgner A, Williams BJ, Zaveri RA. Nitrate radicals and biogenic volatile organic compounds: oxidation, mechanisms, and organic aerosol. Atmospheric Chemistry and Physics 2017;17(3):2103-2162. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) R835403 (2015) R835403 (Final) |
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Nguyen TKV, Zhang Q, Jimenez JL, Pike M, Carlton AG. Liquid water: ubiquitous contributor to aerosol mass. Environmental Science & Technology Letters 2016;3(7):257-263. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) R835877 (Final) R835041 (Final) |
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Ortega AM, Hayes PL, Peng Z, Palm BB, Hu W, Day DA, Li R, Cubison MJ, Brune WH, Graus M, Warneke C, Gilman JB, Kuster WC, de Gouw J, Gutierrez-Montes C, Jimenez JL. Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area. Atmospheric Chemistry and Physics 2016;16(11):7411-7433. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Palm BB, Campuzano-Jost P, Ortega AM, Day DA, Kaser L, Jud W, Karl T, Hansel A, Hunter JF, Cross ES, Kroll JH, Peng Z, Brune WH, Jimenez JL. In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor. Atmospheric Chemistry and Physics 2016;16(5):2943-2970. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Palm BB, Campuzano-Jost P, Day DA, Ortega AM, Fry JL, Brown SS, Zarzana KJ, Dube W, Wagner NL, Draper DC, Kaser L, Jud W, Karl T, Hansel A, Gutierrez-Montes C, Jimenez JL. Secondary organic aerosol formation from in situ OH, O3 , and NO3 oxidation of ambient forest air in an oxidation flow reactor. Atmospheric Chemistry and Physics 2017;17(8):5331-5354. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Palm BB, de Sa SS, Day DA, Campuzano-Jost P, Hu W, Seco R, Sjostedt SJ, Park J-H, Guenther AB, Kim S, Brito J, Wurm F, Artaxo P, Thalman R, Wang J, Yee LD, Wernis R, Isaacman-VanWertz G, Goldstein AH, Liu Y, Springston SR, Souza R, Newburn MK, Alexander ML, Martin ST, Jimenez JL. Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia. Atmospheric Chemistry and Physics 2018;18(1):467-493. |
R835877 (2017) R835877 (2018) R835877 (2019) |
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Peng Z, Jimenez JL. Modeling of the chemistry in oxidation flow reactors with high initial NO. Atmospheric Chemistry and Physics 2017;17(19):11991-12010. |
R835877 (2017) R835877 (2018) R835877 (2019) |
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Peng Z, Palm BB, Day DA, Talukdar RK, Hu W, Lambe AT, Brune WH, Jimenez JL. Model evaluation of new techniques for maintaining high-NO conditions in oxidation flow reactors for the study of OH-initiated atmospheric chemistry. ACS Earth and Space Chemistry 2018;2(2):72-86. |
R835877 (2017) R835877 (2018) R835877 (2019) |
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Platt SM, El Haddad I, Pieber SM, Zardini AA, Suarez-Bertoa R, Clairotte M, Daellenbach KR, Huang RJ, Slowik JG, Hellebust S, Temime-Roussel B, Marchand N, de Gouw J, Jimenez JL, Hayes PL, Robinson AL, Baltensperger U, Astorga C, Prevot ASH. Gasoline cars produce more carbonaceous particulate matter than modern filter-equipped diesel cars. Scientific Reports 2017;7(1):4926 (9 pp.). |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Pye HOT, Murphy BN, Xu L, Ng NL, Carlton AG, Guo H, Weber R, Vasilakos P, Appel KW, Budisulistiorini SH, Surratt JD, Nenes A, Hu W, Jimenez JL, Isaacman-VanWertz G, Misztal PK, Goldstein AH. On the implications of aerosol liquid water and phase separation for organic aerosol mass. Atmospheric Chemistry & Physics 2017;17(1):343-369. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) R835403 (2015) R835403 (Final) R835404 (2015) R835404 (Final) R835407 (Final) R835410 (Final) R835412 (Final) |
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Reddington CL, Carslaw KS, Stier P, Schutgens N, Coe H, Liu D, Allan J, Browse J, Pringle KJ, Lee LA, Yoshioka M, Johnson JS, Regayre LA, Spracklen DV, Mann GW, Clarke A, Hermann M, Henning S, Wex H, Kristensen TB, Leaitch WR, Poeschl U, Rose D, Andreae MO, Schmale J, Kondo Y, Oshima N, Schwarz JP, Nenes A, Anderson B, Roberts GC, Snider JR, Leck C, Quinn PK, Chi X, Ding A, Jimenez JL, Zhang Q. The Global Aerosol Synthesis and Science Project (GASSP): measurements and modelling to reduce uncertainty. Bulletin of the American Meteorological Society 2017;98(9):1857-1877. |
R835877 (2017) R835877 (2018) R835877 (2019) R835877 (Final) |
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Stark H, Yatavelli RLN, Thompson SL, Kang H, Krechmer JE, Kimmel JR, Palm BB, Hu W, Hayes PL, Day DA, Campuzano-Jost P, Canagaratna MR, Jayne JT, Worsnop DR, Jimenez JL. Impact of thermal decomposition on thermal desorption instruments: advantage of thermogram analysis for quantifying volatility distributions of organic species. Environmental Science & Technology 2017;51(15):8491-8500. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Zhang X, Krechmer JE, Groessl M, Xu W, Graf S, Cubison M, Jayne JT, Jimenez JL, Worsnop DR, Canagaratna MR. A novel framework for molecular characterization of atmospherically relevant organic compounds based on collision cross section and mass-to-charge ratio. Atmospheric Chemistry and Physics 2016;16(20):12945-12959. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Zhang Y, Williams BJ, Goldstein AH, Docherty KS, Jimenez JL. A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG). Atmospheric Measurement Techniques 2016;9(11):5637-5653. |
R835877 (2016) R835877 (2017) R835877 (2018) R835877 (2019) |
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Supplemental Keywords:
Secondary organic aerosol, SOA, modeling, atmospheric chemistryProgress and Final Reports:
Original AbstractThe perspectives, information and conclusions conveyed in research project abstracts, progress reports, final reports, journal abstracts and journal publications convey the viewpoints of the principal investigator and may not represent the views and policies of ORD and EPA. Conclusions drawn by the principal investigators have not been reviewed by the Agency.