2016 Progress Report: Rethinking the Formation of Secondary Organic Aerosols (SOA) Under Changing Climate by Incorporating Mechanistic and Field Constraints

EPA Grant Number: R835877
Title: Rethinking the Formation of Secondary Organic Aerosols (SOA) Under Changing Climate by Incorporating Mechanistic and Field Constraints
Investigators: Jimenez, Jose-Luis , Aumont, Bernard , Emmons, Louisa , Hodzic, Alma , 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
Project Period Covered by this Report: January 1, 2016 through December 31,2016
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

  • New SOA modules for global models have been developed using the Statistical Oxidation Model (SOM). The SOM is a semi-explicit model, which was fit to results from chamber experiments. This process allowed taking into account the effect of vapor wall losses on chamber experiments, which results in larger SOA yields, although the effects are quite sensitive to the precursor/oxidant combination. These results are documented in Hodzic et al. (2016).
  • Work is ongoing to develop a mechanism based on the fully explicit GECKO-A model. Base simulations have been generated and VBS fits have been performed for various levels of NOx. Once the final results are generated, this parameterization will be compared to the SOM-derived parameterization shown above.
  • We proposed to use emerging constraints from oxidation of ambient air in Oxidation Flow Reactors (OFRs). The interpretation of the OFR results, to allow evaluation of SOA models, has turned out to be quite complex. For this reason, we have invested a considerable amount of effort to clarify this interpretation, including the quantitative aspects: estimation of OH and NO3 exposures, lack of importance of irrelevant chemistry, quantification of SOA yields, and similarity between the detailed chemistry in the OFR vs. ambient air and laboratory chambers. These results are documented in several publications (Peng et al., AMT 2015; Peng et al., ACP 2016; Peng et al., 2017; Lee-Taylor et al., 2017).
  • An important property of SOA from a global model perspective is its volatility. Older models represented SOA as too volatile, which led to very large effects of temperature on SOA mass as the air moved to different atmospheric regions. For example, some models predicted large amounts of SOA in the upper free troposphere due to this effect, which are not present in the observations. We proposed to use the results of thermal denuder measurements to provide a constraint on the volatility of model SOA. However, there has been some controversy in the field about the realism of VBS determined from thermal denuder measurements. We have worked to clarify this issue, and submitted a paper where we show that TD measurements provide the most accurate representation of OA volatility among the methods currently available (Stark et al., 2017). Based on this information, we will use the TD results from multiple field campaigns to evaluate the volatility of the new VBS parameterizations discussed above.

Objective 2: Implement the new mechanisms in a global model and simulate present conditions

  • The new mechanisms based on SOM (and on GECKO for some precursors) already have been implemented in GEOS-Chem and evaluated against observations, as documented in Hodzic et al. (2016). The updated model presents a more dynamic picture of the life cycle of atmospheric SOA, with production rates 3.9 times higher and sinks a factor of 3.6 more efficient than in the base model. In particular, the updated model predicts larger SOA concentrations in the boundary layer and lower concentrations in the upper troposphere, leading to better agreement with surface and aircraft measurements of organic aerosol compared to the base model. Our analysis thus suggests that the long-standing discrepancy in model predictions of the vertical SOA distribution can now be resolved, at least in part, by a stronger source and stronger sinks leading to a shorter lifetime. The predicted global SOA burden in the updated model is 0.88 Tg and the corresponding direct radiative effect at top of the atmosphere is −0.33 W m-2, which is comparable to recent model estimates constrained by observations. The updated model predicts a population-weighted global mean surface SOA concentration that is a factor of 2 higher than in the base model, suggesting the need for a reanalysis of the contribution of SOA to PM pollution-related human health effects.
  • A great opportunity that was not known at the time of the proposal is the availability of the NASA Atmospheric Tomography (ATom) field campaign data. The Jimenez group and other experimental groups are participating in this series of four campaigns, where aerosols and gases are measured over the remote oceans with nearly pole-to-pole coverage. Four campaigns will be conducted over four different seasons. So far, two campaigns have been conducted with excellent results. These data provide an outstanding opportunity for evaluating parameterizations of SOA in global models, especially concerning the lifetime of SOA, which represents a major uncertainty for climate forcing. We have begun preliminary comparisons of model and measurement for aerosol chemical species and pH by season, altitude and region for the ATom-1 and 2 missions.

Future Activities:

Work will continue along several lines:

  • Completion of the evaluation of OFR chemistry and SOA production using the KinSim and GECKO-A models (Peng et al., 2017; Lee-Taylor et al., 2017).
  • Finalizing the parameterizations derived from GECKO-A, comparison with those derived with SOM.
  • Evaluation of SOA production and properties (composition and volatility) for the BEACHON-RoMBAS ambient and OFR cases (also GoAmazon and other cases, if time allows) against the GECKO-A model and the simplified parameterizations. This will allow improved confidence on the parameterizations to be used in the global models.
  • Performance of global model simulations with actual meteorology for improved evaluation of the CESM global model against the ATom-1 and 2 data (as well as other observations).
  • The goal of the items above is to converge towards one or a few SOA model versions to be tested for future climate and emission scenarios in year 3 of the project.
  • We are close to concluding a search for a postdoctoral researcher who will focus on global modeling and will perform the bulk of the work for proposal objectives 2 & 3.

References:

Hodzic, A., P.S. Kasibhatla, D.S. Jo, C. Cappa, J.L. Jimenez, S. Madronich, and R.J. Park. Rethinking the global secondary organic aerosol (SOA) budget: stronger production, faster removal, shorter lifetime. Atmospheric Chemistry and Physics, 16, 7917-7941, doi:10.5194/acp-16-7917-2016, 2016. http://www.atmos-chem-phys.net/16/7917/2016/acp-16-7917-2016.html Exit

Lee-Taylor, J.M., Z. Peng, B. Aumont, A. Hodzic, S. Madronich, and J.L. Jimenez. Comparing VOC oxidation patterns in oxidation flow reactors, environmental chambers, and ambient conditions, using the fully explicit chemical model GECKO-A. In preparation for ACPD.

Ortega, A. M., Hayes, P. L., Peng, Z., Palm, B. B., Hu, W., Day, D. A., Li, R., Cubison, M. J., Brune, W. H., Graus, M., Warneke, C., Gilman, J. B., Kuster, W. C., de Gouw, J., Gutiérrez-Montes, C., and Jimenez, J. L.: Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area, Atmos. Chem. Phys., 16, 7411-7433, doi:10.5194/acp-16-7411-2016, 2016. http://www.atmos-chem-phys.net/16/7411/2016/acp-16-7411-2016.html Exit

Palm, B. B., Campuzano-Jost, P., Day, D. A., Ortega, A. M., Fry, J. L., Brown, S. S., Zarzana, K. J., Dube, W., Wagner, N. L., Draper, D. C., Kaser, L., Jud, W., Karl, T., Hansel, A., Gutiérrez-Montes, C., and Jimenez, J. L.: Secondary organic aerosol formation from in situ OH, O3, and NO3 oxidation of ambient forest air in an oxidation flow reactor, Atmos. Chem. Phys. Discuss., doi:10.5194/acp-2016-1080, in review, 2017. http://www.atmos-chem-phys-discuss.net/acp-2016-1080/ Exit

Palm, B.B., P. Campuzano-Jost, A.M. Ortega, D.A. Day, L. Kaser, W. Jud, T. Karl, A. Hansel, J.F. Hunter, E.S. Cross, J.H. Kroll, A. Turnipseed, Z. Peng, W.H. Brune, and J.L. Jimenez. In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor. Atmospheric Chemistry and Physics, 16, 2943-2970, doi:10.5194/acp-16-2943-2016. http://www.atmos-chem-phys.net/16/2943/2016/acp-16-2943-2016.html Exit

Peng, Z., and J.L. Jimenez. Modeling of the chemistry in oxidation flow reactors with high initial NO. Atmos. Chem. Phys. Discuss., submitted, Mar. 2017.

Peng, Z., D.A. Day, A.M. Ortega, B.B. Palm, W. Hu, H. Stark, R. Li, K. Tsigaridis, W.H. Brune, and J.L. Jimenez. Non-OH chemistry in oxidation flow reactors for the study of atmospheric chemistry systematically examined by modeling Atmospheric Chemistry and Physics, 16, 4283-4305, doi:10.5194/acp-16-4283-2016, 2016.

Peng, Z., D.A. Day, H. Stark, R. Li, B.B. Palm, W.H. Brune, and J.L. Jimenez. HOx radical chemistry in oxidation flow reactors with low-pressure mercury lamps systematically examined by modeling. Atmospheric Measurement Techniques, 8, 4863-4890, doi:10.5194/amt-8-4863-2015, 2015.

Stark, H., R.L.N. Yatavelli, S.L. Thompson, H. Kang, J.E. Krechmer, J.R. Kimmel, B.B. Palm, W. Hu, P.L. Hayes, D.A. Day, P. Campuzano Jost, M.R. Canagaratna, J.T. Jayne, D.R. Worsnop, J.L. Jimenez. Impact of thermal decomposition on thermal desorption instruments: advantage of thermogram analysis for quantifying volatility distributions of organic species Environ. Sci. Technol., 51, 8491–8500, doi:10.1021/acs.est.7b00160, 2017.


Journal Articles on this Report : 16 Displayed | Download in RIS Format

Other project views: All 16 publications 16 publications in selected types All 16 journal articles
Type Citation Project Document Sources
Journal Article 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)
  • Full-text: ACP-Full Text PDF
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  • Abstract: ACP-Abstract
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  • Other: Harvard University-Abstract
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  • Journal Article 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)
  • Full-text: ACP-Full Text PDF
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  • Abstract: ACP-Abstract
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  • Other: Harvard University-Abstract
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  • Journal Article 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)
  • Abstract from PubMed
  • Full-text: University of California, Berkeley-Full Text PDF
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  • Abstract: ES&T-Abstract
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  • Other: ES&T-Full Text PDF
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  • Journal Article 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)
  • Full-text: ACP-Full Text PDF
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  • Abstract: ACP-Abstract
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  • Other: Harvard University-Abstract
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  • Journal Article 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)
  • Full-text: NERC-Abstract & Full Text PDF
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  • Abstract: Wiley-Abstract
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  • Other: Harvard University-Abstract
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  • Journal Article 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)
  • Full-text: ACP-Full Text PDF
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  • Abstract: ACP-Abstract
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  • Other: ResearchGate-Abstract & Full Text-PDF
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  • Journal Article 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)
    R835403 (2015)
    R835403 (Final)
  • Full-text: ACP-Full Text PDF
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  • Abstract: ACP-Abstract
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  • Other: University of Kentucky-Abstract & Full Text PDF
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  • Journal Article 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)
  • Full-text: ACS-Full Text PDF
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  • Abstract: ACS-Abstract
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  • Journal Article 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)
  • Full-text: ACP-Full Text PDF
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  • Abstract: ACP-Abstract
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  • Other: Harvard-Abstract
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  • Journal Article 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)
  • Full-text: ACCP-Full Text PDF
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  • Abstract: ACP-Abstract
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  • Other: Havard University-Abstract
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  • Journal Article 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)
  • Full-text: ACP-Full Text PDF
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  • Abstract: ACP-Abstract
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  • Other: OSTI-Abstract
  • Journal Article 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)
  • Full-text from PubMed
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  • Associated PubMed link
  • Full-text: Scientific Reports-Full Text HTML
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  • Abstract: Scientific Reports-Abstract
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  • Other: Scientific Reports-Full Text PDF
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  • Journal Article 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 and Physics 2017;17(1):343-369. R835877 (2016)
    R835403 (2015)
    R835403 (Final)
    R835404 (2015)
    R835404 (Final)
    R835407 (Final)
  • Full-text: ACP-Full Text PDF
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  • Abstract: ACP-Abstract
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  • Other: ResearchGate-Abstract & Full Text PDF
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  • Journal Article 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)
  • Abstract from PubMed
  • Full-text: ES&T-Full Text HTML
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  • Abstract: ES&T-Abstract
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  • Other: ES&T-Full Text PDF
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  • Journal Article 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)
  • Full-text: ACP-Full Text PDF
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  • Abstract: ACP-Abstract
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  • Other: Harvard University-Abstract
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  • Journal Article 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)
  • Full-text: AMT-Full Text PDF
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  • Abstract: AMT-Abstract
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  • Other: Harvard University-Abstract
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  • Supplemental Keywords:

    Secondary organic aerosol, SOA, modeling, atmosphere, climate

    Progress and Final Reports:

    Original Abstract