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dc.contributor.authorPike-Thackray, Colin
dc.contributor.authorFriedman, Carey
dc.contributor.authorZhang, Yanxu
dc.contributor.authorSelin, Noelle E.
dc.date.accessioned2016-08-25T18:36:46Z
dc.date.available2016-08-25T18:36:46Z
dc.date.issued2015-06
dc.date.submitted2015-06
dc.identifier.issn0013-936X
dc.identifier.issn1520-5851
dc.identifier.urihttp://hdl.handle.net/1721.1/103991
dc.description.abstractWe quantitatively examine the relative importance of uncertainty in emissions and physicochemical properties (including reaction rate constants) to Northern Hemisphere (NH) and Arctic polycyclic aromatic hydrocarbon (PAH) concentrations, using a computationally efficient numerical uncertainty technique applied to the global-scale chemical transport model GEOS-Chem. Using polynomial chaos (PC) methods, we propagate uncertainties in physicochemical properties and emissions for the PAHs benzo[a]pyrene, pyrene and phenanthrene to simulated spatially resolved concentration uncertainties. We find that the leading contributors to parametric uncertainty in simulated concentrations are the black carbon-air partition coefficient and oxidation rate constant for benzo[a]pyrene, and the oxidation rate constants for phenanthrene and pyrene. NH geometric average concentrations are more sensitive to uncertainty in the atmospheric lifetime than to emissions rate. We use the PC expansions and measurement data to constrain parameter uncertainty distributions to observations. This narrows a priori parameter uncertainty distributions for phenanthrene and pyrene, and leads to higher values for OH oxidation rate constants and lower values for European PHE emission rates.en_US
dc.description.sponsorshipNational Institutes of Health (U.S.) (NIH Postdoctoral Training Grant #5T32ES007020-39)en_US
dc.description.sponsorshipNational Science Foundation (U.S.) (Atmospheric Chemistry Program (#1053658)en_US
dc.description.sponsorshipNational Science Foundation (U.S.) (Arctic Natural Sciences Program (#1203526))en_US
dc.language.isoen_US
dc.publisherAmerican Chemical Society (ACS)en_US
dc.relation.isversionofhttp://dx.doi.org/10.1021/acs.est.5b01823en_US
dc.rightsArticle is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.en_US
dc.sourcePMCen_US
dc.titleQuantitative Assessment of Parametric Uncertainty in Northern Hemisphere PAH Concentrationsen_US
dc.typeArticleen_US
dc.identifier.citationThackray, Colin P., Carey L. Friedman, Yanxu Zhang, and Noelle E. Selin. “Quantitative Assessment of Parametric Uncertainty in Northern Hemisphere PAH Concentrations.” Environ. Sci. Technol. 49, no. 15 (August 4, 2015): 9185–9193.en_US
dc.contributor.departmentMIT Institute for Data, Systems, and Societyen_US
dc.contributor.departmentMassachusetts Institute of Technology. Center for Global Change Scienceen_US
dc.contributor.departmentMassachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciencesen_US
dc.contributor.mitauthorPike-Thackray, Colinen_US
dc.contributor.mitauthorFriedman, Careyen_US
dc.contributor.mitauthorSelin, Noelle E.en_US
dc.relation.journalEnvironmental Science & Technologyen_US
dc.eprint.versionAuthor's final manuscripten_US
dc.type.urihttp://purl.org/eprint/type/JournalArticleen_US
eprint.statushttp://purl.org/eprint/status/PeerRevieweden_US
dspace.embargo.termsNen_US
dc.identifier.orcidhttps://orcid.org/0000-0003-0439-3270
dc.identifier.orcidhttps://orcid.org/0000-0002-6396-5622
mit.licensePUBLISHER_POLICYen_US


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