Quantitative Assessment of Parametric Uncertainty in Northern Hemisphere PAH Concentrations
We 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 techni...
| Main Authors: | , , , |
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| Format: | Article |
| Language: | en_US |
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American Chemical Society (ACS)
2016
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| Online Access: | http://hdl.handle.net/1721.1/103991 https://orcid.org/0000-0003-0439-3270 https://orcid.org/0000-0002-6396-5622 |
| _version_ | 1826202925037256704 |
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| author | Pike-Thackray, Colin Friedman, Carey Zhang, Yanxu Selin, Noelle E |
| author2 | Massachusetts Institute of Technology. Institute for Data, Systems, and Society |
| author_facet | Massachusetts Institute of Technology. Institute for Data, Systems, and Society Pike-Thackray, Colin Friedman, Carey Zhang, Yanxu Selin, Noelle E |
| author_sort | Pike-Thackray, Colin |
| collection | MIT |
| description | We 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. |
| first_indexed | 2024-09-23T12:25:40Z |
| format | Article |
| id | mit-1721.1/103991 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T12:25:40Z |
| publishDate | 2016 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1039912024-05-15T08:25:39Z Quantitative Assessment of Parametric Uncertainty in Northern Hemisphere PAH Concentrations Pike-Thackray, Colin Friedman, Carey Zhang, Yanxu Selin, Noelle E Massachusetts Institute of Technology. Institute for Data, Systems, and Society Massachusetts Institute of Technology. Center for Global Change Science Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences Pike-Thackray, Colin Friedman, Carey Selin, Noelle E. We 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. National Institutes of Health (U.S.) (NIH Postdoctoral Training Grant #5T32ES007020-39) National Science Foundation (U.S.) (Atmospheric Chemistry Program (#1053658) National Science Foundation (U.S.) (Arctic Natural Sciences Program (#1203526)) 2016-08-25T18:36:46Z 2016-08-25T18:36:46Z 2015-06 2015-06 Article http://purl.org/eprint/type/JournalArticle 0013-936X 1520-5851 http://hdl.handle.net/1721.1/103991 Thackray, 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. https://orcid.org/0000-0003-0439-3270 https://orcid.org/0000-0002-6396-5622 en_US http://dx.doi.org/10.1021/acs.est.5b01823 Environmental Science & Technology Article 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. application/pdf American Chemical Society (ACS) PMC |
| spellingShingle | Pike-Thackray, Colin Friedman, Carey Zhang, Yanxu Selin, Noelle E Quantitative Assessment of Parametric Uncertainty in Northern Hemisphere PAH Concentrations |
| title | Quantitative Assessment of Parametric Uncertainty in Northern Hemisphere PAH Concentrations |
| title_full | Quantitative Assessment of Parametric Uncertainty in Northern Hemisphere PAH Concentrations |
| title_fullStr | Quantitative Assessment of Parametric Uncertainty in Northern Hemisphere PAH Concentrations |
| title_full_unstemmed | Quantitative Assessment of Parametric Uncertainty in Northern Hemisphere PAH Concentrations |
| title_short | Quantitative Assessment of Parametric Uncertainty in Northern Hemisphere PAH Concentrations |
| title_sort | quantitative assessment of parametric uncertainty in northern hemisphere pah concentrations |
| url | http://hdl.handle.net/1721.1/103991 https://orcid.org/0000-0003-0439-3270 https://orcid.org/0000-0002-6396-5622 |
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