Observations of sesquiterpenes and their oxidation products in central Amazonia during the wet and dry seasons

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dc.contributor.authorYee, Lindsay D.en
dc.contributor.authorIsaacman-VanWertz, Gabrielen
dc.contributor.authorWernis, Rebecca A.en
dc.contributor.authorMeng, Mengen
dc.contributor.authorRivera, Venturaen
dc.contributor.authorKreisberg, Nathan M.en
dc.contributor.authorHering, Susanne V.en
dc.contributor.authorBering, Mads S.en
dc.contributor.authorGlasius, Marianneen
dc.contributor.authorUpshur, Mary Aliceen
dc.contributor.authorBe, Ariana Grayen
dc.contributor.authorThomson, Regan J.en
dc.contributor.authorGeiger, Franz M.en
dc.contributor.authorOffenberg, John H.en
dc.contributor.authorLewandowski, Michaelen
dc.contributor.authorKourtchev, Ivanen
dc.contributor.authorKalberer, Markusen
dc.contributor.authorde Sa, Suzane S.en
dc.contributor.authorMartin, Scot T.en
dc.contributor.authorAlexander, M. Lizabethen
dc.contributor.authorPalm, Brett B.en
dc.contributor.authorHu, Weiweien
dc.contributor.authorCampuzano-Jost, Pedroen
dc.contributor.authorDay, Douglas A.en
dc.contributor.authorJimenez, Jose L.en
dc.contributor.authorLiu, Yingjunen
dc.contributor.authorMcKinney, Karena A.en
dc.contributor.authorArtaxo, Pauloen
dc.contributor.authorViegas, Juarezen
dc.contributor.authorManzi, Antonioen
dc.contributor.authorOliveira, Maria B.en
dc.contributor.authorde Souza, Rodrigoen
dc.contributor.authorMachado, Luiz A. T.en
dc.contributor.authorLongo, Karlaen
dc.contributor.authorGoldstein, Allen H.en
dc.contributor.departmentCivil and Environmental Engineeringen
dc.date.accessioned2019-11-21T14:35:33Zen
dc.date.available2019-11-21T14:35:33Zen
dc.date.issued2018-07-23en
dc.description.abstractBiogenic volatile organic compounds (BVOCs) from the Amazon forest region represent the largest source of organic carbon emissions to the atmosphere globally. These BVOC emissions dominantly consist of volatile and intermediate-volatility terpenoid compounds that undergo chemical transformations in the atmosphere to form oxygenated condensable gases and secondary organic aerosol (SOA). We collected quartz filter samples with 12 h time resolution and performed hourly in situ measurements with a semi-volatile thermal desorption aerosol gas chromatograph (SV-TAG) at a rural site ("T3") located to the west of the urban center of Manaus, Brazil as part of the Green Ocean Amazon (GoAmazon2014/5) field campaign to measure intermediate-volatility and semi-volatile BVOCs and their oxidation products during the wet and dry seasons. We speciated and quantified 30 sesquiterpenes and 4 diterpenes with mean concentrations in the range 0.01-6.04 ng m(-3) (1670 ppq(v)). We estimate that sesquiterpenes contribute approximately 14 and 12% to the total reactive loss of O-3 via reaction with isoprene or terpenes during the wet and dry seasons, respectively. This is reduced from similar to 50-70% for within-canopy reactive O-3 loss attributed to the ozonolysis of highly reactive sesquiterpenes (e.g., beta-caryophyllene) that are reacted away before reaching our measurement site. We further identify a suite of their oxidation products in the gas and particle phases and explore their role in biogenic SOA formation in the central Amazon region. Synthesized authentic standards were also used to quantify gas-and particle-phase oxidation products derived from beta-caryophyllene. Using tracer-based scaling methods for these products, we roughly estimate that sesquiterpene oxidation contributes at least 0.4-5% (median 1 %) of total submicron OA mass. However, this is likely a low-end estimate, as evidence for additional unaccounted sesquiterpenes and their oxidation products clearly exists. By comparing our field data to laboratory-based sesquiterpene oxidation experiments we confirm that more than 40 additional observed compounds produced through sesquiterpene oxidation are present in Amazonian SOA, warranting further efforts towards more complete quantification.en
dc.description.notesThe UC Berkeley team was supported for the GoAmazon2014/15 field campaign by NSF ACP grant no. 1332998 and for further analysis of the dataset by DOE ASR grant no. DE-SC0014040. The Northwestern University team was supported by the National Science Foundation (NSF) under grant no. CHE-1607640. The instrument as deployed was developed through support from the U.S. Department of Energy (DOE) SBIR grant DE-SC0004698. We gratefully acknowledge support from the Central Office of the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA), the Instituto Nacional de Pesquisas da Amazonia (INPA), the Universidade do Estado do Amazonia (UEA), and the local foundation FAPEAM. The work was conducted under 001030/2012-4 of the Brazilian National Council for Scientific and Technological Development (CNPq). We acknowledge logistical support from the Atmospheric Radiation Measurement (ARM) Climate Research Facility, a U.S. Department of Energy Office of Science user facility sponsored by the Office of Biological and Environmental Research. ARM-collected data, including ozone and meteorology, were obtained from MAOS. Lindsay D. Yee acknowledges support from a University of California Berkeley Chancellor's Postdoctoral Fellowship. Gabriel Isaacman-VanWertz acknowledges support from an NSF Graduate Research Fellowship (no. DGE 1106400). Brett B. Palm acknowledges support from a U. S. EPA STAR Graduate Fellowship (FP-91761701-0). The University of Colorado group acknowledges support from DOE (BER/ASR) DE-SC0016559 and EPA-STAR 83587701-0. Ariana Gray Be and Mary Alice Upshur gratefully acknowledge support from NSF Graduate Research Fellowships. Mary Alice Upshur also acknowledges an NSF GROW award, National Aeronautics and Space Administration Earth and Space (NASA ESS) Fellowship, and a P. E. O. Scholar Award. Franz M. Geiger gratefully acknowledges support from the Alexander von Humboldt Foundation.en
dc.description.sponsorshipNSF ACP grant [1332998]; DOE ASR grant [DE-SC0014040]; National Science Foundation (NSF)National Science Foundation (NSF) [CHE-1607640]; U.S. Department of Energy (DOE) SBIR grant [DE-SC0004698]; Central Office of the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA); Instituto Nacional de Pesquisas da Amazonia (INPA); Universidade do Estado do Amazonia (UEA); local foundation FAPEAM; Office of Biological and Environmental Research; University of California Berkeley Chancellor's Postdoctoral Fellowship; NSF Graduate Research FellowshipNational Science Foundation (NSF) [DGE 1106400]; U. S. EPA STAR Graduate FellowshipUnited States Environmental Protection Agency [FP-91761701-0]; DOE (BER/ASR)United States Department of Energy (DOE) [DE-SC0016559]; EPA-STARUnited States Environmental Protection Agency [83587701-0]; NSF Graduate Research FellowshipsNational Science Foundation (NSF); NSF GROW award; National Aeronautics and Space Administration Earth and Space (NASA ESS) Fellowship; Alexander von Humboldt FoundationAlexander von Humboldt Foundation; P. E. O. Scholar Awarden
dc.format.mimetypeapplication/pdfen
dc.identifier.doihttps://doi.org/10.5194/acp-18-10433-2018en
dc.identifier.eissn1680-7324en
dc.identifier.issn1680-7316en
dc.identifier.issue14en
dc.identifier.urihttp://hdl.handle.net/10919/95826en
dc.identifier.volume18en
dc.language.isoenen
dc.publisherEuropean Geophysical Unionen
dc.rightsCreative Commons Attribution 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/en
dc.titleObservations of sesquiterpenes and their oxidation products in central Amazonia during the wet and dry seasonsen
dc.title.serialAtmospheric Chemistry and Physicsen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten
dc.type.dcmitypeStillImageen

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