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

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Lindsay D. Yee1, Gabriel Isaacman‐VanWertz1,2, Rebecca A. Wernis3, Meng Meng4,5, Ventura Rivera4, Nathan M. Kreisberg6, Susanne V. Hering6, Mads S. Bering7, Marianne Glasius7, Mary Alice Upshur8, Ariana Gray Bé8, Regan J. Thomson8, Franz M. Geiger8, John H. Offenberg9, Michael Lewandowski9, Ivan Kourtchev10, Markus Kalberer10, Suzane de Sá11, Scot T. Martin12,11, M. Lizabeth Alexander13, Brett B. Palm14, Weiwei Hu14, Pedro Campuzano‐Jost14, D. A. Day14, J. L. Jiménez14, Yingjun Liu11,15, K. A. McKinney11,16, Paulo Artaxo17, Gunilla Svensson18, Antônio O. Manzi18, Maria Betânia Leal de Oliveira19, Rodrigo Augusto Ferreira De Souza19, Luiz A. T. Machado20, K. Longo21, A. H. Goldstein1
1Department of Environmental Science, Policy and Management, University of California Berkeley, Berkeley, California, 94720, USA
2now at: Department of Civil and Environmental Engineering, Virginia Tech, Blacksburg, Virginia 24061, USA
3Department of Civil and Environmental Engineering, University of California, Berkeley, Berkeley, California 94720, USA
4Department of Chemical Engineering, University of California, Berkeley, Berkeley, California, 94720, USA
5now at: Department of Chemical Engineering and Applied Chemistry, University of Toronto, Toronto, CA, USA
6Aerosol Dynamics Inc., Berkeley, California 94710, USA
7Department of Chemistry, Aarhus University, 8000 Aarhus C, Denmark
8Department of Chemistry, Northwestern University, Evanston, Illinois 60208, USA
9National Exposure Research Laboratory, Exposure Methods and Measurements Division, United States Environmental Protection Agency, Research Triangle Park, North Carolina 27711, USA
10Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
11School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, USA
12Department of Earth and Planetary Sciences, Harvard University, Cambridge, Massachusetts 02138 USA
13Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99352 USA
14Dept. of Chemistry and Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, Colorado 80309, USA
15now at: Department of Environmental Science, Policy, and Management, University of California, Berkeley, Berkeley, California 94720, USA
16now at: Department of Chemistry, Colby College, Waterville, Maine 04901, USA
17Department of Applied Physics, University of São Paulo, SP, Brazil
18Instituto Nacional de Pesquisas da Amazonia, Manaus, AM, Brazil
19Universidade do Estado do Amazonas, Manaus, AM, Brazil
20Instituto Nacional de Pesquisas Espiacais, São José dos Campos, SP, Brazil
21Instituto Nacional de Pesquisas Espiacais, Cachoeira Paulista, SP, Brazil

Tóm tắt

Abstract. Biogenic 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 (1–670 ppqv). We estimate that sesquiterpenes contribute approximately 14 and 12 % to the total reactive loss of O3 via reaction with isoprene or terpenes during the wet and dry seasons, respectively. This is reduced from  ∼  50–70 % for within-canopy reactive O3 loss attributed to the ozonolysis of highly reactive sesquiterpenes (e.g., β-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 β-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.

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