Aircraft observations of the chemical composition and aging of aerosol in the Manaus urban plume during GoAmazon 2014/5

Shilling, John E.; Pekour, Mikhail S.; Fortner, Edward C.; Artaxo, Paulo; de Sá, Suzane; Hubbe, John M.; Longo, Karla M.; Machado, Luiz A. T.; Martin, Scot T.; Springston, Stephen R.; Tomlinson, Jason; Wang, Jian

doi:10.5194/acp-18-10773-2018

Title: Aircraft observations of the chemical composition and aging of aerosol in the Manaus urban plume during GoAmazon 2014/5

Journal Article · Mon Jul 30 00:00:00 EDT 2018 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-18-10773-2018· OSTI ID:1462125

;

; Fortner, Edward C.;

; de Sá, Suzane; Hubbe, John M.; Longo, Karla M.;

; Martin, Scot T.;

; Tomlinson, Jason;

Abstract. The Green Ocean Amazon (GoAmazon 2014/5) campaign, conducted fromJanuary 2014 to December 2015 in the vicinity of Manaus, Brazil, was designedto study the aerosol life cycle and aerosol–cloud interactions in bothpristine and anthropogenically influenced conditions. As part of thiscampaign, the U.S. Department of Energy (DOE) Gulfstream 1 (G-1) research aircraft wasdeployed from 17 February to 25 March 2014 (wet season) and 6 September to5 October 2014 (dry season) to investigate aerosol and cloud propertiesaloft. Here, we present results from the G-1 deployments focusing onmeasurements of the aerosol chemical composition and secondary organicaerosol (SOA) formation and aging. In the first portion of the paper, we provide an overview of the dataand compare and contrast the data from the wet and dry season. Organic aerosol (OA) dominates the deployment-averaged chemical composition,comprising 80% of the non-refractory PM₁ aerosol mass, with sulfatecomprising 14%, nitrate 2%, and ammonium 4%. This productdistribution was unchanged between seasons, despite the fact that totalaerosol loading was significantly higher in the dry season and that regionaland local biomass burning was a significant source of OA mass in the dry,but not wet, season. However, the OA was more oxidized in the dry season,with the median of the mean carbon oxidation state increasing from -0.45 inthe wet season to -0.02 in the dry season. In the second portion of the paper, we discuss the evolution of theManaus plume, focusing on 13 March 2014, one of the exemplary days in thewet season. On this flight, we observe a clear increase in OA concentrationsin the Manaus plume relative to the background. As the plume is transporteddownwind and ages, we observe dynamic changes in the OA. The mean carbonoxidation state of the OA increases from -0.6 to -0.45 during the 4–5hof photochemical aging. Hydrocarbon-like organic aerosol (HOA) mass is lost,with ΔHOA/ΔCO valuesdecreasing from 17.6µgm^-3ppmv^-1 over Manaus to 10.6µgm^-3ppmv^-1 95km downwind.Loss of HOA is balanced out by formation of oxygenated organic aerosol (OOA),with ΔOOA/ΔCO increasing from 9.2 to 23.1µgm^-3ppmv^-1.Because hydrocarbon-like organic aerosol (HOA) loss is balanced by OOA formation, we observelittle change in the net Δorg/ΔCO values;Δorg/ΔCO averages 31µgm^-3ppmv^-1 and does notincrease with aging. Analysis of the Manaus plume evolution using data fromtwo additional flights in the wet season showed similar trends in Δorg/ΔCOto the 13 March flight; Δorg/ΔCO valuesaveraged 34µgm^-3ppmv^-1 and showed little change over4–6.5h of aging. Our observation of constant Δorg/ΔCOare in contrast to literature studies of the outflow of several NorthAmerican cities, which report significant increases inΔorg/ΔCO for the first day of plume aging. These observations suggest that SOAformation in the Manaus plume occurs, at least in part, by a differentmechanism than observed in urban outflow plumes in most other literaturestudies. Constant Δorg/ΔCO with plume aging has beenobserved in many biomass burning plumes, but we are unaware of reports offresh urban emissions aging in this manner. These observations show thaturban pollution emitted from Manaus in the wet season forms less particulatedownwind as it ages than urban pollution emitted from North American cities.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC06-76RLO 1830; AC05-76RL01830; SC0012704

OSTI ID:: 1462125

Alternate ID(s):: OSTI ID: 1491165; OSTI ID: 1524544

Report Number(s):: PNNL-SA-132487; BNL-211718-2019-JAAM

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Vol. 18 Journal Issue: 14; ISSN 1680-7324

Publisher:: Copernicus Publications, EGUCopyright Statement

Country of Publication:: Germany

Language:: English

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Cited by: 28 works

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