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

Abstract

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 inthemore » 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.« less

Authors:
ORCiD logo; ORCiD logo; ; ORCiD logo; ; ; ; ORCiD logo; ; ORCiD logo; ; ORCiD logo
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1462125
Alternate Identifier(s):
OSTI ID: 1491165; OSTI ID: 1524544
Report Number(s):
PNNL-SA-132487; BNL-211718-2019-JAAM
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
AC06-76RLO 1830; AC05-76RL01830; SC0012704
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 18 Journal Issue: 14; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES

Citation Formats

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, and Wang, Jian. Aircraft observations of the chemical composition and aging of aerosol in the Manaus urban plume during GoAmazon 2014/5. Germany: N. p., 2018. Web. doi:10.5194/acp-18-10773-2018.
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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. Aircraft observations of the chemical composition and aging of aerosol in the Manaus urban plume during GoAmazon 2014/5. Germany. https://doi.org/10.5194/acp-18-10773-2018
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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, and Wang, Jian. Mon . "Aircraft observations of the chemical composition and aging of aerosol in the Manaus urban plume during GoAmazon 2014/5". Germany. https://doi.org/10.5194/acp-18-10773-2018.
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@article{osti_1462125,
title = {Aircraft observations of the chemical composition and aging of aerosol in the Manaus urban plume during GoAmazon 2014/5},
author = {Shilling, John E. and Pekour, Mikhail S. and Fortner, Edward C. and Artaxo, Paulo and de Sá, Suzane and Hubbe, John M. and Longo, Karla M. and Machado, Luiz A. T. and Martin, Scot T. and Springston, Stephen R. and Tomlinson, Jason and Wang, Jian},
abstractNote = {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.},
doi = {10.5194/acp-18-10773-2018},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 14,
volume = 18,
place = {Germany},
year = {Mon Jul 30 00:00:00 EDT 2018},
month = {Mon Jul 30 00:00:00 EDT 2018}
}
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The Amazon Tall Tower Observatory (ATTO): overview of pilot measurements on ecosystem ecology, meteorology, trace gases, and aerosols
journal, January 2015

  • Andreae, M. O.; Acevedo, O. C.; Araùjo, A.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 18
  • DOI: 10.5194/acp-15-10723-2015

Hydrocarbon-like and oxygenated organic aerosols in Pittsburgh: insights into sources and processes of organic aerosols
journal, January 2005

  • Zhang, Q.; Worsnop, D. R.; Canagaratna, M. R.
  • Atmospheric Chemistry and Physics, Vol. 5, Issue 12
  • DOI: 10.5194/acp-5-3289-2005

O/C and OM/OC Ratios of Primary, Secondary, and Ambient Organic Aerosols with High-Resolution Time-of-Flight Aerosol Mass Spectrometry
journal, June 2008

  • Aiken, Allison C.; DeCarlo, Peter F.; Kroll, Jesse H.
  • Environmental Science & Technology, Vol. 42, Issue 12
  • DOI: 10.1021/es703009q

Composition and Sources of Particulate Matter Measured near Houston, TX: Anthropogenic-Biogenic Interactions
journal, May 2016

Emission factors of hydrocarbons, halocarbons, trace gases and particles from biomass burning in Brazil
journal, December 1998

  • Ferek, Ronald J.; Reid, Jeffrey S.; Hobbs, Peter V.
  • Journal of Geophysical Research: Atmospheres, Vol. 103, Issue D24
  • DOI: 10.1029/98JD00692

Evidence for a significant proportion of Secondary Organic Aerosol from isoprene above a maritime tropical forest
journal, January 2011

  • Robinson, N. H.; Hamilton, J. F.; Allan, J. D.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 3
  • DOI: 10.5194/acp-11-1039-2011

Chemical composition of summertime aerosol in the Po Valley (Italy), northern Adriatic and Black Sea
journal, July 2007

  • Crosier, J.; Allan, J. D.; Coe, H.
  • Quarterly Journal of the Royal Meteorological Society, Vol. 133, Issue S1
  • DOI: 10.1002/qj.88

Substantial convection and precipitation enhancements by ultrafine aerosol particles
journal, January 2018

Reactive intermediates revealed in secondary organic aerosol formation from isoprene
journal, December 2009

  • Surratt, J. D.; Chan, A. W. H.; Eddingsaas, N. C.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 15
  • DOI: 10.1073/pnas.0911114107

Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements
journal, January 2015

  • Hu, W. W.; Campuzano-Jost, P.; Palm, B. B.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 20
  • DOI: 10.5194/acp-15-11807-2015

Biogenic carbon and anthropogenic pollutants combine to form a cooling haze over the southeastern United States
journal, May 2009

  • Goldstein, A. H.; Koven, C. D.; Heald, C. L.
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 22
  • DOI: 10.1073/pnas.0904128106

Evolution of Organic Aerosols in the Atmosphere
journal, December 2009

Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data
journal, January 2009

  • Ulbrich, I. M.; Canagaratna, M. R.; Zhang, Q.
  • Atmospheric Chemistry and Physics, Vol. 9, Issue 9
  • DOI: 10.5194/acp-9-2891-2009

A technology-based global inventory of black and organic carbon emissions from combustion
journal, January 2004

Response of an aerosol mass spectrometer to organonitrates and organosulfates and implications for atmospheric chemistry
journal, March 2010

  • Farmer, D. K.; Matsunaga, A.; Docherty, K. S.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 15
  • DOI: 10.1073/pnas.0912340107

Overview of the South American biomass burning analysis (SAMBBA) field experiment
conference, January 2013

  • Morgan, W. T.; Allan, J. D.; Flynn, M.
  • NUCLEATION AND ATMOSPHERIC AEROSOLS: 19th International Conference, AIP Conference Proceedings
  • DOI: 10.1063/1.4803339

Evolution of trace gases and particles emitted by a chaparral fire in California
journal, January 2012

  • Akagi, S. K.; Craven, J. S.; Taylor, J. W.
  • Atmospheric Chemistry and Physics, Vol. 12, Issue 3
  • DOI: 10.5194/acp-12-1397-2012

Airborne observations of IEPOX-derived isoprene SOA in the Amazon during SAMBBA
journal, January 2014

  • Allan, J. D.; Morgan, W. T.; Darbyshire, E.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 20
  • DOI: 10.5194/acp-14-11393-2014

Budget of organic carbon in a polluted atmosphere: Results from the New England Air Quality Study in 2002
journal, January 2005

Isoprene Epoxydiols as Precursors to Secondary Organic Aerosol Formation: Acid-Catalyzed Reactive Uptake Studies with Authentic Compounds
journal, November 2011

  • Lin, Ying-Hsuan; Zhang, Zhenfa; Docherty, Kenneth S.
  • Environmental Science & Technology, Vol. 46, Issue 1
  • DOI: 10.1021/es202554c

Comparison of chemical characteristics of 495 biomass burning plumes intercepted by the NASA DC-8 aircraft during the ARCTAS/CARB-2008 field campaign
journal, January 2011

The time evolution of aerosol composition over the Mexico City plateau
journal, January 2008

  • Kleinman, L. I.; Springston, S. R.; Daum, P. H.
  • Atmospheric Chemistry and Physics, Vol. 8, Issue 6
  • DOI: 10.5194/acp-8-1559-2008

An overview of the Amazonian Aerosol Characterization Experiment 2008 (AMAZE-08)
journal, January 2010

  • Martin, S. T.; Andreae, M. O.; Althausen, D.
  • Atmospheric Chemistry and Physics, Vol. 10, Issue 23
  • DOI: 10.5194/acp-10-11415-2010

Effects of aging on organic aerosol from open biomass burning smoke in aircraft and laboratory studies
journal, January 2011

  • Cubison, M. J.; Ortega, A. M.; Hayes, P. L.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 23
  • DOI: 10.5194/acp-11-12049-2011

Atmospheric Degradation of Volatile Organic Compounds
journal, December 2003

  • Atkinson, Roger; Arey, Janet
  • Chemical Reviews, Vol. 103, Issue 12
  • DOI: 10.1021/cr0206420

Evolution of brown carbon in wildfire plumes
journal, June 2015

  • Forrister, Haviland; Liu, Jiumeng; Scheuer, Eric
  • Geophysical Research Letters, Vol. 42, Issue 11
  • DOI: 10.1002/2015GL063897

Estimates of global terrestrial isoprene emissions using MEGAN (Model of Emissions of Gases and Aerosols from Nature)
journal, January 2006

  • Guenther, A.; Karl, T.; Harley, P.
  • Atmospheric Chemistry and Physics, Vol. 6, Issue 11
  • DOI: 10.5194/acp-6-3181-2006

Evolution of submicron organic aerosol in polluted air exported from Tokyo
journal, January 2006

  • Takegawa, N.; Miyakawa, T.; Kondo, Y.
  • Geophysical Research Letters, Vol. 33, Issue 15
  • DOI: 10.1029/2006GL025815
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