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Title: Deriving brown carbon from multiwavelength absorption measurements: Method and application to AERONET and Aethalometer observations

Abstract

The radiative impact of organic aerosols (OA) is a large source of uncertainty in estimating the global direct radiative effect (DRE) of aerosols. This radiative impact includes not only light scattering but also light absorption from a subclass of OA referred to as brown carbon (BrC). However, the absorption properties of BrC are poorly understood, leading to large uncertainties in modeling studies. To obtain observational constraints from measurements, a simple absorption Ångström exponent (AAE) method is often used to separate the contribution of BrC absorption from that of black carbon (BC). However, this attribution method is based on assumptions regarding the spectral dependence of BC that are often violated in the ambient atmosphere. Here we develop a new AAE method which improves upon previous approaches by using the information from the wavelength-dependent measurements themselves and by allowing for an atmospherically relevant range of BC properties, rather than fixing these at a single assumed value. We note that constraints on BC optical properties and mixing state would help further improve this method. We apply this method to multiwavelength absorption aerosol optical depth (AAOD) measurements at AERONET sites worldwide and surface aerosol absorption measurements at multiple ambient sites. We estimate that BrCmore » globally contributes up to 40 % of the seasonally averaged absorption at 440 nm. We find that the mass absorption coefficient of OA (OA-MAC) is positively correlated with the BC/OA mass ratio. Based on the variability in BC properties and BC/OA emission ratio, we estimate a range of 0.05–1.5 m2 g−1 for OA-MAC at 440 nm. Using the combination of AERONET and OMI UV absorption observations we estimate that the AAE388/440 nm for BrC is generally ~4 worldwide, with a smaller value in Europe (< 2). Our analyses of observations at two surface sites (Cape Cod, to the southeast of Boston, and the GoAmazon2014/5 T3 site, to the west of Manaus, Brazil) reveal no significant relationship between BrC absorptivity and photochemical aging in urban-influenced conditions. However, the absorption of BrC measured during the biomass burning season near Manaus is found to decrease with photochemical aging with a lifetime of ~1 day. This lifetime is comparable to previous observations within a biomass burning plume but much slower than estimated from laboratory studies. Given the large uncertainties associated with AERONET retrievals of AAOD, the most challenging aspect of our analysis is that an accurate, globally distributed, multiple-wavelength aerosol absorption measurement dataset is unavailable at present. Thus, achieving a better understanding of the properties, evolution, and impacts of global BrC will rely on the future deployment of accurate multiple-wavelength absorption measurements to which AAE methods, such as the approach developed here, can be applied.« less

Authors:
 [1];  [1];  [2];  [3];  [3];  [4];  [2];  [5];  [2];  [6]
+ Show Author Affiliations
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Harvard Univ., Cambridge, MA (United States)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  5. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  6. Univ. of Sao Paulo (Brazil)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC). Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1329806
Alternate Identifier(s):
OSTI ID: 1369212
Report Number(s):
BNL-112751-2016-JA; LA-UR-17-24402
Journal ID: ISSN 1680-7316; R&D Project: 2016-BNL-EE630EECA-Budg; KP1701000
Grant/Contract Number:  
SC00112704; AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics
Additional Journal Information:
Journal Volume: 16; Journal Issue: 19; Journal ID: ISSN 1680-7316
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Earth Sciences; aerosol, black carbon, brown carbon, angstrom exponent, ambient aerosol, mass absorption coefficient, absorbing aerosol, GoAmazon, Atmospheric Radiation Measurement Facility

Citation Formats

Wang, X., Heald, C. L., Sedlacek, A., de Sa, S. S., Martin, S. T., Alexander, M. L., Watson, T. B., Aiken, A. C., Springston, S. R., and Artaxo, P. Deriving brown carbon from multiwavelength absorption measurements: Method and application to AERONET and Aethalometer observations. United States: N. p., 2016. Web. doi:10.5194/acp-16-12733-2016.
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Wang, X., Heald, C. L., Sedlacek, A., de Sa, S. S., Martin, S. T., Alexander, M. L., Watson, T. B., Aiken, A. C., Springston, S. R., & Artaxo, P. Deriving brown carbon from multiwavelength absorption measurements: Method and application to AERONET and Aethalometer observations. United States. https://doi.org/10.5194/acp-16-12733-2016
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Wang, X., Heald, C. L., Sedlacek, A., de Sa, S. S., Martin, S. T., Alexander, M. L., Watson, T. B., Aiken, A. C., Springston, S. R., and Artaxo, P. Thu . "Deriving brown carbon from multiwavelength absorption measurements: Method and application to AERONET and Aethalometer observations". United States. https://doi.org/10.5194/acp-16-12733-2016. https://www.osti.gov/servlets/purl/1329806.
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@article{osti_1329806,
title = {Deriving brown carbon from multiwavelength absorption measurements: Method and application to AERONET and Aethalometer observations},
author = {Wang, X. and Heald, C. L. and Sedlacek, A. and de Sa, S. S. and Martin, S. T. and Alexander, M. L. and Watson, T. B. and Aiken, A. C. and Springston, S. R. and Artaxo, P.},
abstractNote = {The radiative impact of organic aerosols (OA) is a large source of uncertainty in estimating the global direct radiative effect (DRE) of aerosols. This radiative impact includes not only light scattering but also light absorption from a subclass of OA referred to as brown carbon (BrC). However, the absorption properties of BrC are poorly understood, leading to large uncertainties in modeling studies. To obtain observational constraints from measurements, a simple absorption Ångström exponent (AAE) method is often used to separate the contribution of BrC absorption from that of black carbon (BC). However, this attribution method is based on assumptions regarding the spectral dependence of BC that are often violated in the ambient atmosphere. Here we develop a new AAE method which improves upon previous approaches by using the information from the wavelength-dependent measurements themselves and by allowing for an atmospherically relevant range of BC properties, rather than fixing these at a single assumed value. We note that constraints on BC optical properties and mixing state would help further improve this method. We apply this method to multiwavelength absorption aerosol optical depth (AAOD) measurements at AERONET sites worldwide and surface aerosol absorption measurements at multiple ambient sites. We estimate that BrC globally contributes up to 40 % of the seasonally averaged absorption at 440 nm. We find that the mass absorption coefficient of OA (OA-MAC) is positively correlated with the BC/OA mass ratio. Based on the variability in BC properties and BC/OA emission ratio, we estimate a range of 0.05–1.5 m2 g−1 for OA-MAC at 440 nm. Using the combination of AERONET and OMI UV absorption observations we estimate that the AAE388/440 nm for BrC is generally ~4 worldwide, with a smaller value in Europe (< 2). Our analyses of observations at two surface sites (Cape Cod, to the southeast of Boston, and the GoAmazon2014/5 T3 site, to the west of Manaus, Brazil) reveal no significant relationship between BrC absorptivity and photochemical aging in urban-influenced conditions. However, the absorption of BrC measured during the biomass burning season near Manaus is found to decrease with photochemical aging with a lifetime of ~1 day. This lifetime is comparable to previous observations within a biomass burning plume but much slower than estimated from laboratory studies. Given the large uncertainties associated with AERONET retrievals of AAOD, the most challenging aspect of our analysis is that an accurate, globally distributed, multiple-wavelength aerosol absorption measurement dataset is unavailable at present. Thus, achieving a better understanding of the properties, evolution, and impacts of global BrC will rely on the future deployment of accurate multiple-wavelength absorption measurements to which AAE methods, such as the approach developed here, can be applied.},
doi = {10.5194/acp-16-12733-2016},
journal = {Atmospheric Chemistry and Physics},
number = 19,
volume = 16,
place = {United States},
year = {Thu Oct 13 00:00:00 EDT 2016},
month = {Thu Oct 13 00:00:00 EDT 2016}
}
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https://doi.org/10.5194/acp-16-12733-2016
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  • Atmospheric Chemistry and Physics Discussions, Vol. 15, Issue 21
  • DOI: 10.5194/acpd-15-30175-2015

Enhanced light absorption by mixed source black and brown carbon particles in UK winter
text, January 2015

Enhanced light absorption by mixed source black and brown carbon particles in UK winter
text, January 2015

  • Chhabra, Puneet S.; Cappa, Christopher D.; Brooks, William A.
  • Nature Publishing Group
  • DOI: 10.7892/boris.73275

Exploiting simultaneous observational constraints on mass and absorption to estimate the global direct radiative forcing of black carbon and brown carbon
journal, January 2014

  • Wang, X.; Heald, C. L.; Ridley, D. A.
  • Atmospheric Chemistry and Physics Discussions, Vol. 14, Issue 11
  • DOI: 10.5194/acpd-14-17527-2014
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    • DOI: 10.5194/acp-19-7973-2019

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    • Atmospheric Measurement Techniques Discussion
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    journal, January 2019

    • Curci, Gabriele; Alyuz, Ummugulsum; Barò, Rocio
    • Atmospheric Chemistry and Physics, Vol. 19, Issue 1
    • DOI: 10.5194/acp-19-181-2019
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