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Title: Light absorption by brown carbon over the South-East Atlantic Ocean

Abstract

Biomass burning emissions often contain brown carbon (BrC), which represents a large family of light-absorbing organics that are chemically complex, thus making it difficult to estimate their absorption of incoming solar radiation, resulting in large uncertainties in the estimation of the global direct radiative effect of aerosols. Here we investigate the contribution of BrC to the total light absorption of biomass burning aerosols over the South-East Atlantic Ocean with different optical models, utilizing a suite of airborne measurements from the ORACLES 2018 campaign. An effective refractive index of black carbon (BC), meBC = 1.95 + ikeBC, that characterizes the absorptivity of all absorbing components at 660 nm wavelength was introduced to facilitate the attribution of absorption at shorter wavelengths, i.e. 470 nm. Most values of the imaginary part of the effective refractive index, keBC, were larger than those commonly used for BC from biomass burning emissions, suggesting contributions from absorbers besides BC at 660 nm. The TEM-EDX single-particle analysis further suggests that these long-wavelength absorbers might include iron oxides, as iron is found to be present only when large values of keBC are derived. Using this effective BC refractive index, we find that the contribution of BrC to the totalmore » absorption at 470 nm (RBrC,470) ranges from ~8 %–22 %, with the organic aerosol mass absorption coefficient (MACOA,470) at this wavelength ranging from 0.30±0.27 to 0.68±0.08 m2 g-1. The core–shell model yielded much higher estimates of MACOA,470 and RBrC,470 than homogeneous mixing models, underscoring the importance of model treatment. Absorption attribution using the Bruggeman mixing Mie model suggests a minor BrC contribution of 4 % at 530 nm, while its removal would triple the BrC contribution to the total absorption at 470 nm obtained using the AAE (absorption Ångström exponent) attribution method. Thus, it is recommended that the application of any optical properties-based attribution method use absorption coefficients at the longest possible wavelength to minimize the influence of BrC and to account for potential contributions from other absorbing materials.« less

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [5];  [6];  [7]; ORCiD logo [8];  [9]; ORCiD logo [10]
+ Show Author Affiliations
  1. Tel Aviv Univ., Tel Aviv (Israel)
  2. Tel Aviv Univ., Tel Aviv (Israel) ; Bay Area Environmental Research Institute, Moffett Field, Mountain View, CA (United States); NASA Ames Research Center (ARC), Moffett Field, Mountain View, CA (United States)
  3. Tel Aviv Univ., Tel Aviv (Israel)
  4. NASA Ames Research Center (ARC), Moffett Field, Mountain View, CA (United States); Oak Ridge Associated Universities, Oak Ridge, TN (United States)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
  6. Univ. of Miami, FL (United States)
  7. Mount Allison University, Sackville (Canada)
  8. Centre National de la Recherche Scientifique (CNRS) (France)
  9. Univ. of Hawaii at Manoa, Honolulu, HI (United States)
  10. Ecole Polytechnique Federale Lausanne (EPFL Switzerland); Foundation for Research & Technology-Hellas, Heraklion (Greece)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center; Brookhaven National Laboratory (BNL), Upton, NY (United States); Tel Aviv Univ. (Israel)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1878461
Alternate Identifier(s):
OSTI ID: 1868513; OSTI ID: 1958405
Report Number(s):
BNL-222992-2022-JAAM
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
SC0020084; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 22; Journal Issue: 14; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Brown Carbon, Optical properties, TEM, Mie scattering

Citation Formats

Zhang, Lu, Segal-Rozenhaimer, Michal, Che, Haochi, Dang, Caroline, Sedlacek III, Arthur J., Lewis, Ernie R., Dobracki, Amie, Wong, Jenny S., Formenti, Paola, Howell, Steven G., and Nenes, Athanasios. Light absorption by brown carbon over the South-East Atlantic Ocean. United States: N. p., 2022. Web. doi:10.5194/acp-22-9199-2022.
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Zhang, Lu, Segal-Rozenhaimer, Michal, Che, Haochi, Dang, Caroline, Sedlacek III, Arthur J., Lewis, Ernie R., Dobracki, Amie, Wong, Jenny S., Formenti, Paola, Howell, Steven G., & Nenes, Athanasios. Light absorption by brown carbon over the South-East Atlantic Ocean. United States. https://doi.org/10.5194/acp-22-9199-2022
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Zhang, Lu, Segal-Rozenhaimer, Michal, Che, Haochi, Dang, Caroline, Sedlacek III, Arthur J., Lewis, Ernie R., Dobracki, Amie, Wong, Jenny S., Formenti, Paola, Howell, Steven G., and Nenes, Athanasios. Mon . "Light absorption by brown carbon over the South-East Atlantic Ocean". United States. https://doi.org/10.5194/acp-22-9199-2022. https://www.osti.gov/servlets/purl/1878461.
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@article{osti_1878461,
title = {Light absorption by brown carbon over the South-East Atlantic Ocean},
author = {Zhang, Lu and Segal-Rozenhaimer, Michal and Che, Haochi and Dang, Caroline and Sedlacek III, Arthur J. and Lewis, Ernie R. and Dobracki, Amie and Wong, Jenny S. and Formenti, Paola and Howell, Steven G. and Nenes, Athanasios},
abstractNote = {Biomass burning emissions often contain brown carbon (BrC), which represents a large family of light-absorbing organics that are chemically complex, thus making it difficult to estimate their absorption of incoming solar radiation, resulting in large uncertainties in the estimation of the global direct radiative effect of aerosols. Here we investigate the contribution of BrC to the total light absorption of biomass burning aerosols over the South-East Atlantic Ocean with different optical models, utilizing a suite of airborne measurements from the ORACLES 2018 campaign. An effective refractive index of black carbon (BC), meBC = 1.95 + ikeBC, that characterizes the absorptivity of all absorbing components at 660 nm wavelength was introduced to facilitate the attribution of absorption at shorter wavelengths, i.e. 470 nm. Most values of the imaginary part of the effective refractive index, keBC, were larger than those commonly used for BC from biomass burning emissions, suggesting contributions from absorbers besides BC at 660 nm. The TEM-EDX single-particle analysis further suggests that these long-wavelength absorbers might include iron oxides, as iron is found to be present only when large values of keBC are derived. Using this effective BC refractive index, we find that the contribution of BrC to the total absorption at 470 nm (RBrC,470) ranges from ~8 %–22 %, with the organic aerosol mass absorption coefficient (MACOA,470) at this wavelength ranging from 0.30±0.27 to 0.68±0.08 m2 g-1. The core–shell model yielded much higher estimates of MACOA,470 and RBrC,470 than homogeneous mixing models, underscoring the importance of model treatment. Absorption attribution using the Bruggeman mixing Mie model suggests a minor BrC contribution of 4 % at 530 nm, while its removal would triple the BrC contribution to the total absorption at 470 nm obtained using the AAE (absorption Ångström exponent) attribution method. Thus, it is recommended that the application of any optical properties-based attribution method use absorption coefficients at the longest possible wavelength to minimize the influence of BrC and to account for potential contributions from other absorbing materials.},
doi = {10.5194/acp-22-9199-2022},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 14,
volume = 22,
place = {United States},
year = {Mon Jul 18 00:00:00 EDT 2022},
month = {Mon Jul 18 00:00:00 EDT 2022}
}
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    Works referencing / citing this record:

    Seasonal variations in fire conditions are important drivers in the trend of aerosol optical properties over the south-eastern Atlantic
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    • Che, Haochi; Segal-Rozenhaimer, Michal; Zhang, Lu
    • Atmospheric Chemistry and Physics, Vol. 22, Issue 13
    • DOI: 10.5194/acp-22-8767-2022
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