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

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 modelling 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 method that decreases the uncertainties associated with estimating BrC absorption. By applying this method to multi-wavelength 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 6-40% of the absorption at 440nm. We find that the mass absorption coefficient of OA (OA-MAC) is positively correlated with BC/OA mass ratio. Based on the variability of BC properties and BC/OA emission ratio, we estimate a range of 0.05-1.2 m2/gmore » for OA-MAC at 440nm. Using the combination of AERONET and OMI UV absorption observations we estimate that the AAE388/440nm for BrC is generally ~4 world-wide, with a smaller value in Europe (< 2). Our analyses of 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 typical 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.« less
Authors:
 [1] ;  [1] ;  [2] ;  [3] ;  [3] ;  [4] ;  [2] ;  [5] ;  [2] ;  [6]
  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:
OSTI Identifier:
1329806
Report Number(s):
BNL--112751-2016-JA
Journal ID: ISSN 1680-7316; R&D Project: 2016-BNL-EE630EECA-Budg; KP1701000
Grant/Contract Number:
SC00112704
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
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES