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 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.