Non-reversible aging increases the solar absorptivity of African biomass
burning plumes
Abstract
Biomass-burning emissions impact almost all of the radiative forcing
terms considered by the IPCC, yet little is known about smoke aerosol
aging in nature beyond a few days. The marine southeast Atlantic
free-troposphere is a natural testbed for examining aging through
photolysis/oxidation of African continental fire emissions advected
westward. In-situ measurements primarily from September, 2016 indicate
highly-oxidized aerosol with minimal primary source signatures after 4-9
model-predicted days since emission. Aerosol loses approximately
one-half of its organic aerosol over the ocean. The organic aerosol to
black carbon mass ratios decrease from 14 to 10, significantly lower
than many model predictions. This mass loss, combined with stability in
black carbon, supports an observed 20% increase in solar absorptivity.
The decreased single scattering albedos, reaching 0.83 at 9 days,
arguably represent the lowest values measured globally. The relationship
of the aerosol properties to model-derived time since emission suggests
a useful new modeling constraint.