posted on 2024-02-21, 21:07authored byCarolyn Liu-Kang, Anna Sokolova, Yufeng Gong, William D. Fahy, Hui Peng, Jonathan P. D. Abbatt
Biomass
burning brown carbon (BrC) aerosol affects the climate
by absorbing light in the visible and UV wavelengths, with daytime
photochemistry changing its optical properties. Here, aging by UVB
irradiation of BrC in both the aqueous and particle states was conducted
to evaluate the conditions and mechanism required to change the ability
of BrC to absorb light with an emphasis on the role of radicals and
oxidation. Photoreactions enhanced visible light absorption with O2 present in both the aqueous phase and particulate states.
Deoxygenated samples did not show this enhancement, indicating the
importance of oxidation in this aging mechanism. Using furfuryl alcohol
as a singlet oxygen (1O2) scavenger, it was
shown that 1O2 contributes to roughly one third
of the visible absorption increase in the aqueous phase. Conversely,
hydroxyl radicals (OH) were demonstrated to have no impact. Carbon-centered
radicals, as measured by electron paramagnetic resonance in the particle
state, were formed when O2 was present but not for deoxygenated
irradiation. Overall, the dependence on O2 indicates that
highly viscous BrC particles, as will be present in the atmosphere
at low temperatures and/or low relative humidity, may not experience
the same degree of photochemical change as more liquid-like particles.