Impact of secondary and primary particulate matter (PM) sources on the enhanced light absorption by brown carbon (BrC) particles in central Los Angeles.

ABSTRACT

In this study, we investigated aerosol chemical composition, spectral properties of aerosol extracts, and source contributions to the aerosol light-absorbing brown carbon (BrC) in central Los Angeles from July 2018 to March 2019, during warm and cold seasons. Spectrophotometric measurements (water and methanol extracts; 200 < λ < 1100) and chemical analyses were performed on collected particulate matter (PM), and relationships of BrC light absorption (Abs365) to source tracer chemical species were evaluated. Mass absorption efficiency (MAE) of both water and methanol extracted solutions exhibited an increasing trend from warm period to cold season, with an annual average value of 0.61 ± 0.22 m2.g-1 and 1.38 ± 0.89 m2.g-1, respectively. Principal component analysis (PCA) were coupled with multiple linear regression (MLR) to identify and quantify sources of BrC light absorption in each of the seasons. Our finding documented fossil fuel combustion as the dominant source of BrC light absorption during warm season, with relative contribution of 38% to total BrC light absorption, followed by (secondary organic aerosol) SOA (30%) and biomass burning (12%). In contrast, biomass burning was the major source of BrC during the cold season (53%), while fossil fuel combustion and SOA contributed to 18% and 12% of BrC, respectively. Significantly higher contribution of biomass burning to BrC during the cold season suggested that residential heating activities (wood burning) play a major role in increased BrC concentrations. Previously collected Aethalometer model data documented fossil fuel combustion as the dominant contributing source to >90% of BC throughout the year. Finally, the solar radiation absorption ratio of BrC to elemental carbon (EC) in the ultraviolet range (300-400 nm) was maximum during the cold season with the annual corresponding values of 13-25% and 17-29% for water- and methanol-soluble BrC, respectively; which provides further evidence of the important effect of BrC light absorption on atmospheric radiative balance.