Atmospheric brown carbon (BrC) is an important constituent of light-absorbing organic aerosols with many unclear issues. Here, the light-absorption properties of BrC with different polarity characteristics at a regional site of Pearl River Delta Region during 2016-2017, influenced by sources and molecular compositions, were revealed using radiocarbon analysis and Fourier transform ion cyclotron resonance mass spectrometry. Humic-like substance (HULIS), middle polar (MP), and low polar (LP) carbon fractions constitute 46 +/- 17%, 30 +/- 7%, and 7 +/- 3% of total absorption coefficient from bulk extracts, respectively. Our results show that the absorption proportions of HULIS and MP to the total BrC absorption are higher than their mass proportions to organic carbon mass, indicating that HULIS and MP are the main light-absorbing components in water-soluble and water-insoluble organic carbon fractions, respectively. With decreases in non-fossil HULIS, MP, and LP carbon fractions (66 +/- 2%, 52 +/- 2%, and 36 +/- 3%, respectively), the abundances of unsaturated compounds and mass absorption efficiency at 365 nm of three fractions decreased synchronously. Increases in both nonfossil carbon and levoglucosan in winter imply that the enhanced light-absorption could be attributed to elevated levels of biomass burning organic aerosols (BBOA), which increases the number of light-absorbing nitrogencontaining compounds. Moreover, the major type of potential BrC in HULIS and MP carbon fractions are oxidized BBOA, but the potential BrC chromophores in LP are mainly associated with primary BBOA. This study reveals that biomass burning has adverse effects on radiative forcing and air quality, and probably indicates the significant influences of atmospheric oxidation reactions on the forms of chromophores.

Understanding of carbonaceous aerosols from different combustion sources and their optical properties are important to better understand atmospheric aerosol sources and estimate their radiative forcing. In this study, eight organic carbon (OC) and elemental carbon (EC) sub-fractions and light absorption properties of EC are investigated using thermal/optical method and compared among six typical solid and liquid fossil fuel combustion sources (e.g., coal combustion, industry, power plant, diesel and gasoline vehicle, and ship emissions) and within each source type, with consideration of different fuel types and combustion conditions. The results indicate that OC and EC sub-fraction distributions and mass absorption efficiency of EC (MAE(EC)) are sensitive and specific to sources, fuels, combustion and operating conditions. The differences in carbon fractions and AE(EC) between solid and fossil fuel source emissions are statistically significant (p < 0.05). The average MAE(EC) from liquid fossil fuel sources (7.9 +/- 3.5 m(2)/g) are around1.5-fold higher than those from solid fossil fuels (5.3 +/- 4.0 m(2)/g). Correlation analysis indicates that light attenuation of EC positively correlates with EC1 and EC2 fractions with correlation coefficients (r) around 0.6, while negatively correlates with the percentages of OC2 and OC3 in total carbon. Inter-comparisons of distributions of carbon sub-fractions and MAE(EC) from different coal samples indicate the tested new stoves and honeycomb-like shape may contribute to lower EC emission factors but with stronger light absorptivity of EC, suggesting curbing short-lived pollutants (e.g., EC) with improvement of coal stoves and clean coal at current stage might not always result in co-benefits of air quality and climate.