Modeling Investigation of Brown Carbon Aerosol and Its Light Absorption in China

Brown carbon (BrC) is a type of organic carbon with light-absorbing abilities, especially in ultraviolet (UV) radiation, which could significantly contribute to global warming. Observations have shown high BrC concentrations and absorption in China, suggesting potentially large BrC emissions. The potential contribution of fossil fuel combustion to BrC emission has been ignored in most previous studies. Here, we use GEOS-Chem to simulate BrC distribution and absorption in China, accounting for three major primary BrC sources: residential coal and biofuel combustion, vehicle exhausts, and open biomass burning. Based on the literature and related energy consumption data, we estimate the specific emission ratio of BrC versus BC, and BrC mass absorption efficiency (MAE) for each source. Combined with BC emission, total BrC emission in China is then estimated to be 3.42 Tg yr(-1) in 2018, of which 71% is from residential combustion, 14% is from vehicle exhaust, and 15% is from open biomass burning. Residential combustion is the main source of surface BrC in China, accounting for 60% on average, followed by open biomass burning (23%) and vehicle exhaust emissions (17%). There is a clear seasonality in surface BrC concentrations with the maximum in winter (5.1 mu g m(-3)), followed by spring (2.8 mu g m(-3)), autumn (2.3 mu g m(-3)), and summer (1.3 mu g m(-3)). BrC AAOD at 365 nm ranges from 0.0017 to 0.060 in China, mainly dominated by residential combustion (73%), followed by open biomass burning (16%), and vehicle exhaust emissions (11%). It is also estimated that BrC accounts for 45-67% (52% on average) of total carbonaceous aerosol AAOD at 365 nm, implying an equal importance of BrC and BC regarding the absorption in UV radiation.