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Refractory black carbon (rBC) is a primary aerosol species, produced through incomplete combustion, that absorbs sunlight and contributes to positive radiative forcing. The overall climate effect of rBC depends on its spatial distribution and atmospheric lifetime, both of which are impacted by the efficiency with which rBC is transported or removed by convective systems. These processes are poorly constrained by observations. It is especially interesting to investigate rBC transport efficiency through the Asian Summer Monsoon (ASM) since this meteorological pattern delivers vast quantities of boundary layer air from Asia, where rBC emissions are high to the upper troposphere/lower stratosphere (UT/LS) where the lifetime of rBC is expected to be long. Here, we present in situ observations of rBC made during the Asian Summer Monsoon Chemistry and Climate Impact Project of summer, 2022. We use observed relationships between rBC and CO in ASM outflow to show that rBC is removed nearly completely (>98%) from uplifted air and that rBC concentrations in ASM outflow are statistically indistinguishable from the UT/LS background. We compare observed rBC and CO concentrations to those expected based on two chemical transport models and find that the models reproduce CO to within a factor of 2 at all altitudes whereas rBC is overpredicted by a factor of 20-100 at altitudes associated with ASM outflow. We find that the rBC particles in recently convected air have thinner coatings than those found in the UTLS background, suggesting transport of a small number of rBC particles that are negligible for concentration.

期刊论文 2025-02-16 DOI: 10.1029/2024JD042692 ISSN: 2169-897X

Black carbon (BC) is one important component contributing to global warming and its climate-related impacts strongly depend on mixing state. Previous observations at ground level indicated BC aging was at a fast rate in daytime with efficient photochemical reactions, while BC aging significantly weakened at night. Here we present evidences that BC aging still occurs efficiently at night in the residual layer (RL). The ratio of thickly coated refractory BC (rBC) in total rBC (f(BC)) increased from 51.3% at 00:00 LST to 61.5% at 07:00 LST at the CITIC station, which located in the RL at night, with an increasing rate of 1.4% per hour. Such an increasing rate was even higher than that during noontime (11:00 to 15:00 LST, 0.7% per hour). Similar trend also reflected in the coating thickness (Dp/Dc) of rBC particles, which increased from 1.52 at 00:00 LST to 1.63 at 07:00 LST. The aging of rBC in the RL at night enhances light absorption of rBC particles correspondingly; calculated absorption enhancement (E-abs) increased from 1.64 at 00:00 LST to 1.79 in at 07:00 LST. Further analysis indicated that the Eabs depends not only on the D-p/D-c of rBC particles, but also on its size. An increase in the size of rBC particles in polluted episode can also enhance the Eabs. Combined observations of development of boundary layer and pollutants at the CITIC station suggested that rBC particles were upwards transported in daytime and trapped in the RL at night, where they were aged efficiently. These results will improve our understanding on rBC aging in the atmosphere, and hence help to evaluate its radiative forcing.

期刊论文 2023-02-15 DOI: 10.1016/j.atmosenv.2022.119558 ISSN: 1352-2310
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