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Climatic Effects of Black Carbon Aerosols over the Tibetan Plateau

Abstract

Black carbon (BC), also known as soot, has been identified as the second most important anthropogenic emissions in terms of global climate forcing in the current atmosphere. Ample evidence has shown that BC deposition is an important driver of rapid snow melting and glacier retreat over the Tibetan Plateau, which holds the largest snow/ice mass outside polar regions. However, the climatic effects of BC over the Tibetan Plateau have not been thoroughly investigated in such a manner as to understand, quantify, and reduce large uncertainties in the estimate of radiative and hydrological effects. Thus, this Ph.D. study seeks to understand and improve key processes controlling BC life cycle in global and regional models and to quantify BC radiative effects over the Tibetan Plateau. First, the capability of a state-of-the-art global chemical transport model (CTM), GEOS-Chem, and the associated model uncertainties are systematically evaluated in simulating BC over the Tibetan Plateau, using in situ measurements of BC in surface air, BC in snow, and BC absorption optical depth. The effects of three key factors on the simulation are also delineated, including Asian anthropogenic emissions, BC aging process, and model resolution. Subsequently, a microphysics-based BC aging scheme that accounts for condensation, coagulation, and heterogeneous chemical oxidation processes is developed and examined in GEOS-Chem by comparing with aircraft measurements. Compared to the default aging scheme, the microphysical scheme reduces model-observation discrepancies by a factor of ~3, particularly in the middle and upper troposphere. In addition, a theoretical BC aging-optics model is developed to account for three typical evolution stages, namely, freshly emitted aggregates, coated BC by soluble material, and BC particles undergoing further hygroscopic growth. The geometric-optics surface-wave (GOS) approach is employed to compute the BC single-scattering properties at each aging stage, which are subsequently compared with laboratory measurements. Results show large variations in BC optical properties caused by coating morphology and aging stages. Furthermore, a comprehensive intercomparison of the GOS approach, the superposition T-matrix method, and laboratory measurements is performed for optical properties of BC with complex structures during aging. Moreover, a new snow albedo model is developed for widely-observed close-packed snow grains internally mixed with BC. Results indicate that albedo simulations that account for snow close packing match closer to observations. Close packing enhances BC-induced snow albedo reduction and associated surface radiative forcing by up to 15% (20%) for fresh (old) snow, which suggests that BC-snow albedo forcing is underestimated in previous modeling studies without accounting for close packing. Finally, the snow albedo forcing and direct radiative forcing (DRF) of BC in the Tibetan Plateau are estimated using GEOS-Chem in conjunction with a stochastic snow model and a radiative transfer model. This, for the first time, accounts for realistic non-spherical snow grain shape and stochastic multiple inclusions of BC within snow in assessing BC-snow interactions. The annual mean BC snow albedo forcing is 2.9 W m-2 over snow-covered Plateau regions. BC-snow internal mixing increases the albedo forcing by 40-60% compared with external mixing, whereas Koch snowflakes reduce the forcing by 20-40% relative to spherical snow grains. BC DRF at the top of the atmosphere is 2.3 W m-2 with uncertainties of -70% - +85% in the Plateau. The BC forcings are further attributed to emissions from different regions.

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