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.

Black carbon (BC), the byproduct of incomplete combustion, is considered to be the second most important anthropogenic climate forcing agent after carbon dioxide. BC warms the atmosphere by absorbing solar radiation (direct effect), alters cloud and precipitation formation by acting as cloud condensation nuclei (indirect effect), and modifies cloud distribution via cloud burn-off (semi-direct effect).

Currently, there are large discrepancies in general circulation model estimates of the influence of BC on precipitation. Even less known is how BC changes precipitation on regional scales. In the drought-stricken western United States (WUS), where BC emissions are known to affect the hydrological cycle, an investigation on how BC influences precipitation is warranted.

In this study, we employ the Weather Research and Forecasting-Chemistry (WRF Chem) model (version 3.6.0) with the newly chemistry- and microphysics-coupled Fu-Liou-Gu radiation scheme to study how black carbon affects precipitation by separating BC-related effects into direct and semi-direct, and indirect effects. In this three-part study, we use a recent wet year (2005) to investigate black carbon effects. We first examine BC effects during a heavy wintertime heavy precipitation event (7-11 January 2005), a heavy summertime precipitation week for comparison to the wintertime event (20-24 July 2005), and finally, examine these same effects for the months of January to June 2005 to investigate month-long trends.

We find that BC suppresses precipitation, predominantly through its direct and semi-direct effects. The direct and semi-direct effects warm the air aloft, and cool the lower levels of the atmosphere (surface dimming) through the reduction of downward shortwave radiation flux at the surface. These changes in vertical temperature increase the stability of the atmosphere and reduce convective precipitation. Convective precipitation reduction accounts for approximately 60 75% of the total precipitation reduction. Additionally, cooling in the lower levels reduces evaporation from the surface, which reduces the moisture needed for non-convective precipitation. Subsequently, reduced moisture in the atmosphere suppresses non-convective precipitation by approximately 10-40%. The indirect effects also reduce precipitation, but to a much smaller extent of 5-20%.

Although we use an atypical BC emission dataset is used in this study, the resulting reduction of the different types of precipitation sheds light on the physical mechanisms of BC-cloud-radiation interactions by which the reductions follow. In particular, our results highlight the importance of the cumulus and surface layer parameterizations that house the triggering mechanism and surface moisture flux parameterizations in future studies.

In this research we find the NEI 2005 emissions did not significantly change precipitation. This is likely due to the aggressive emission regulations that exist for the United States. Emission regulations, however, do not exist or are enforced equally across the globe. In the developing countries that rely on inefficient cook stoves and heating systems, the populations suffer the most due to black carbon emission. Along with respiratory and cardiovascular impacts from black carbon, they may suffer from reduced water resources from suppressed precipitation, as well. In a larger sense, findings from this research serve as a platform for understanding the wider-reaching effects of black carbon on regional precipitation and drought. In particular, in areas where there are no black carbon emission regulations, this would highlight health and potentially significant environmental benefits that could be achieved from a black carbon cap and trade.