Black carbon simulations using a size- and mixing-state-resolved three-dimensional model: 1. Radiative effects and their uncertaintiesBlack carbon simulations using a size- and mixing-state-resolved three-dimensional model: 1. Radiative effects and their uncertainties
This study quantifies how uncertainties in the size distribution and mixing state parameters of black carbon (BC) emissions translate into the uncertainties in BC radiative effects by using a particle-size- and mixing-state-resolved three-dimensional model, the Weather Research and Forecasting model with chemistry (WRF-chem) with the Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS) and the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC). The WRF-chem/ATRAS-MOSAIC model can explicitly calculate BC processes in the atmosphere, such as BC aging due to condensation and coagulation and the resulting enhancement of absorption and cloud condensation nuclei activity, with 12 size and 10 BC mixing state bins (128 bins in total). Fifteen model simulations perturbing the emission parameters within their uncertainties are conducted over East Asia (spring 2009) to understand which parameters and processes are important and which are associated with the uncertainty in evaluating BC radiative effects. The simulations reveal a large variability (uncertainty) of BC optical and radiative variables over the East Asian region (the variability is 58–99%), which corresponds to ranges of BC radiative effect of 1.6–2.8 W m−2 at the top of the atmosphere and from −5.2 to −2.1 W m−2 at the surface over East Asia. BC optical and radiative variables are 3 to 5 times sensitive to the size and the mixing state in emissions than BC mass concentrations (the variability is 20%). The two main causes of the difference in sensitivity are the reduction of the variability of BC mass concentrations by coagulation and the enhancement of the variability of BC absorption by resolving BC mixing state. These complicated responses of aerosol processes can be calculated for the first time using a detailed aerosol model such as ATRAS. The results suggest that the following two points are important in the estimation of BC radiative effects: (1) reduction of the uncertainties in the aerosol size distribution and mixing state in emissions and (2) improvement of the representation of BC mixing state and absorption enhancement in aerosol models because most models do not treat them sufficiently.