Modelling Cloud Processing of Gases and Particles In Urban-industrial Plumes: Comparison of Several Meso-scale Aerosol Forecasting Models

Abstract

Clouds play an active role in the processing and cycling of chemicals in the atmosphere. Particularly, it is known that a large portion of the atmospheric particulate sulphate, which contributes to a significant fraction of the total PM mass, is produced in cloud via aqueous-phase oxidation. As a result, most of the current aerosol forecast models do include the representation of in-cloud oxidation. On the other hand, the modelling of cloud processing of gases and aerosols and its evaluation are challenging. Past studies have shown that the modeled cloud processing of gases and aerosols depends critically on the predicted cloud microphysics fields. Furthermore, observations suited for evaluating cloud chemistry in models are extremely limited, and there is also the issue with scale disparity (both temporal and spatial) between the model resolution and the observation. This study examines model simulations from three different regional/meso-scale aerosol models, WRF-CHEM (NOAA/ESRL), MESO-NHC (LA/CNRS), and AURAMS (EC), with a focus on cloud processing of urban-industrial plumes. The study case is based on airborne measurements from two flights during the ICARTT field campaign in summer 2004, when the National Research Council of Canada Convair 580 sampled in and below stratocumulus downwind of Chicago along each of the 84°W and 86°W meridians between 40.5 and 42.6°N. The Chicago urban plume was encountered along both meridians, and the observations indicate cloud processing. Model simulations of cloud microphysics, trace gases and aerosol particle concentrations are compared with aircraft observations. Uncertainties in model predicted gases and aerosol concentrations due to model resolution, microphysics and aqueous-phase chemistry parameterization will be assessed.