Transport of 222radon to the remote troposphere using the Model of Atmospheric Transport and Chemistry and assimilated winds from ECMWF and the National Center for Environmental Prediction/NCAR

Abstract

The Model of Atmospheric Transport and Chemistry (MATCH) is used to simulate the transport of 222Rn using both European Centre for Medium‐Range Weather Forecasts (ECMWF) winds and National Center for Environmental Prediction/National Center for Atmospheric Research (hereafter referred to as NCEP) reanalysis winds. These winds have the advantage of being based on observed winds but have the disadvantage that the subgrid‐scale transport processes are not routinely archived. MATCH derives subgrid‐scale mixing rates for the boundary layer using a nonlocal scheme and for moist convective mixing using one of two parameterizations (Tiedtke [1989] or Pan and Wu [1997]). This paper describes the ability of the model to recreate mixing rates of 222Rn using the forecast center winds. Radon 222 is a species with a continental crust source and a simple sink involving radioactive decay with an e‐folding timescale of 5.5 days. This atmospheric constituent is therefore a good tracer for testing the vertical transport in the chemical transport model, as well as the horizontal transport from continental regions to remote oceanic regions. The various simulations of 222Rn are compared with observations as well as with each other, allowing an estimate of the uncertainty in transport due to uncertainties in the winds and subgrid‐scale processes. The calculated vertical profiles over the western United States are somewhat similar to observed, and the upper tropospheric concentrations compare reasonably well in their spatial distribution with data collected during Tropospheric Ozone II (TROPOZ II), although the model values tend to be higher than observed values, especially in the upper troposphere. The model successfully simulates specific observed pollution events at Cape Grim. It has more difficulty at sites farther from continental source regions, although the model captures the seasonal structure of the pollution events at these sites (Macquarie Island, Amsterdam Island, Kerguelen Island, and Crozet Island). Inclusion of a moist convective mixing scheme in MATCH increases 222Rn concentrations in the upper troposphere by 50% compared to not having moist convective mixing, while surface concentrations do not appear to be very sensitive to moist convection. In addition, differences between the upper tropospheric concentrations of radon predicted using the ECMWF and NCEP winds can be 30% for large areas of the globe, due to either differences in the forecast center winds themselves or the moist convective mixing schemes used in conjunction with them. This has implications for model simulations of radiatively and chemically important trace species in the atmosphere.