Exploring the sensitivity of atmospheric nitrate concentrations to nitric acid uptake rate using the Met Office's Unified Model

Abstract

Ammonium nitrate is a major aerosol constituent over many land regions and contributes to air pollution episodes, ecosystem destruction, regional haze, and aerosol-induced climate forcing. Many climate models that represent ammonium nitrate assume that the ammonium-sulfate-nitrate chemistry reaches thermodynamic equilibrium instantaneously without considering kinetic limitations on condensation rates. The Met Office's Unified Model (UM) is employed to investigate the sensitivity of ammonium nitrate concentrations to the nitric acid uptake coefficient (γ) in a newly developed nitrate scheme in which first-order condensation theory is utilised to limit the rate at which thermodynamic equilibrium is attained. Two values of γ representing fast (γCombining double low line0.193) and slow (γCombining double low line0.001) uptake rates are tested in 20-year global UM integrations. The global burden of nitrate associated with ammonium in the "fast"simulation (0.11Tg[N]) is twice as great as in the "slow"simulation (0.05Tg[N]), while the top-of-the-atmosphere radiative impact of representing nitrate is -0.19Wm-2m in the fast simulation and -0.07Wm-2 in the slow simulation. In general, the fast simulation exhibits better spatial correlation with observed nitrate concentrations, while the slow simulation better resolves the magnitude of concentrations. Local near-surface nitrate concentrations are found to be highly correlated with seasonal ammonia emissions, suggesting that ammonia is the predominant limiting factor controlling nitrate prevalence. This study highlights the high sensitivity of ammonium nitrate concentrations to nitric acid uptake rates and provides a novel mechanism for reducing nitrate concentration biases in climate model simulations. The new UM nitrate scheme represents a step change in aerosol modelling capability in the UK across weather and climate timescales.