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DOI	10.5194/acp-21-15901-2021
	Exploring the sensitivity of atmospheric nitrate concentrations to nitric acid uptake rate using the Met Office's Unified Model
	Jones A.C.; Hill A.; Remy S.; Abraham N.L.; Dalvi M.; Hardacre C.; Hewitt A.J.; Johnson B.; Mulcahy J.P.; Turnock S.T.
发表日期	2021
ISSN	1680-7316
起始页码	15901
结束页码	15927
卷号	21 期号:20
英文摘要	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. © Author(s) 2021.
语种	英语
scopus关键词	aerosol composition; atmospheric chemistry; atmospheric forcing; concentration (composition); nitrate; sensitivity analysis; United Kingdom
来源期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/246476
作者单位	Met Office, Fitzroy Road, Exeter, EX1 3PB, United Kingdom; HYGEOS, Lille, France; National Centre for Atmospheric Science, Leeds, LS2 9PH, United Kingdom; Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, United Kingdom; Met Office Strategic Research Group, School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, United Kingdom
推荐引用方式 GB/T 7714	Jones A.C.,Hill A.,Remy S.,et al. Exploring the sensitivity of atmospheric nitrate concentrations to nitric acid uptake rate using the Met Office's Unified Model[J],2021,21(20).
APA	Jones A.C..,Hill A..,Remy S..,Abraham N.L..,Dalvi M..,...&Turnock S.T..(2021).Exploring the sensitivity of atmospheric nitrate concentrations to nitric acid uptake rate using the Met Office's Unified Model.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(20).
MLA	Jones A.C.,et al."Exploring the sensitivity of atmospheric nitrate concentrations to nitric acid uptake rate using the Met Office's Unified Model".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.20(2021).