Abstract

Abstract. Schemes used to parameterise ozone dry deposition velocity at the oceanic surface mainly differ in terms of how the dominant term of surface resistance is parameterised. We examine three such schemes and test them in a global climate–chemistry model that incorporates meteorological nudging and monthly-varying reactive-gas emissions. The default scheme invokes the commonly used assumption that the water surface resistance is constant. The other two schemes, named the one-layer and two-layer reactivity schemes, include the simultaneous influence on the water surface resistance of ozone solubility in water, waterside molecular diffusion and turbulent transfer, and a first-order chemical reaction of ozone with dissolved iodide. Unlike the one-layer scheme, the two-layer scheme can indirectly control the degree of interaction between chemical reaction and turbulent transfer through the specification of a surface reactive layer thickness. A comparison is made of the modelled deposition velocity dependencies on sea surface temperature (SST) and wind speed with recently reported cruise-based observations. The default scheme overestimates the observed deposition velocities by a factor of 2–4 when the chemical reaction is slow (e.g. under colder SSTs in the Southern Ocean). The default scheme has almost no temperature, wind speed, or latitudinal variations in contrast with the observations. The one-layer scheme provides noticeably better variations, but it overestimates deposition velocity by a factor of 2–3 due to an enhancement of the interaction between chemical reaction and turbulent transfer. The two-layer scheme with a surface reactive layer thickness specification of 2.5 µm, which is approximately equal to the reaction-diffusive length scale of the ozone–iodide reaction, is able to simulate the field measurements most closely with respect to absolute values as well as SST and wind-speed dependence. The annual global oceanic deposition of ozone determined using this scheme is approximately half of the original oceanic deposition obtained using the default scheme, and it corresponds to a 10 % decrease in the original estimate of the total global ozone deposition. The previously reported modelled estimate of oceanic deposition is roughly one-third of total deposition and with this new parameterisation it is reduced to 12 % of the modelled total global ozone deposition. Deposition parameterisation influences the predicted atmospheric ozone mixing ratios, especially in the Southern Hemisphere. For the latitudes 45–70° S, the two-layer scheme improves the prediction of ozone observed at an altitude of 1 km by 7 % and that within the altitude range 1–6 km by 5 % compared to the default scheme.

Highlights

  • Ozone (O3) is not emitted directly into the atmosphere but is formed in both the stratosphere and troposphere by photochemical reactions involving natural and anthropogenic precursor species

  • Ozone dry deposition parameterisation schemes are best evaluated within an integrated modelling framework that includes multi-parameter interdependencies of deposition as exist in the field

  • We assessed the performance of three ozone dry deposition schemes for seawater within the global climate–chemistry model ACCESS-UKCA, incorporating meteorological nudging and monthly-varying emissions

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Summary

Introduction

Ozone (O3) is not emitted directly into the atmosphere but is formed in both the stratosphere and troposphere by photochemical reactions involving natural and anthropogenic precursor species. The “present-day” (about the year 2000) total global dry deposition of ozone estimated by the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) is of the order of 1094±264 Tg yr−1, which is almost double the flux of ozone from the stratosphere to the troposphere (477 ± 96 Tg yr−1) While a constant rc may be a good first-order estimate of global and long-term average oceanic dry deposition, it does not include any spatial and temporal dependencies of the surface uptake process on any oceanic physical, chemical, or biological properties or processes. The surface ocean acts as a gateway for molecules to enter the atmosphere or ocean medium and contains complex chemical reactions of inorganic components and dissolved organic matter Some of these reactions are important sources or sinks of climatically active trace gases. In the surface turbulent layer (∼ 10–50 m) below the viscous sublayer, turbulent processes dominate

Mechanistic approaches to determining rc
ACCESS-UKCA chemistry–climate model
Current scheme for ozone dry deposition to water
Ozone loss in seawater
An alternative scheme for rc in ACCESS-UKCA
Two-layer reactivity scheme – improved formulation
Sensitivity analysis
Comparison with data
Deposition velocity
Ozone loss
Ozone concentration
Findings
Conclusions
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