Abstract

Abstract. Dry deposition to vegetation is a major sink of ground-level ozone and is responsible for about 20 % of the total tropospheric ozone loss. Its parameterization in atmospheric chemistry models represents a significant source of uncertainty for the global tropospheric ozone budget and might account for the mismatch with observations. The model used in this study, the Modular Earth Submodel System version 2 (MESSy2) linked to the fifth-generation European Centre Hamburg general circulation model (ECHAM5) as an atmospheric circulation model (EMAC), is no exception. Like many global models, EMAC employs a “resistance in series” scheme with the major surface deposition via plant stomata which is hardly sensitive to meteorology, depending only on solar radiation. Unlike many global models, however, EMAC uses a simplified high resistance for non-stomatal deposition which makes this pathway negligible in the model. However, several studies have shown this process to be comparable in magnitude to the stomatal uptake, especially during the night over moist surfaces. Hence, we present here a revised dry deposition in EMAC including meteorological adjustment factors for stomatal closure and an explicit cuticular pathway. These modifications for the three stomatal stress functions have been included in the newly developed MESSy VERTEX submodel, i.e. a process model describing the vertical exchange in the atmospheric boundary layer, which will be evaluated for the first time here. The scheme is limited by a small number of different surface types and generalized parameters. The MESSy submodel describing the dry deposition of trace gases and aerosols (DDEP) has been revised accordingly. The comparison of the simulation results with measurement data at four sites shows that the new scheme enables a more realistic representation of dry deposition. However, the representation is strongly limited by the local meteorology. In total, the changes increase the dry deposition velocity of ozone up to a factor of 2 globally, whereby the highest impact arises from the inclusion of cuticular uptake, especially over moist surfaces. This corresponds to a 6 % increase of global annual dry deposition loss of ozone resulting globally in a slight decrease of ground-level ozone but a regional decrease of up to 25 %. The change of ozone dry deposition is also reasoned by the altered loss of ozone precursors. Thus, the revision of the process parameterization as documented here has, among others, the potential to significantly reduce the overestimation of tropospheric ozone in global models.

Highlights

  • Ground-level ozone is a secondary air pollutant which is harmful for humans and ecosystems

  • For the gradient method used at the Borden forest research station, the dry deposition flux was estimated from concentration gradients below and above the canopy and the eddy diffusivity according to the Monin–Obukhov similarity theory

  • Revising the dry deposition scheme of EMAC leads to an improved representation of surface ozone in regions with a positive model ozone bias (e.g. Europe)

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Summary

Introduction

Ground-level ozone is a secondary air pollutant which is harmful for humans and ecosystems. The different parameterizations of the (surface) resistances cause main model uncertainties in computing dry deposition fluxes of trace gases, which depend on the response to hydroclimate and land-type-specific properties (Hardacre et al, 2015; Wu et al, 2018; Wesely and Hicks, 2000). Findings by Solberg et al (2008), Andersson and Engardt (2010) and Wong et al (2019) highlight the importance of considering the dry deposition–meteorology dependence in global models Such an extension would realistically enhance the sensitivity of dry deposition to climate variability and would result in a more accurate prediction of groundlevel ozone.

Model description
The new VERTEX vertical exchange submodel
Dry deposition over vegetation
Uptake through plant stomata
Cuticular deposition
Simulations
VERTEX evaluation
Evaluation with deposition measurements
Annual cycle of dry deposition
Importance of stress factors for the diurnal variation of deposition
Global impact on ground-level ozone
Uncertainties in modelling stomatal conductance
Sensitivity to model resolution
Conclusion and recommendations
Outlook
Full Text
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