Abstract

Abstract. In this study we introduce an in-cloud wet deposition scheme for liquid and ice phase clouds for global aerosol–climate models which use a size-segregated aerosol description. For in-cloud nucleation scavenging, the scheme uses cloud droplet activation and ice nucleation rates obtained from the host model. For in-cloud impaction scavenging, we used a method where the removal rate depends on the wet aerosol size and cloud droplet radii. We used the latest release version of ECHAM-HAMMOZ (ECHAM6.3-HAM2.3-MOZ1.0) with the Sectional Aerosol module for Large Scale Applications version 2.0 (SALSA) microphysics package to test and compare our scheme. The scheme was compared to a scheme that uses fixed scavenging coefficients. The comparison included vertical profiles and mass and number distributions of wet deposition fluxes of different aerosol compounds and for different latitude bands. Using the scheme presented here, mass concentrations for black carbon, organic carbon, sulfate, and the number concentration of particles with diameters larger than 100 nm are higher than using fixed scavenging coefficients, with the largest differences in the vertical profiles in the Arctic. On the other hand, the number concentrations of particles smaller than 100 nm in diameter show a decrease, especially in the Arctic region. These results could indicate that, compared to fixed scavenging coefficients, nucleation scavenging is less efficient, resulting in an increase in the number concentration of particles larger than 100 nm. In addition, changes in rates of impaction scavenging and new particle formation (NPF) can be the main cause of reduction in the number concentrations of particles smaller than 100 nm. Without further adjustments in the host model, our wet deposition scheme produced unrealistically high aerosol concentrations, especially at high altitudes. This also leads to a spuriously long lifetime of black carbon aerosol. To find a better setup for simulating aerosol vertical profiles and transport, sensitivity simulations were conducted where aerosol emission distribution and hygroscopicity were altered. Vertical profiles of aerosol species simulated with the scheme which uses fixed scavenging rates and the abovementioned sensitivity simulations were evaluated against vertical profiles from aircraft observations. The lifetimes of different aerosol compounds were also evaluated against the ensemble mean of models involved in the Aerosol Comparisons between Observations and Models (AEROCOM) project. The best comparison between the observations and the model was achieved with our wet deposition scheme when black carbon was emitted internally mixed with soluble compounds instead of keeping it externally mixed. This also produced atmospheric lifetimes for the other species which were comparable to the AEROCOM model means.

Highlights

  • The estimated radiation budget of the Earth has large uncertainties, and a majority of these uncertainties are related to the uncertainties in the direct and indirect effects of atmospheric aerosol (IPCC, 2014)

  • We focused on SO4, organic carbon (OC), and Black carbon (BC) as they are readily available from the Atmospheric Tomography (ATom) aircraft campaign measurements

  • The scavenging coefficients are calculated using the size-segregated fraction of activated particles from a cloud activation scheme

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Summary

Introduction

The estimated radiation budget of the Earth has large uncertainties, and a majority of these uncertainties are related to the uncertainties in the direct and indirect effects of atmospheric aerosol (IPCC, 2014). In order to estimate the radiation budget of the Earth correctly, aerosols and their physical properties affecting radiation and cloud formation have to be modeled realistically. Black carbon (BC) is one of the aerosol compounds which has an effect on the Earth’s radiation budget via absorbing solar radiation, accelerating the melting of snow and ice, and influencing cloud formation and life cycle (Bond et al, 2013). Due to its ability to darken snow and ice covers, BC has been found to be a major warming agent at high latitudes (AMAP, 2015). It has been proposed that the mitigation of BC is one of the possible means to slow Arctic warming (Stone et al, 2014)

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