Source attribution of cloud condensation nuclei and their impact on stratocumulus clouds and radiation in the south-eastern Atlantic

Abstract

Abstract. The semi-permanent stratocumulus clouds over the South-eastern Atlantic Ocean (SEA) can act as an “air conditioners” to the regional and global climate system. The interaction of aerosols and clouds become important in this region, and can lead to negative radiative effects, partially offsetting the positive radiative forcing of greenhouse gases. A key pathway of aerosols affecting cloud properties is by acting as cloud condensation nuclei (CCN). In this paper, we use the United Kingdom Earth System Model to investigate the sources of CCN (from atmospheric processes and emission sources) in the SEA, and the response of cloud droplet number concentration (CDNC), cloud liquid water path (LWP), and radiative forcing to those sources. Overall, total nucleation (binary nucleation) is the most important source of CCN0.2 % in the marine boundary layer, contributing an annual average of 50 % of CCN0.2 %. In terms of emission sources, anthropogenic emissions (from energy, industry, agriculture, etc.) contribute the most to the annual average CCN0.2 % in the marine boundary layer, followed by BB. In the free troposphere, however, BB becomes the dominant source of CCN0.2 %, accounting for 64 % of the annual average. The contribution of aerosols from different sources to CDNC is consistent with their contribution to CCN0.2 % within the marine boundary layer, with total nucleation being the most important source of CDNC overall. In terms of emissions, anthropogenic sources are also the largest contributors to the annual average of CDNC, closely followed by BB. The contribution of BB to CDNC is more significant than its increase to CCN0.2 %, mainly because BB aerosol also can increase CDNC by enhancing the maximum supersaturation through the radiative effect of shortwave absorption. For an aerosol source that shows an increase in CDNC, it also shows an increase in LWP resulting from a reduction in autoconversion. BB aerosol, due to the absorption effect, can enhance existing temperature inversions and reduce the entrainment of sub-saturated air, leading to a further increase in LWP. As a result, the contribution of BB to LWP is second only to total nucleation. These findings demonstrate that BB is not the dominant source of CCN within the marine boundary layer from an emission source perspective. However, its contribution to clouds increases due to its absorption effect (about the same as anthropogenic sources for CDNC and more than anthropogenic sources for LWP), highlighting the crucial role of its radiative effect on clouds. The results on the radiative effects of aerosols show that BB aerosol exhibits an overall positive RFari (radiative forcing associated with aerosol-radiation interaction), but its net effective radiative forcing remains negative due to its effect on clouds (mainly by absorbing effect). By quantifying aerosol and cloud properties affected by different sources, this paper provides a framework to understand aerosol sources effects on the marine cirrocumulus clouds and radiation in the SEA.