Marine aerosol properties over the Southern Ocean in relation to the wintertime meteorological conditions

Journal article, 2022

Given the vast expanse of oceans on our planet, marine aerosols (and sea salt in particular) play an important role in the climate system via multitude of direct and indirect effects. The efficacy of their net impact, however, depends strongly on the local meteorological conditions that influence their physical, optical and chemical properties. Understanding the coupling between aerosol properties and meteorological conditions is therefore important. It has been historically difficult to statistically quantify this coupling over larger oceanic areas due to the lack of suitable observations, leading to large uncertainties in the representation of aerosol processes in climate models. Perhaps no other region shows higher uncertainties in the representation of marine aerosols and their effects than the Southern Ocean. During winter the Southern Ocean boundary layer is dominated by sea salt emissions. Here, using 10 years of austral winter period (June, July and August, 2007-2016) space-based aerosol profiling by CALIOP-CALIPSO in combination with meteorological reanalysis data, we investigated the sensitivity of marine aerosol properties over the Southern Ocean (40-65 degrees S) to various meteorological parameters, such as vertical relative humidity (RH), surface wind speed and sea surface temperature (SST) in terms of joint histograms. The sensitivity study is done for the climatological conditions and for the enhanced cyclonic and anticyclonic conditions in order to understand the impact of large-scale atmospheric circulation on the aerosol properties. We find a clear demarcation in the 532 nm aerosol backscatter and extinction at RH around 60 %, irrespective of the state of the atmosphere. The backscatter and extinction increase at higher relative humidity as a function of surface wind speed. This is mainly because of the water uptake by the wind-driven sea salt aerosols at high RH near the ocean surface resulting in an increase in size, which is confirmed by the decreased depolarization for the wet aerosols. An increase in aerosol backscatter and extinction is observed during the anticyclonic conditions compared to cyclonic conditions for the higher wind speeds and relative humidity, mainly due to aerosols being confined to the boundary layer, and their proximity to the ocean surface facilitates the growth of the particles. We further find a very weak dependency of aerosol backscatter on SSTs at lower wind speeds. However, when the winds are stronger than about 12 m s(-1), the backscattering coefficient generally increases with SST. When aerosol properties are investigated in terms of aerosol verticality and in relation to meteorological parameters, it is seen that the aerosol backscatter values in the free troposphere (pressure <850 hPa) are much lower than in the boundary layer, irrespective of the RH and the three weather states. This indicates that the local emissions from the ocean surface make the dominant contribution to aerosol loads over the Southern Ocean. A clear separation of particulate depolarization is observed in the free and lower troposphere, more prominent in the climatological mean and the cyclonic states. For RH > 60 %, low depolarization values are noticeable in the lower troposphere, which is an indication of the dominance of water-coated and mostly spherical sea salt particles. For RH < 60 %, there are instances when the aerosol depolarization increases in the boundary layer; this is more prominent in the mean and anticyclonic cases, which can be associated with the presence of drier aerosol particles. Based on the joint histograms investigated here, we provide third-degree polynomials to obtain aerosol extinction and backscatter as a function of wind speed and relative humidity. Additionally, backscattering coefficient is also expressed jointly in terms of wind speed and sea surface temperature. Furthermore, depolarization is expressed as a function of relative humidity. These fitting functions would be useful to test and improve the parameterizations of sea salt aerosols in the climate models. We also note some limitations of our study. For example, interpreting the verticality of aerosol properties (especially depolarization) in relation to the meteorological conditions in the free and upper troposphere (pressure <850 hPa) was challenging. Furthermore, we do not see any direct evidence of sudden crystallization (efflorescence), deliquescence or hysteresis effects of the aerosols. Observing such effects will likely require a targeted investigation of individual cases considering tracer transport, rather than the statistical sensitivity study that entails temporally and geographically averaged large data sets.