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Aerosols and clouds are key components of the marine atmosphere, impacting the Earth’s radiative budget with a net cooling effect over the industrial era that counterbalances greenhouse gas warming, yet with an uncertain amplitude. Here we report recent advances in our understanding of how open ocean aerosol sources are modulated by ocean biogeochemistry and how they, in turn, shape cloud coverage and properties. We organize these findings in successive steps from ocean biogeochemical processes to particle formation by nucleation and sea spray emissions, further particle growth by condensation of gases, the potential to act as cloud condensation nuclei or ice nucleating particles, and finally, their effects on cloud formation, optical properties, and life cycle. We discuss how these processes may be impacted in a warming climate and the potential for ocean biogeochemistry—climate feedbacks through aerosols and clouds. 

Terrestrial volcanism is known to emit mercury (Hg) into the atmosphere. However, despite many years of investigation, its net impact on the atmospheric Hg budget remains insufficiently constrained, in part because the transformations of Hg in volcanic plumes as they age and mix with background air are poorly understood. Here we report the observation of complete gaseous elemental mercury (GEM) depletion events in dilute and moderately aged (∼3–7 hours) volcanic plumes from Piton de la Fournaise on Réunion Island. While it has been suggested that co-emitted bromine could, once photochemically activated, deplete GEM in a volcanic plume, we measured low bromine concentrations in both the gas- and particle-phase and observed complete GEM depletion even before sunrise, ruling out a leading role of bromine chemistry here. Instead, we hypothesize that the GEM depletions were mainly caused by gas–particle interactions with sulfate-rich volcanic particles (mostly of submicron size), abundantly present in the dilute plume. We consider heterogeneous GEM oxidation and GEM uptake by particles as plausible manifestations of such a process and derive empirical rate constants. By extrapolation, we estimate that volcanic aerosols may scavenge 210 Mg y−1 (67–480 Mg y−1) of Hg from the atmosphere globally, acting effectively as atmospheric mercury sink. While this estimate is subject to large uncertainties, it highlights that Hg transformations in aging volcanic plumes must be better understood to determine the net impact of volcanism on the atmospheric Hg budget and Hg deposition pathways. 

Abstract Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments. Ambient INPs were measured in a remote mountaintop location at –46 °C and an ice supersaturation of 30% with concentrations ranging from 0.1 to 70 L –1 . Concentrations of depositional INPs were positively correlated with the mass fractions and loadings of isoprene-derived secondary organic aerosols. Compositional analysis of ice residuals showed that ambient particles with isoprene-derived SOA material can act as depositional ice nuclei. Laboratory experiments further demonstrated the ability of isoprene-derived SOA to nucleate ice under a range of atmospheric conditions. We further show that ambient concentrations of isoprene-derived SOA can be competitive with other INP sources. This demonstrates that isoprene and potentially other biogenically-derived SOA materials could influence cirrus formation and properties. 

Abstract. Due to its remote location and extreme weather conditions, atmospheric in situmeasurements are rare in the Southern Ocean. As a result, aerosol–cloudinteractions in this region are poorly understood and remain a major source ofuncertainty in climate models. This, in turn, contributes substantially topersistent biases in climate model simulations such as the well-known positiveshortwave radiation bias at the surface, as well as biases in numericalweather prediction models and reanalyses. It has been shown in previousstudies that in situ and ground-based remote sensing measurements across theSouthern Ocean are critical for complementing satellite data sets due to theimportance of boundary layer and low-level cloud processes. These processesare poorly sampled by satellite-based measurements and are often obscured bymultiple overlying cloud layers. Satellite measurements also do not constrainthe aerosol–cloud processes very well with imprecise estimation of cloudcondensation nuclei. In this work, we present a comprehensive set of ship-basedaerosol and meteorological observations collected on the 6-weekSouthern Ocean Ross Sea Marine Ecosystem and Environment voyage(TAN1802) voyage of RV Tangaroa across the Southern Ocean, from Wellington, New Zealand, tothe Ross Sea, Antarctica. The voyage was carried out from 8 February to21 March 2018. Many distinct, but contemporaneous, data sets were collectedthroughout the voyage. The compiled data sets include measurements from arange of instruments, such as (i) meteorological conditions at the sea surfaceand profile measurements; (ii) the size and concentration of particles; (iii)trace gases dissolved in the ocean surface such as dimethyl sulfide andcarbonyl sulfide; (iv) and remotely sensed observations of low clouds. Here,we describe the voyage, the instruments, and data processing, and provide a briefoverview of some of the data products available. We encourage the scientificcommunity to use these measurements for further analysis and model evaluationstudies, in particular, for studies of Southern Ocean clouds, aerosol, andtheir interaction. The data sets presented in this study are publiclyavailable at https://doi.org/10.5281/zenodo.4060237 (Kremser et al., 2020).