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We present a framework for estimating concentrations of episodically elevated high-temperature marine ice nucleating particles (INPs) in the sea surface microlayer and their subsequent emission into the atmospheric boundary layer. These episodic INPs have been observed in multiple ship-based and coastal field campaigns, but the processes controlling their ocean concentrations and transfer to the atmosphere are not yet fully understood. We use a combination of empirical constraints and simulation outputs from an Earth System Model to explore different hypotheses for explaining the variability of INP concentrations, and the occurrence of episodic INPs, in the marine atmosphere. In our calculations, we examine two proposed oceanic sources of high-temperature INPs: heterotrophic bacteria and marine biopolymer aggregates (MBPAs). Furthermore, we assume that the emission of these INPs is determined by the production of supermicron sea spray aerosol formed from jet drops, with an entrainment probability that is described by Poisson statistics. The concentration of jet drops is derived from the number concentration of supermicron sea spray aerosol calculated from model runs. We then derive the resulting number concentrations of marine high-temperature INPs (≥ 253 K) in the atmospheric boundary layer and compare their variability to atmospheric observations of INP variability. Specifically, we compare against concentrations of episodically occurring high-temperature INPs observed during field campaigns in the Southern Ocean, the Equatorial Pacific, and the North Atlantic. We find that heterotrophic bacteria and MBPAs acting as INPs provide only a partial explanation for the observed high INP concentrations. We note, however, that there are still substantial knowledge gaps, particularly concerning the identity of the oceanic INPs contributing most frequently to episodic high-temperature INPs, their specific ice nucleation activity, and the enrichment of their concentrations during the sea-air transfer process. Therefore, targeted measurements investigating the composition of these marine INPs as well as drivers for their emission are needed, ideally in combination with modeling studies focused on the potential cloud impacts of these high-temperature INPs.

Sea spray emissions are an important source for ice nucleating particles (INPs) over remote ocean regions. Over the past years, our understanding of marine organic surfactants acting as INPs has advanced a lot. However, there are still significant knowledge gaps regarding the role of larger marine biogenic particles (e.g. polymers, diatom fragments, protists and bacteria) which are potentially the drivers of episodically observed high INP concentrations.In this study, we use a combination of ARM (Atmospheric Radiation Measurement) observations and output from E3SM (Energy Exascale Earth System Model) simulation runs to investigate the impact of larger marine biogenic particles acting as INPs. We use heterotrophic bacteria and nanogels (polymeric particles) as two hypothesized classes of marine INPs which can get transported across the sea-air interface. Based on the offline-calculated concentrations of these ice nucleating entities in the ocean surface layer, we conduct sensitivity studies to estimate INP concentration ranges, relying on current knowledge of enrichment factors and ice nucleation activities (e.g., ns values from McCluskey et al. (2018)). In comparison to observations of episodic high INP concentrations, our estimated concentrations are consistently lower. However, one of the main conclusions of our study is that large uncertainties regarding the links between ocean biology, organic matter in sea spray and ice nucleation properties, remain. Therefore, comprehensive observational datasets, including sea spray size distributions, aerosol and INP compositions, and ice nucleation efficiencies of individual marine species, are needed.

In order to better understand the processes governing the production of marine aerosols a repeatable, controlled method for their generation is required. The Marine Aerosol Reference Tank (MART) has been designed to closely approximate oceanic conditions by producing an evolving bubble plume and surface foam patch. The tank utilizes an intermittently plunging sheet of water and large volume tank reservoir to simulate turbulence, plume and foam formation, and the water flow is monitored volumetrically and acoustically to ensure the repeatability of conditions.

In order to understand the processes governing the production of marine aerosols, repeatable, controlled methods for their generation are required. A new system, the miniature Marine Aerosol Reference Tank (miniMART) has been designed after the success of the original MART system, to approximate a small oceanic spilling breaker by producing an evolving bubble plume and surface foam patch. The smaller tank utilizes an intermittently plunging jet of water produced by a rotating water wheel, into an approximately 6 L reservoir to simulate bubble plume and foam formation and generate aerosols. This system produces bubble plumes characteristic of small whitecaps without the large external pump inherent in the original MART design. Without the pump it is possible to easily culture delicate planktonic and microbial communities in the bulk water during experiments while continuously producing aerosols for study. However, due to the reduced volume and smaller plunging jet, the absolute numbers of particles generated are approximately an order of magnitude less than in the original MART design.

In order to better understand the processes governing the production of marine aerosols a repeatable, controlled method for their generation is required. The Marine Aerosol Reference Tank (MART) has been designed to closely approximate oceanic conditions by producing an evolving bubble plume and surface foam patch. The tank utilizes an intermittently plunging sheet of water and large volume tank reservoir to simulate turbulence, plume and foam formation, and is monitored volumetrically and acoustically to ensure the repeatability of conditions.