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Abstract. We present a framework for estimating concentrations of episodicallyelevated high-temperature marine ice nucleating particles (INPs) in the seasurface microlayer and their subsequent emission into the atmosphericboundary layer. These episodic INPs have been observed in multipleship-based and coastal field campaigns, but the processes controlling theirocean concentrations and transfer to the atmosphere are not yet fullyunderstood. We use a combination of empirical constraints and simulationoutputs from an Earth system model to explore different hypotheses forexplaining the variability of INP concentrations, and the occurrence ofepisodic INPs, in the marine atmosphere. In our calculations, we examine the following 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 (at 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. In this case study, we evaluate our framework at 253 K because reliable observational data at this temperature are available across three different ocean regions, but suitable data are sparse at higher temperatures. We find that heterotrophic bacteria and MBPAs acting as INPs provide only apartial explanation for the observed high INP concentrations. We note,however, that there are still substantial knowledge gaps, particularlyconcerning the identity of the oceanic INPs contributing most frequently toepisodic high-temperature INPs, their specific ice nucleation activity, andthe enrichment of their concentrations during the sea–air transfer process. Therefore, targeted measurements investigating the composition of these marine INPs and drivers for their emissions are needed, ideally incombination with modeling studies focused on the potential cloud impacts ofthese high-temperature INPs. 

Abstract To resolve the various types of biological ice nuclei (IN) with atmospheric models, an extension of the empirical parameterization (EP) (Phillips et al. 2008; 2013) is proposed to predict the active IN from multiple groups of primary biological aerosol particles (PBAPs). Our approach is to utilize coincident observations of PBAP sizes, concentrations, biological composition, and ice-nucleating ability. The parameterization organizes the PBAPs into five basic groups: fungal spores, bacteria, pollen, viral particles, plant/animal detritus, algae, and their respective fragments. This new biological component of the EP was constructed by fitting predicted concentrations of PBAP IN to those observed at the Amazon Tall Tower Observatory (ATTO) site located in the central Amazon. The fitting parameters for pollen and viral particles, plant/animal detritus, which are much less active as IN than fungal and bacterial groups, are constrained based on their ice nucleation activity from the literature. The parameterization has empirically derived dependencies on the surface area of each group (except algae), and the effects of variability in their mean sizes and number concentrations are represented via their influences on the surface area. The concentration of active algal IN is estimated from literature-based measurements. Predictions of this new biological component of the EP are consistent with previous laboratory and field observations not used in its construction. The EP scheme was implemented in a 0D parcel model. It confirms that biological IN account for most of the total IN activation at temperatures warmer than −20°C and at colder temperatures dust and soot become increasingly more important to ice nucleation. 

Ice nucleating particles (INPs) are a rare subset of particles that can have an outsized impact relative to their prevalence. To simulate INP variability, models require parameterizations for the most important sources of INPs. Most parameterizations in the literature were developed from laboratory experiments that used proxies for ambient particles. Whether these laboratory models effectively represent ambient aerosol is still not well understood and parameterizations developed from field measurements may be more atmospherically relevant. Expanding on previous work in which we used an ice chamber and a single‐particle mass spectrometer (SPMS) to characterize INP composition, we calculate heterogeneous ice nucleation rate coefficients for ambient particles. We find good agreement between our dust and previous measurements of airborne dust. We also use a Monte Carlo approach to assess the relative contribution of each measurement to the uncertainty and find that the biggest source is the sampling efficiency of the SPMS.