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The amount of ice versus supercooled water in clouds is important for their radiative properties and role in climate feedbacks. Hence, knowledge of the concentration of ice-nucleating particles (INPs) is needed. Generally, the concentrations of INPs are found to be very low in remote marine locations allowing cloud water to persist in a supercooled state. We had expected the concentrations of INPs at the North Pole to be very low given the distance from open ocean and terrestrial sources coupled with effective wet scavenging processes. Here we show that during summer 2018 (August and September) high concentrations of biological INPs (active at >−20°C) were sporadically present at the North Pole. In fact, INP concentrations were sometimes as high as those recorded at mid-latitude locations strongly impacted by highly active biological INPs, in strong contrast to the Southern Ocean. Furthermore, using a balloon borne sampler we demonstrated that INP concentrations were often different at the surface versus higher in the boundary layer where clouds form. Back trajectory analysis suggests strong sources of INPs near the Russian coast, possibly associated with wind-driven sea spray production, whereas the pack ice, open leads, and the marginal ice zone were not sources of highly active INPs. These findings suggest that primary ice production, and therefore Arctic climate, is sensitive to transport from locations such as the Russian coast that are already experiencing marked climate change., Journal of Geophysical Research: Atmospheres, 127 (6), ISSN:0148-0227, ISSN:2169-897X

Clouds containing supercooled water are important for both climate and weather, but our knowledge of which aerosol particle types nucleate ice in these clouds is far from complete. Combustion aerosols have strong anthropogenic sources, and if these aerosol types were to nucleate ice in clouds, they might exert a climate forcing. Here, we quantified the atmospheric ice‐nucleating particle (INP) concentrations during the United Kingdom's annual Bonfire Night celebrations, which are characterized by large amounts of combustion aerosol from bonfires and fireworks. We used three immersion mode techniques covering more than 6 orders of magnitude in INP concentration over the temperature range from −10°C to homogeneous freezing. We found no observable systematic change in the INP concentration on three separate nights, despite more than a factor of 10 increase in aerosol number concentrations, up to a factor of 10 increase in PM10 concentration, and more than a factor of 100 increase in black carbon (BC) mass concentration relative to pre‐event levels. This implies that BC and other combustion aerosol such as ash did not compete with the INPs present in the background air. Furthermore, the upper limit of the ice‐active site surface density, ns(T), of BC generated in these events was shown to be consistent with several other recent laboratory studies, showing a very low ice‐nucleating activity of BC. We conclude that combustion aerosol particles similar to those emitted on Bonfire Night are at most of secondary importance for the INP population relevant for mixed‐phase clouds in typical midlatitude terrestrial locations. © 2020 American Geophysical Union. ISSN:0148-0227 ISSN:2169-897X

In recent years, sea spray and the biological material it contains has received increased attention as a source of ice nucleating particles (INPs). Such INPs may play a role in remote marine regions, where other sources of INPs are scarce or absent. Marine aerosol is of diverse nature, so identifying sources of INPs is challenging. One fraction of marine bioaerosol, phytoplankton and their exudates, has been a particular focus of marine INP research. In our study we attempt to address three main questions. Firstly, we compare the ice nucleating ability of two common phytoplankton species with Arctic seawater microlayer samples using the same instrumentation to see if these phytoplankton species produce ice nucleating material with sufficient activity to account for the ice nucleation observed in Arctic microlayer samples. We present first measurements of the ice nucleating ability of two predominant phytoplankton species, Melosira arctica, a common Arctic diatom species and Skeletonema marinoi, a ubiquitous diatom species across oceans worldwide. To determine the potential effect of nutrient conditions and characteristics of the algal culture, such as the amount of organic carbon associated with algal cells, on the ice nucleation activity, the Skeletonema marinoi was grown under different nutrient regimes. From comparison of the ice nucleation data of the algal cultures to those obtained from a range of sea surface microlayer (SML) samples obtained during three different field expeditions to the Arctic (ACCACIA, NETCARE, ASCOS) we found that although these diatoms do produce ice nucleating material, they were not as ice active as the investigated microlayer samples. Secondly, to improve our understanding of local Arctic marine sources as atmospheric INP we applied several aerosolisation techniques to analyse the ice nucleating ability of aerosolised microlayer and algae samples. The aerosols were generated either by direct nebulisation of the undiluted bulk solutions, or by the addition of the samples to a sea spray simulation chamber filled with artificial seawater. The latter method generates aerosol particles using a plunging jet to mimic the process of oceanic wave-breaking. We observed that the aerosols produced using this approach can be ice active indicating that the ice nucleating material in seawater can indeed transfer to the aerosol phase. Thirdly, we attempted to measure ice nucleation activity across the entire temperature range relevant for mixed-phase clouds using a suite of ice nucleation measurement techniques- an expansion cloud chamber, a continuous flow diffusion chamber, and a cold stage. In order to compare the measurements made using the different instruments, we have normalised the data in relation to the mass of salt present in the nascent sea spray aerosol. At temperatures above 248 K some of the SML samples were very effective at nucleating ice, but there was substantial variability between the different samples. In contrast, there was much less variability between samples below 248 K.

The freezing of supercooled water to ice and the materials which catalyse this process are of fundamental interest to a wide range of fields. At present, our ability to control, predict or monitor ice formation processes is poor. The isolation and characterisation of frozen droplets from supercooled liquid droplets would provide a means of improving our understanding and control of these processes. Here, we have developed a microfluidic platform for the continuous flow separation of frozen from unfrozen picolitre droplets based on differences in their density, thus allowing the sorting of ice crystals and supercooled water droplets into different outlet channels with 94 ± 2% efficiency. This will, in future, facilitate downstream or off-chip processing of the frozen and unfrozen populations, which could include the analysis and characterisation of ice-active materials or the selection of droplets with a particular ice-nucleating activity.

A minute fraction of atmospheric particles exert a disproportionate effect on the phase of mixed-phase clouds by acting as ice-nucleating particles (INPs). To understand the effects of these particles on weather and climate, both now and into the future, we must first develop a quantitative understanding of the major INP sources worldwide. Previous work has demonstrated that aerosols such as desert dusts are globally important INPs, but the role of biogenic INPs is unclear, with conflicting evidence for their importance. Here, we show that at a temperate site all INPs active above −18 °C at concentrations >0.1 L−1 are destroyed on heating, consistent with these INPs being of biological origin. Furthermore, we show that a global model of desert dust INPs dramatically underestimates the measured INP concentrations, but is consistent with the thermally-stable component. Notably, the heat sensitive INPs are active at temperatures where shallow cloud layers in Northern Europe are frequently observed to glaciate. Hence, we suggest that biogenic material is important for primary ice production in this region. The prevalence of heat sensitive, most likely biogenic, INPs in this region highlights that, as a community, we need to quantify the sources and transport of these particles as well as determine their atmospheric abundance across the globe and at cloud altitudes.

Ice-nucleating particles (INPs) play a significant role in the climate and hydrological cycle by triggering ice formation in supercooled clouds, thereby causing precipitation and affecting cloud lifetimes and their radiative properties. However, despite their importance, INP often comprise only 1 in 103–106 ambient particles, making it difficult to ascertain and predict their type, source, and concentration. The typical techniques for quantifying INP concentrations tend to be highly labour-intensive, suffer from poor time resolution, or are limited in sensitivity to low concentrations. Here, we present the application of microfluidic devices to the study of atmospheric INPs via the simple and rapid production of monodisperse droplets and their subsequent freezing on a cold stage. This device offers the potential for the testing of INP concentrations in aqueous samples with high sensitivity and high counting statistics. Various INPs were tested for validation of the platform, including mineral dust and biological species, with results compared to literature values. We also describe a methodology for sampling atmospheric aerosol in a manner that minimises sampling biases and which is compatible with the microfluidic device. We present results for INP concentrations in air sampled during two field campaigns: (1) from a rural location in the UK and (2) during the UK’s annual Bonfire Night festival. These initial results will provide a route for deployment of the microfluidic platform for the study and quantification of INPs in upcoming field campaigns around the globe, while providing a benchmark for future lab-on-a-chip-based INP studies. Electronic supplementary material The online version of this article (10.1007/s10404-018-2069-x) contains supplementary material, which is available to authorized users.

Ice-nucleating particles (INPs) are of atmospheric importance because they catalyse the freezing of supercooled cloud droplets, strongly affecting the lifetime and radiative properties of clouds. There is a need to improve our knowledge of the global distribution of INPs, their seasonal cycles and long-term trends, but our capability to make these measurements is limited. Atmospheric INP concentrations are often determined using assays involving arrays of droplets on a cold stage, but such assays are frequently limited by the number of droplets that can be analysed per experiment, often involve manual processing (e.g. pipetting of droplets), and can be susceptible to contamination. Here, we present a microfluidic platform, the LOC-NIPI (Lab-on-a-Chip Nucleation by Immersed Particle Instrument), for the generation of water-in-oil droplets and their freezing in continuous flow as they pass over a cold plate for atmospheric INP analysis. LOC-NIPI allows the user to define the number of droplets analysed by simply running the platform for as long as required. The use of small (∼100 μm diameter) droplets minimises the probability of contamination in any one droplet and therefore allows supercooling all the way down to homogeneous freezing (around −36 °C), while a temperature probe in a proxy channel provides an accurate measure of temperature without the need for temperature modelling. The platform was validated using samples of pollen extract and Snomax®, with hundreds of droplets analysed per temperature step and thousands of droplets being measured per experiment. Homogeneous freezing of purified water was studied using >10 000 droplets with temperature increments of 0.1 °C. The results were reproducible, independent of flow rate in the ranges tested, and the data compared well to conventional instrumentation and literature data. The LOC-NIPI was further benchmarked in a field campaign in the Eastern Mediterranean against other well-characterised instrumentation. The continuous flow nature of the system provides a route, with future development, to the automated monitoring of atmospheric INP at field sites around the globe.