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Ice nucleating particles (INPs) are a rare but important type of atmospheric aerosol particles, contributed mostly by mineral dust particles and by biogenic macromolecules expressed by a range of different microorganisms. INPs’ ability to nucleate ice in cloud droplets already far above their homogeneous freezing temperature (at ~ -38°C) influences for instance cloud radiative processes and precipitation formation.Despite a recent surge of research on INPs, neither are all important sources of atmospheric INP sufficiently known, nor their atmospheric abundance which varies with location and season.Here we examine the heat sensitivity of some types of INP of biogenic origin by exposing them to a range of different heating temperatures (60°C, 85°C, and 90°C) for one hour. The heating is expected to destroy proteinaceous ice active macromolecules. The ice activity of different samples was examined before and after heating.Examined samples included birch pollen (Betula pendula), fungi (Mortierella alpina, Fusarium acuminatum), the bacteria Pseudomonas syringae (from a commercially available SNOMAX sample) and aspen leaves (from Populus tremuloides) which had been sampled and freeze-dried decades ago. We compare their heat sensitivity to that of INPs from airborne aerosol samples collected on filters in summer months at Villum Research Station (VRS) in North Greenland, which were exposed to the same heating procedure.For samples from F. acuminatum and P. syringae, a continuing decrease in ice activity (expressed as INP per sample mass) was observed for each of the heating steps. The decrease was larger than one order of magnitude for each heating step across the examined temperature range (roughly -5°C to -25°C). For the B. pendula sample, highly ice active macromolecules inducing ice nucleation at > -10°C were already destroyed by heating to 60°C, while the signal below -15°C was changed much less by any of the heating steps. The M. alpina sample showed no change in ice activity after heating to 60°C, but a strong decrease across the examined temperature range after heating further to 85°C, and some additional decrease (roughly one order of magnitude) after heating to 90°C. The aspen leave samples showed no noticeable reaction to heating at freezing temperatures below -15°C, but behaved similar to the M. alpina sample at -10°C.Interestingly, for freezing temperatures > -10°C, INP concentrations of VRS summer samples also showed no or only a small decrease in ice activity upon heating to 60°C, similar as the M. alpina and aspen leave samples. Also similar to these two, VRS samples showed a very pronounced decrease upon heating to 85°C and some further decrease upon heating to 90°C. This is interesting in the light that recent research suggested that M. alpina, together with the bacteria species Pantoea ananatis, are likely sources of the INPs present in a aspen leave sample of the same batch as the one examined here. Combining these findings, we speculate that M. alpina may be of considerable importance as terrestrially sourced atmospheric INPs for regions even including the summer Arctic.

Pollen belong to a subset of atmospheric aerosol particles that enable the glaciation of supercooled liquid water, which is present in clouds down to an ambient temperature of -38°C. While the ice nucleating properties of pollen are widely researched in laboratory studies, it is challenging to evaluate their effect on clouds in observations at a large scale. Using a combination of ground-based measurements of pollen concentration and satellite observations of cloud properties during springtime, we show that the ice nucleating properties of pollen promote the glaciation of supercooled liquid water. We further establish the link between the pollen-induced increase in cloud ice to a higher precipitation frequency. In light of anthropogenic climate change, the extended and strengthened pollen season and alterations in biodiversity can, therefore, introduce a localized climate forcing and a modification of the precipitation frequency and intensity, especially during springtime.

Arctic clouds are poorly represented in climate models partly due to a lack of understanding of their source and nucleating capability of natural aerosol in the high Arctic. Recent field campaigns provided evidence of a source of sea salt aerosol (SSA) from blowing snow above sea ice, which can account for SSA winter/spring maxima observed in the polar regions. SSA emissions from sea ice sources can potentially influence regional climate via the indirect radiative effect, but contributions to cloud-forming particles, in particular, ice-nucleating particles (INP), are unknown. Here we report the first online spring-time observations of INPs in the Central Arctic. INP concentrations were on the order of a few tens [particle m-3] activating between -38 and -15°C and were often associated with high wind speeds. Initial offline droplet assay analysis of snow on sea ice indicates the presence of potential INPs in winter/spring activating at -29 to -25°C. This is evidence that snow on sea ice represents a viable reservoir of INPs, which can be physically released via the blowing snow mechanism to the air above. We discuss sea ice sources of coarse SSA and INPs and their role in the lower atmosphere with a focus on blowing snow. To do this, we consider the comprehensive set of MOSAiC observations, including aerosol size and composition, airborne snow particles, and chemical and physical properties of both aerosol and snow on sea ice.

The remoteness of the Antarctic continent has important implications for the microphysical properties of clouds: In particular, the rare abundance of ice-nucleating particles (INP) limits the primary nucleation of ice crystals. Yet, persistent mixed-phase clouds with ice crystal number concentrations of 0.1-1l-1 are still observed in the Arctic and Antarctic. However, the ability of regional climate models to reproduce these mixed-phase clouds remains limited, much like the knowledge about their climatological effects. Thus, we added a module to the regional climate model COSMO-CLM² aimed at improving the parametrisation of the aerosol-cycle, which allows us to prescribe different concentrations of INPs. We examined the model response to different concentrations by running it in an area around the Belgian Princess Elisabeth Station in Dronning Maud Land for one month and with four different concentration settings: The first, corresponding to the low end of INP concentrations we observed at the station, the second, corresponding to the high end of INP concentrations we observed at the station, and the third and fourth, to the low and high end of continental observations. The performance was evaluated by comparing the simulation results with radar and ceilometer observations taken at the station. Finally, we analysed the differences between the four simulations to determine the overall sensitivity of the model to variability in INP concentrations, which allows us to draw conclusions about the importance of accurately simulating processes related to ice nucleation, and about the climatological implications that a change in aerosol concentrations would have.

Transparent exopolymer particles (TEP) exhibit the properties of gels and are ubiquitously found in the world oceans. Here we demonstrate that TEP may enter the atmosphere as part of sea spray aerosol and likely influence cloud properties. We show number concentrations of TEP with a diameter > 4.5 µm, hence covering a part of the supermicron particle range measured in ambient aerosol and cloud water samples from the tropical Atlantic Ocean. Furthermore, TEP were analysed in generated aerosol particles using a plunging waterfall tank that was filled with the ambient seawater.Based on Na+ concentrations in seawater and the atmosphere, the enrichment of TEP in the tank generated aerosol particles was well in-line with another study. The TEP enrichments in the ambient atmosphere were, however, up to two orders of magnitude higher compared to the tank study and such high values are thus far not reported for supermicron aerosol particles. We propose that the high enrichment of TEP in the particles and in cloud water result from a combination of enrichment during bubble-bursting transfer from the ocean and secondary in-situ atmospheric formation. We suggest that similar (biotic and abiotic) formation mechanism reported for TEP formation in the (sea)water might take place in the atmosphere as well, as the required conditions (e.g. high concentrations of dissolved TEP precursors such as polysaccharides, presence of bacteria in the cloud water) were given.TEP concentrations in the atmosphere were two orders of magnitude higher than INP concentrations in the aerosol particles and cloud water, respectively. However, only a part of the TEP population, assumingly the one colonized by bacteria, might contribute to INP population, and are worth further studies.The study contributes to the international SOLAS program.Ref. : van Pinxteren, M., Robinson, T.-B., Zeppenfeld, S., Gong, X., Bahlmann, E., Fomba, K. W., Triesch, N., Stratmann, F., Wurl, O., Engel, A., Wex, H., and Herrmann, H.: High number concentrations of transparent exopolymer particles in ambient aerosol particles and cloud water – a case study at the tropical Atlantic Ocean, Atmos. Chem. Phys., 22, 5725–5742, https://doi.org/10.5194/acp-22-5725-2022, 2022.

Atmospheric ice nucleating particle (INP) concentration data from the free troposphere are sparse, but urgently needed to understand vertical transport processes of INPs and their influence on cloud formation and properties. Here, we introduce the new High-volume flow aERosol particle filter sAmpler (HERA) which was specially developed for installation on research aircraft and subsequent offline INP analysis. HERA is a modular system constisting of a sampling unit and a powerful pump unit and has several features which were integrated specifically for INP sampling. Firstly, the pump unit enables sampling at flow rates exceeding 100 L min−1, which is well above typical flow rates of aircraft INP sampling systems described in the literature (~10 L min−1). Consequently, required sampling times to capture rare, high-temperature INPs (≥-15 °C) are reduced in comparison to other systems and potential source regions of INPs can be confined more precisely. Secondly, the sampling unit is designed as a seven-way valve, enabling switching between six filter holders and a bypass with one filter being sampled at a time. In contrast to other aircraft INP sampling systems, the valve position is controlled remotely via software so that manual filter changes in-flight are eliminated and the potential for sample contamination is decreased. This design is compatible with a high degree of automation, i.e., triggering filter changes depending on parameters like flight altitude, geographical location, temperature, or time. In addition to the design and principle of operation of HERA, this paper presents laboratory characterization experiments with size-selected test substances, i.e., SNOMAX® and Arizona Test Dust. The particles were sampled on filters with HERA, varying either particle diameter (300 nm to 800 nm) or flow rate (10 L min−1 to 100 L min−1) between experiments. The subsequent offline INP analysis showed good agreement with literature data and comparable sampling efficiencies for all investigated particle sizes and flow rates. Furthermore, the deposition efficiency of atmospheric INPs in HERA was compared to a straightforward filter sampler and good agreement was found. Finally, results from the first campaign of HERA on the High Altitude and LOng range research aircraft (HALO) demonstrate the functionality of the new system in the context of aircraft application.

Ice-nucleating particles (INPs) can initiate ice formation in clouds at temperatures above -38 °C through heterogeneous ice nucleation. As a result, INPs affect cloud microphysical and radiative properties, cloud lifetime, and precipitation behavior and thereby ultimately the Earth’s climate. Yet, little is known regarding the sources, abundance and properties of INPs, especially in remote regions such as the Arctic. In this study, 2-yearlong INP measurements (from July 2018 to September 2020) at Villum Research Station in northern Greenland are presented. A low-volume filter sampler was deployed to collect filter samples for offline INP analysis. An annual cycle of INP concentration (NINP) was observed, and the fraction of heat-labile INPs was found to be higher in months with low to no snow cover and lower in months when the surface was well covered in snow (> 0.8 m). Samples were categorized into three different types based only on the slope of their INP spectra, namely into summer, winter and mix type. For each of the types a temperature-dependent INP parameterization was derived, clearly different depending on the time of the year. Winter and summer types occurred only during their respective seasons and were seen 60 % of the time. The mixed type occurred in the remaining 40 % of the time throughout the year. April, May and November were found to be transition months. A case study comparing April 2019 and April 2020 was performed. The month of April was selected because a significant difference in NINP was observed during these two periods, with clearly higher NINP in April 2020. In parallel to the observed differences in NINP, also a higher cloud-ice fraction was observed in satellite data for April 2020, compared to April 2019. NINP in the case study period revealed no clear dependency on either meteorological parameters or different surface types which were passed by the collected air masses. Overall, the results suggest that the coastal regions of Greenland were the main sources of INPs in April 2019 and 2020, most likely including both local terrestrial and marine sources., Atmospheric Chemistry and Physics, 23 (8), ISSN:1680-7375, ISSN:1680-7367

Ice-nucleating particles (INPs) initiate the primary ice formation in clouds at temperatures above ca. −38 ∘C and have an impact on precipitation formation, cloud optical properties, and cloud persistence. Despite their roles in both weather and climate, INPs are not well characterized, especially in remote regions such as the Arctic. We present results from a ship-based campaign to the European Arctic during May to July 2017. We deployed a filter sampler and a continuous-flow diffusion chamber for offline and online INP analyses, respectively. We also investigated the ice nucleation properties of samples from different environmental compartments, i.e., the sea surface microlayer (SML), the bulk seawater (BSW), and fog water. Concentrations of INPs (NINP) in the air vary between 2 to 3 orders of magnitudes at any particular temperature and are, except for the temperatures above −10 ∘C and below −32 ∘C, lower than in midlatitudes. In these temperature ranges, INP concentrations are the same or even higher than in the midlatitudes. By heating of the filter samples to 95 ∘C for 1 h, we found a significant reduction in ice nucleation activity, i.e., indications that the INPs active at warmer temperatures are biogenic. At colder temperatures the INP population was likely dominated by mineral dust. The SML was found to be enriched in INPs compared to the BSW in almost all samples. The enrichment factor (EF) varied mostly between 1 and 10, but EFs as high as 94.97 were also observed. Filtration of the seawater samples with 0.2 µm syringe filters led to a significant reduction in ice activity, indicating the INPs are larger and/or are associated with particles larger than 0.2 µm. A closure study showed that aerosolization of SML and/or seawater alone cannot explain the observed airborne NINP unless significant enrichment of INP by a factor of 105 takes place during the transfer from the ocean surface to the atmosphere. In the fog water samples with −3.47 ∘C, we observed the highest freezing onset of any sample. A closure study connecting NINP in fog water and the ambient NINP derived from the filter samples shows good agreement of the concentrations in both compartments, which indicates that INPs in the air are likely all activated into fog droplets during fog events. In a case study, we considered a situation during which the ship was located in the marginal sea ice zone and NINP levels in air and the SML were highest in the temperature range above −10 ∘C. Chlorophyll a measurements by satellite remote sensing point towards the waters in the investigated region being biologically active. Similar slopes in the temperature spectra suggested a connection between the INP populations in the SML and the air. Air mass history had no influence on the observed airborne INP population. Therefore, we conclude that during the case study collected airborne INPs originated from a local biogenic probably marine source.

Marine viruses have thoroughly been studied in seawater, yet their dispersal from neuston ecosystems at the air-sea interface towards the atmosphere remains a knowledge gap. Here, we show that 6.2 % of the studied virus population were shared between air-sea interface ecosystems and rainwater. Virus enrichment in the 1-mm thin surface microlayer and sea foams happened selectively, and variant analysis proved virus transfer to aerosols and rain. Viruses detected in rain and aerosols showed a significantly higher percent G/C base content compared to marine viruses, and a genetically distinct rain virome supports that those viruses could inhabit higher air masses. CRISPR spacer matches of marine prokaryotes to “foreign” viruses from rainwater prove regular virus-host encounters at the air-sea interface. Our findings on aerosolization and long-range atmospheric dispersal implicate virus-mediated carbon turnover in remote areas, viral dispersal mechanisms relevant to human health, and involvement of viruses in atmospheric processes like ice-nucleation.

Within the Southern Ocean, the greatest warming is occurring on the Antarctic Peninsula (AP) where clear cryospheric and biological consequences are being observed. Antarctic coastal systems harbour a high diversity of marine and terrestrial ecosystems heavily influenced by Antarctic seaweeds (benthonic macroalgae) and bird colonies (mainly penguins). Primary sea spray aerosols (SSA) formed by the outburst of bubbles via the sea-surface microlayer depend on the organic composition of the sea water surface. In order to gain insight into the influence of ocean biology and bio-geochemistry on atmospheric aerosol, we performed in situ laboratory aerosol bubble chamber experiments to study the effect of different leachates of biogenic material - obtained from common Antarctic seaweeds as well as penguin guano - on primary SSA. The addition of different leachate materials on a seawater sample showed a dichotomous effect depending on the leachate material added - either suppressing (up to 52%) or enhancing (22–88%) aerosol particle production. We found high ice nucleating particle number concentrations resulting from addition of guano leachate material. Given the evolution of upper marine polar coastal ecosystems in the AP, further studies on ocean-atmosphere coupling are needed in order to represent the currently poorly understood climate feedback processes., The study was further supported by the Spanish Ministry of Economy through project PI-ICE (no. CTM 2017–89117-R) and the Ramon y Cajal fellowship (no. RYC-2012-11922). This work acknowledges the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000928-S). The National Centre for Atmospheric Science (NCAS) Birmingham group is funded by the UK Natural Environment Research Council. We gratefully acknowledge the funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation, Projektnummer 268020496–TRR 172) within the Transregional Collaborative Research Center “ArctiC Amplification: Climate Relevant Atmospheric and SurfaCe Processes, and Feedback Mechanisms (AC)3” in subproject B04.

By serving as condensation and ice nuclei, aerosols play a vital role in the formation of clouds. This has significant implications for the radiation balance and precipitation amounts over the Antarctic Ice Sheet, where type and amount of aerosols differ significantly from other places because of its remote location. However, that is also the reason observations are sparse, and consequently, few studies exist examining this effect. Recently, a module was added to the COSMO-CLM² regional climate model to account for the aerosol-cycle. The model was integrated for the region around the Princess Elisabeth Antarctic research station (PEA) in Dronning Maud Land for a period of 10 days in January 2016, of which the first 3 days were discarded. Varying cloud condensation and ice nuclei were prescribed to the model, based on observations from PEA. The model output was compared to observations of cloud structure and precipitation amounts taken at PEA, as well as the unmodified COSMO-CLM² model. The model integrations indicate that the number of ice nuclei has a significant impact on the microphysical composition of clouds, with higher numbers being associated with a lower amount of liquid water content of clouds and higher precipitation amounts. Additional runs are performed to confirm and extend these findings for an entire year. Recent measurements of ice nuclei particle concentrations obtained during two austral summers are also considered. Moreover, we analysed how atmospheric dynamics affect the cloud-aerosol interaction by analysing the model sensitivity for different weather regimes.

Ice nucleating particles (INPs) are rare but important atmospheric particles as they induce the formation of primary ice in mixed phase clouds and also in some cirrus clouds. A plethora of substances which can be found in atmospheric particles can induce ice nucleation. The most important ice active particle types in the atmosphere are assumed to be mineral dust and biological particles, which can originate from a large number of sources. It is hence not surprising that INP concentrations vary over several orders of magnitude at any ice nucleation temperature, with concentrations being typically larger in continental than in marine environments. Although research concerning INP and their global occurrence has seen a steep rise in the past years, global INP concentrations are still not well known, and not all important INP sources are clear, neither are there good parameterizations for describing INP concentrations in models.To increase the knowledge of typical global INP concentrations and to draw conclusions about INP sources, we examined INP concentrations in the Antarctic region, namely at the German research Station Neumayer III, located at shelf ice in close proximity (only some 10 km) to the ice edge, at the Belgian research Station Princess Elisabeth, located roughly 200 km inland and at an altitude of 1390 m, and during a campaign including ship- and land-based data at the Antarctic peninsula. We used our well-established methods of filter collection and off-line analysis with cold-stages to derive INP concentrations in these locations.For Neumayer, two years of data are available. INP concentrations there were generally lower than values derived, e.g., for northern mid latitudes, and they were similar to values published for the Southern Ocean in literature. No pronounced annual cycle was observed. Around and on the Antarctic peninsula, INP concentrations were roughly similar to those observed at Neumayer. However, the Princess Elisabeth station, for which only data obtained during two austral summers are available, showed the lowest values detected in this study. Our results suggest that sources of INP in the Antarctic region are rare, and particularly so on Antarctica itself.

The sources and abundance of ice-nucleating particles (INPs) that initiate cloud ice formation remain understudied, especially in the Southern Hemisphere. In this study, we present INP measurements taken close to Punta Arenas, Chile, at the southernmost tip of South America from May 2019 to March 2020, during the Dynamics, Aerosol, Cloud, And Precipitation Observations in the Pristine Environment of the Southern Ocean (DACAPO-PESO) campaign. The highest ice nucleation temperature was observed at −3◦C, and from this temperature down to ∼ −10◦C, a sharp increase of INP number concentration (NINP) was observed. Heating of the samples revealed that roughly 90 % and 80 % of INPs are proteinaceous-based biogenic particles at > −10 and −15◦C, respectively. The NINP at Punta Arenas is much higher than that in the Southern Ocean, but it is comparable with an agricultural area in Argentina and forestry environment in the US. Ice active surface site density (ns) is much higher than that for marine aerosol in the Southern Ocean, but comparable to English fertile soil dust. Parameterization based on particle number concentration in the size range larger than 500 nm (N>500 nm) from the global average (DeMott et al., 2010) overestimates the measured INP, but the parameterization representing biological particles from a forestry environment (Tobo et al., 2013) yields NINP comparable to this study. No clear seasonal variation of NINP was observed. High precipitation is one of the most important meteorological parameters to enhance the NINP in both cold and warm seasons. A comparison of data from in situ and lidar measurements showed good agreement for concentrations of large aerosol particles (> 500 nm) when assuming continental conditions for retrieval of the lidar data, suggesting that these particles were well mixed within the planetary boundary layer (PBL). This corroborates the continental origin of these particles, consistent with the results from our INP source analysis. Overall, we suggest that a high NINP of biogenic INPs originated from terrestrial sources and were added to the marine air masses during the overflow of a maximum of roughly 150 km of land before arriving at the measurement station.

The aim of this study is to show how a newly developed aerodynamic lens system (ALS), a delayed ion extraction (DIE), and better electric shielding improve the efficiency of the Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA). These improvements are applicable to single-particle laser ablation mass spectrometers in general. To characterize the modifications, extensive size-resolved measurements with spherical polystyrene latex particles (PSL; 150–6000 nm) and cubic sodium chloride particles (NaCl; 400–1700 nm) were performed. Measurements at a fixed ALS position show an improved detectable particle size range of the new ALS compared to the previously used Liu-type ALS, especially for supermicron particles. At a lens pressure of 2.4 hPa, the new ALS achieves a PSL particle size range from 230 to 3240 nm with 50 % detection efficiency and between 350 and 2000 nm with 95 % detection efficiency. The particle beam divergence was determined by measuring the detection efficiency at variable ALS positions along the laser cross sections and found to be minimal for PSL at about 800 nm. Compared to measurements by single-particle mass spectrometry (SPMS) instruments using Liu-type ALSs, the minimum particle beam divergence is shifted towards larger particle sizes. However, there are no disadvantages compared to the Liu-type lenses for particle sizes down to 200 nm. Improvements achieved by using the DIE and an additional electric shielding could be evaluated by size-resolved measurements of the hit rate, which is the ratio of laser pulses yielding a detectable amount of ions to the total number of emitted laser pulses. In particular, the hit rate for multiply charged particles smaller than 500 nm is significantly improved by preventing an undesired deflection of these particles in the ion extraction field. Moreover, it was found that by using the DIE the ion yield of the ablation, ionization, and ion extraction process could be increased, resulting in up to 7 times higher signal intensities of the cation spectra. The enhanced ion yield results in a larger effective width of the ablation laser beam, which in turn leads to a hit rate of almost 100 % for PSL particles in the size range from 350 to 2000 nm. Regarding cubic NaCl particles the modifications of the ALABAMA result in an up to 2 times increased detection efficiency and an up to 5 times increased hit rate. The need for such instrument modifications arises in particular for measurements of particles that are present in low number concentrations such as ice-nucleating particles (INPs) in general, but also aerosol particles at high altitudes or in pristine environments. Especially for these low particle number concentrations, improved efficiencies help to overcome the statistical limitations of single-particle mass spectrometer measurements. As an example, laboratory INP measurements carried out in this study show that the application of the DIE alone increases the number of INP mass spectra per time unit by a factor of 2 to 3 for the sampled substances. Overall, the combination of instrument modifications presented here resulted in an increased measurement efficiency of the ALABAMA for different particle types and particles shape as well as for highly charged particles.

Transparent exopolymer particles (TEP) exhibit the properties of gels and are ubiquitously found in the world oceans. Possibly, TEP may enter the atmosphere as part of sea spray aerosol. Here, we report number concentrations of TEP (diameter > 4.5 µm) in ambient aerosol and cloud water samples from the tropical Atlantic Ocean as well as in generated aerosol particles using a plunging waterfall tank that was filled with the ambient sea water. The ambient TEP concentrations ranged between 7 × 102 and 3 × 104 #TEP m−3 in supermicron aerosol particles and correlations to sodium (Na+) and calcium (Ca2+) (R2 = 0.5) suggested some contribution via bubble bursting. Cloud water TEP concentrations were between 4 × 106 and 9 × 106 #TEP L−1 corresponding to equivalent air concentrations of 2–4 × 103 #TEP m−3. The TEP concentrations in the tank-generated aerosol particles, produced from the same waters and sampled with an equivalent system, were significantly lower (4 × 102–2 × 103 #TEP m−3) compared to the ambient concentrations. Based on Na+ concentrations in seawater and in the atmosphere, the enrichment factor for TEP in the atmosphere was calculated. The tank-generated TEP were enriched by a factor of 50 compared to sea water and, therefore, in-line with published enrichment factors for supermicron organic matter in general and TEP specifically. TEP enrichment in the ambient atmosphere was on average 1 × 103 in cloud water and 9 × 103 in ambient aerosol particles and therefore about two orders of magnitude higher than the corresponding enrichment from the tank study. Such high enrichment of supermicron particulate organic constituents in the atmosphere is uncommon and we propose that atmospheric TEP concentrations resulted from a combination of enrichment during bubble bursting transfer from the ocean and TEP in-situ formation in atmospheric phases. Abiotic in-situ formation might have occurred from aqueous reactions of dissolved organic precursors that were present in particle and cloud water samples, while biotic formation involves bacteria, which were abundant in the cloud water samples. The ambient TEP number concentrations were two orders of magnitude higher than recently reported ice nucleating particle (INP) concentrations measured at the same location. As TEP likely possess good properties to act as INP, in future experiments it is worth studying if a certain part of TEP contributes a fraction of the biogenic INP population.

The Cape Verde Atmospheric Observatory (CVAO), which is influenced by both, marine and desert dust air masses, has been used for long-term measurements of different properties of the atmospheric aerosol from 2008 to 2017. These properties include particle number size distributions (PNSD), light absorbing carbon (LAC) and concentrations of cloud condensation nuclei (CCN) together with their hygroscopicity. Here we summarize the results obtained for these properties and use an unsupervised machine learning algorithm for the classification of aerosol types. Five types of aerosols, i.e., marine, freshly-formed, mixture, moderate dust and heavy dust, were classified. Air masses during marine periods are from the Atlantic Ocean and during dust periods are from the Sahara. Heavy dust was more frequently present during wintertime, whereas the clean marine periods were more frequently present during springtime. It was observed that during the dust periods CCN number concentrations at a supersaturation of 0.30 % are roughly 2.5 times higher than during marine periods, but the hygroscopicity (κ) of particles in the size range from ∼30 to ∼175 nm during marine and dust periods are comparable. The long-term data presented here, together with the aerosol classification, can be used as a base to improve our understanding of annual cycles of the atmospheric aerosol in the eastern tropical Atlantic and on aerosol-cloud interactions and it can be used as a base for driving, evaluating and constraining atmospheric model simulations.

In a warming Arctic the increased occurrence of new particle formation (NPF) is believed to originate from the declining ice coverage during summertime. Understanding the physico-chemical properties of newly formed particles, as well as mechanisms that control both particle formation and growth in this pristine environment, is important for interpreting aerosol–cloud interactions, to which the Arctic climate can be highly sensitive. In this investigation, we present the analysis of NPF and growth in the high summer Arctic. The measurements were made on-board research vessel Polarstern during the PS106 Arctic expedition. Four distinctive NPF and subsequent particle growth events were observed, during which particle (diameter in a range 10–50 nm) number concentrations increased from background values of approx. 40 up to 4000 cm−3. Based on particle formation and growth rates, as well as hygroscopicity of nucleation and the Aitken mode particles, we distinguished two different types of NPF events. First, some NPF events were favored by negative ions, resulting in more-hygroscopic nucleation mode particles and suggesting sulfuric acid as a precursor gas. Second, other NPF events resulted in less-hygroscopic particles, indicating the influence of organic vapors on particle formation and growth. To test the climatic relevance of NPF and its influence on the cloud condensation nuclei (CCN) budget in the Arctic, we applied a zero-dimensional, adiabatic cloud parcel model. At an updraft velocity of 0.1 m s−1, the particle number size distribution (PNSD) generated during nucleation processes resulted in an increase in the CCN number concentration by a factor of 2 to 5 compared to the background CCN concentrations. This result was confirmed by the directly measured CCN number concentrations. Although particles did not grow beyond 50 nm in diameter and the activated fraction of 15–50 nm particles was on average below 10 %, it could be shown that the sheer number of particles produced by the nucleation process is enough to significantly influence the background CCN number concentration. This implies that NPF can be an important source of CCN in the Arctic. However, more studies should be conducted in the future to understand mechanisms of NPF, sources of precursor gases and condensable vapors, as well as the role of the aged nucleation mode particles in Arctic cloud formation.

11 pages, supporting information https://doi.org/10.1021/acs.est.9b00991, The radiative balance in the Arctic region is sensitive to in-cloud processes, which principally depend on atmospheric aerosols, including ice nucleating particles (INPs). High temperature INPs (active at ≥−15 °C) are common in the Arctic. While laboratory and limited in situ studies show that the high-temperature active INPs are associated with bioaerosols and biogenic compounds, there is still little quantitative insight into the Arctic biogenic INPs and bioaerosols. We measured concentrations of bioaerosols, bacteria, and biogenic INPs at the Villum Research Station (VRS, Station Nord) in a large number of snow (15) and air (51) samples. We found that INPs active at high subzero temperatures were present both in spring and summer. Air INP concentrations were higher in summer (18 INP m–3 at ≥−10 °C) than in spring (

A consortium of polar scientists combined observational forces in a field campaign of unprecedented complexity to uncover the secrets of clouds and their role in Arctic amplification. Two research aircraft, an icebreaker research vessel, an ice-floe camp including an instrumented tethered balloon, and a permanent ground-based measurement station were employed in this endeavour. Clouds play an important role in Arctic amplification. This term represents the recently observed enhanced warming of the Arctic relative to the global increase of near-surface air temperature. However, there are still important knowledge gaps regarding the interplay between Arctic clouds and aerosol particles, surface properties, as well as turbulent and radiative fluxes that inhibit accurate model simulations of clouds in the Arctic climate system. In an attempt to resolve this so-called Arctic cloud puzzle, two comprehensive and closely coordinated field studies were conducted: the ”Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD)” aircraft campaign, and the ”Physical feedbacks of Arctic boundary layer, Sea ice, Cloud and AerosoL (PASCAL)” ice breaker expedition. Both observational studies were performed in the framework of the German ”ArctiC Amplification:Climate Relevant Atmospheric and SurfaCe Processes, and Feedback Mechanisms (AC)3” project. They took place in the vicinity of Svalbard (Norway) in May and June 2017. ACLOUD and PASCAL explored four pieces of the Arctic cloud puzzle: Cloud properties, aerosol impact on clouds, atmospheric radiation, and turbulent-dynamical processes. The two instrumented Polar 5 and Polar 6 aircraft, the icebreaker research vessel (RV) Polarstern, an ice-floe camp including an instrumented tethered balloon, and the permanent, ground-based measurement station at Ny-Ålesund (Svalbard) were employed to observe Arctic low and mid-level, mixed-phase clouds, and to investigate related atmospheric and surface processes. The Polar 5 aircraft served as a remote sensing observatory examining the clouds from above by downward-looking sensors; the Polar 6 aircraft operated as a flying in-situ measurement laboratory sampling inside and below the clouds. Most of the collocated Polar 5/6 flights were conducted either above RV Polarstern or over the Ny-Ålesund station, both of which monitored the clouds from below using similar but upward-looking remote sensing techniques as the Polar 5 aircraft. Several of the flights were carried out underneath collocated satellite tracks. The paper motivates the scientific objectives of the ACLOUD/PASCAL observations and describes the measured quantities, retrieved parameters, and the applied complementary instrumentation. Furthermore, it discusses selected measurement results, and poses critical research questions to be answered in future papers analyzing the data from the two field campaigns.

The historical development of ice nucleating particle concentrations (NINP) is still unknown. Here, we present for the first time NINP from the past 500 years at two Arctic sites derived from ice core samples. The samples originate from the EUROCORE ice core (Summit, Central Greenland) and from the Lomo09 ice core (Lomonosovfonna, Svalbard). No long term trend is obvious in the measured samples, and the overall range of NINP is comparable to present‐day observations. We observe that the short term variations in NINP is larger than the long‐term variability, but neither anthropogenic pollution nor volcanic eruptions seem to have influenced NINP in the measured temperature range. Shape and onset temperature of several INP spectra suggests that INP of biogenic origin contributed to the Arctic INP population throughout the past

16 pages, 7 figures, 3 tables, supporting information https://pubs.acs.org/doi/10.1021/acsearthspacechem.0c00351.-- All data are available on the public repository PANGAEA: https://doi.pangaea.de/10.1594/PANGAEA.927565 (for aerosol particles) and https://doi.pangaea.de/10.1594/PANGAEA.927566 (for seawater), We present ship-borne and land-based measurements of carbohydrate concentrations and patterns in (i) bulk seawater, (ii) sea surface microlayer (SML), and (iii) atmospheric size-resolved aerosol particles (0.05–10 μm) collected in the Western Antarctic Peninsula. In seawater, we find higher combined carbohydrates (CCHO) in both the particulate (PCCHO, 13–248 μg L–1) and dissolved (DCCHO, 14–294 μg L–1) phases than dissolved free carbohydrates (DFCHO, 1.0–17 μg L–1). Moderate enrichment factors are found in the SML samples (median EFSML = 1.4 for PCCHO, DCCHO, and DFCHO). In PM10 atmospheric particles, combined carbohydrates (CCHOaer,PM10 0.2–11.3 ng m–3) were preferably found in particles of two size modes (0.05–0.42 and 1.2–10 μm) and strongly correlated with Na+aer,PM10 and wind speed, hence suggesting oceanic emission as their primary source. In contrast to SML samples, very high enrichment factors for CCHOaer relative to the bulk water (EFaer) were estimated for supermicron (20–4000) and submicron (40–167 000) particles. Notably, the relative atmospheric aerosol monosaccharide compositions strongly differed from the ones sampled in seawater. The prevalence of bacterial monosaccharides (muramic acid, glucosamine) in aerosol particles allows us to suggest a selective consumption and release of polysaccharides by bacteria in the atmosphere. Our results highlight the need to evaluate the role of different ecosystems as aerosol sources around Antarctica, The authors gratefully acknowledge the funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation, Projektnummer 268020496−TRR 172) within the Transregional Collaborative Research Center “ArctiC Amplification: Climate Relevant Atmospheric and SurfaCe Processes, and Feedback Mechanisms (AC)3” in subprojects B04. Additional support through the Leibniz Association SAW funding of the project “Marine biological production, organic aerosol particles and marine clouds: a Process Chain (MarParCloud)” (SAW-2016-TROPOS-2) is also gratefully acknowledged, With the funding support of the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000928-S), of the Spanish Research Agency (AEI)

Low-level mixed-phase clouds are important factors influencing the energy budget of the Arctic boundary layer. The radiative properties of these clouds are determined by their microphysical properties. Aerosol particles that act as Ice Nucleating Particles (INP), impact the primary ice formation inside clouds and thereby affect cloud lifetime, albedo and precipitation formation. The sources of INP in the Arctic, their properties, nature and concentration are poorly understood which results in substantial uncertainties radiative forcing estimates in climate models.Here, we present ship-based measurements of INP in different environmental compartments (air, sea surface microlayer, bulk sea water, fog water) in the Arctic. From May to July 2017 the PASCAL field campaign took place around and north of Svalbard (up to 84°N, between 0° and 35°E) onboard the RV Polarstern. INP concentrations were measured online with the SPIN instrument (Spectrometer for Ice Nuclei, DMT) and offline through filter sampling and analysis with freezing array techniques. We assess possible connections between the INP in the sea water and air, as well as between INP in the fog water and air through a closure study.Generally, INP concentrations in the Arctic were found to be lower than in mid-latitudes with the exception of elevated INP concentrations at temperatures above -15°C and below -30°C. We attribute elevated INP concentrations to the presence of biogenic, probably proteinaceous INP, at the warmer, and to the presence of mineral dust at colder temperatures, respectively. The closure studies revealed that:a) all INP in the air are activated to fog droplets, and b) the INP concentration in seawater alone cannot explain INP concentration in air without a substantial enrichment of INP (factor 104 to 105) during the transfer of INP from the sea surface to the atmosphere. We present indications for a local, marine source of INP from a case study looking at the period when atmospheric INP concentrations were highest in the temperature range above -15°C. These findings highlight the need for future studies to assess especially the production mechanisms and source strength for Arctic INP.We gratefully acknowledge the funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) – Projektnummer 268020496 – TRR 172, within the Transregional Collaborative Research Center “ArctiC Amplification: Climate Relevant Atmospheric and SurfaCe Processes, and Feedback Mechanisms (AC)3

Concentrations of atmospheric ice nucleating particles (INP) were obtained from weekly filter samples which were collected from May 2019 until March 2020 in southern Chile. Sampling took place at an altitude of 620m above sea level, on top of Cerro Mirador, a mountain directly to the west of Punta Arenas (53°S, 71°W). Additional aerosol properties such as particle number size distributions were measured as well. In parallel, ground-based remote sensing measurements with lidar and cloud radar were made in Punta Arenas.INP concentrations were obtained from washing atmospheric aerosol particles off from deployed polycarbonate filters and subsequent analysis of the samples on two different freezing arrays which were used and described by us earlier (e.g., in Gong et al., 2019 and Hartmann et al., 2020). INP concentrations could be obtained over a broad temperature range from above -5°C down to -25°C.INP concentrations were clearly higher than data obtained for the Southern Ocean region as reported in McCluskey et al. (2018) and Welti et al. (2020). Indeed, they were comparable to concentrations measured at Cape Verde (Gong et al., 2020). INP concentrations obtained during the warm season were spreading over ~ 2 orders of magnitude at any temperature. Data obtained for the cold season almost all were at the upper end of the observed INP concentration range, with only one weekly sample featuring low concentrations.Heating of the samples was also applied, and the heated samples had clearly lower INP concentrations across the examined temperatures, implying a biological fraction among the INP of ~ 80%. Therefore, local terrestrial sources may be the source of the observed INP.The assumption of local terrestrial sources is strengthened by a case study. For that, two subsequent samples obtained during the cold season were examined in more detail. These were the one sample with low INP concentrations which was obtained during the cold season during the week from August 14 to August 22, and the subsequent sample collected from August 22 to August 29, which was amongst the highest samples. Backward trajectories together with an analysis of Lidar data showed that the low INP concentrations were obtained for a time during which air masses predominantly came in from the south with little contact to land and for calm weather conditions. Conditions were not as stable during the following week which featured air masses mostly coming in from the north-west. The aerosol backscatter coefficient at the height level of the in-situ measurements was obtained from lidar observations for both weeks and shows about 50 % lower aerosol load for the first week, when INP concentrations were low.All of this hints to local terrestrial sources for the observed highly ice active biogenic INP. Literature:Gong et al. (2019), Atmos. Chem. Phys., 19, 10883-10900, doi:10.5194/acp-19-10883-2019.Gong et al. (2020), Atmos. Chem. Phys., 20, 1451-1468, doi:10.5194/acp-20-1451-2020.Hartmann et al. (2020), Geophys. Res. Lett., 47, doi:10.1029/2020GL087770.McCluskey et al. (2018), Geophys. Res. Lett., 45, doi:10.1029/2018gl079981.Welti et a. (2020), Atmos. Chem. Phys. 20, doi:10.5194/acp-2020-466.

Measurements of lipids as representative species for different lipid classes in the marine environment have been performed to characterize their oceanic sources and their transfer from the ocean into the atmosphere to marine aerosol particles. To this end, a set of lipid classes (hydrocarbons (HC), fatty acid methyl esters (ME), free fatty acids (FFA), alcohols (ALC), 1,3-diacylglycerols (1,3 DG), 1,2-diacylglycerols (1,2 DG), monoacylglycerols (MG), wax esters (WE), triacylglycerols (TG), phospholipids (PP) including phosphatidylglycerols (PG), phosphatidylethanolamine (PE), phosphatidylcholines (PC), glycolipids (GL) including sulfoquinovosyldiacylglycerols (SQDG), monogalactosyl-diacylglycerols (MGDG), digalactosyldiacylglycerols (DGDG) and sterols (ST)) is investigated in both the dissolved and particulate fraction in seawater, differentiated between underlying water (ULW) and the sea surface microlayer (SML), and in ambient submicron aerosol particle samples (PM1) at the Cape Verde Atmospheric Observatory (CVAO) applying concerted measurements. The different lipids are found in all marine compartments but in different compositions. At this point, a certain variability is observed for the concentration of dissolved (∑DLULW: 39.8–128.5 μg L−1, ∑DLSML: 55.7–121.5 μg L−1) and particulate (∑PLULW: 36.4–93.5 μg L−1, ∑PLSML: 61.0–118.1 μg L−1) lipids in seawater of the tropical North Atlantic Ocean along the campaign. Only slight SML enrichments are observed for the lipids with an enrichment factor EFSML of 1.1–1.4 (DL) and 1.0–1.7 (PL). On PM1 aerosol particles, a total lipid concentration between 75.2–219.5 ng m−3 (averaged: 119.9 ng m−3) is measured with high atmospheric concentration of TG (averaged: 21.9 ng m−3) as a potential indicator for freshly emitted sea spray. Besides phytoplankton sources, bacteria influence the lipid concentrations in seawater and on the aerosol particles, so that the phytoplankton tracer (chlorophyll-a) cannot sufficiently explain the lipid abundance. The concentration and enrichment of lipids in the SML is not related to physicochemical properties describing the surface activity. For aerosol, however, the high enrichment of lipids (as a sum) corresponds well with the consideration of their high surface activity, thus the EFaer (enrichment factor on submicron aerosol particles compared to SML) ranges between 9 × 104–7 × 105. Regarding the single lipid groups on the aerosol particles, a weak relation between EFaer and lipophilicity (expressed by the KOW value) was identified, which was absent for the SML. However, overall simple physico-chemical descriptors are not sufficient to fully explain the transfer of lipids. As our findings show that additional processes such as formation and degradation influence the ocean-atmosphere transfer of both OM in general and of lipids in particular, they have to be considered in OM transfer models. Moreover, our data suggest that the extend of enrichment of lipid classes constituents on the aerosol particles might be related to the distribution of the lipid within the bubble-air-water-interface. Lipids, which are preferably arranged within the bubble interface, namely TG and ALC, are transferred to the aerosol particles to the highest extend. Finally, the connection between ice nucleation particles (INP) in seawater, which are active already at higher temperatures (−10 °C to −15 °C), and the lipid classes PE and FFA suggests that lipids formed in the ocean have the potential to contribute to (biogenic) INP activity when transferred to the atmosphere.

Ice nucleating particles (INPs) initiate the primary ice formation in clouds at temperatures above ca. −38° C and have an impact on precipitation formation, cloud optical properties and cloud persistence. Despite their roles in both weather and climate, INPs are not well characterized, especially in remote regions such as the Arctic. We present results from a ship-based campaign to the European Arctic in May to July 2017. We deployed a filter sampler and a continuous flow diffusion chamber for off- and online INP analysis, respectively. We also investigated the ice nucleation properties of samples from different environmental compartments, i.e., the sea surface microlayer (SML), the bulk seawater (BSW), and fog water. Concentrations of INP (NINP) in the air vary between two to three orders of magnitudes at any particular temperature and are, except for the temperatures above −10° C and below −32° C, lower than in mid-latitudes. In these temperature ranges INP concentrations are the same or even higher than in the mid-latitudes. Heating of the filter samples to 95° C for 1 hour we found a significant reduction in ice nucleation activity, i.e., indications that the INPs active at warmer temperatures are biogenic. At colder temperatures the INP population was likely dominated by mineral dust. The SML was found to be enriched in INP compared to the BSW in almost all samples. The enrichment factor (EF) varied mostly between 1 and 10, but EFs as high as 94.97 were also observed. Filtration of the seawater samples with 0.2 µm syringe filters lead to a significant reduction in ice activity, indicating the INPs are larger, and/or are associated with particles larger than 0.2 µm. A closure study showed that aerosolization of SML and/or seawater alone cannot explain the observed air-borne NINP unless significant enrichment of INP by a factor of 105 takes place during the transfer from the ocean surface to the atmosphere. In the fog water samples with −3.47° C we observed the highest freezing onset of any sample. A closure study connecting NINP in fog water and the ambient NINP derived from the filter samples shows good agreement of the concentrations in both compartments, which indicates that INPs in the air are likely all activated into fog droplets during fog events. In a case study we considered a situation during which the ship was located in the marginal sea ice zone and NINP in air and the SML were highest in the temperature range above −10° C. Chlorophyll-a measurements by satellite remote sensing point towards the waters in the investigated region being biologically active. Heat induced reduction of ice nucleating ability indicated the biogenic nature of the air-borne INPs. Similar slopes in the temperature spectra suggested a connection between the INP populations in the SML and the air. Air mass history had no influence on the observed air-borne INP population. Therefore, we conclude that during the case study collected air-borne INPs originated from a local biogenic probably marine source.

The aim of this study is to show how a newly developed aerodynamic lens system (ALS), a delayed ion extraction (DIE) and better electric shielding improve the efficiency of the Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA). These improvements are applicable to single particle laser ablation mass spectrometers in general. To characterize the modifications extensive size-resolved measurements with spherical polystyrene latex particles (PSL; 150–000 nm) and cubic sodium chloride particles (NaCl; 400–1700 nm) were performed. Measurements at a fixed ALS position show an improved detectable particle size range of the new ALS compared to the previously used Liu-type ALS, especially for super-micron particles. At a lens pressure of 2.4 hPa, the new ALS achieves a PSL particle size range from 230 nm to 3240 nm with 50 % detection efficiency and between 350 nm and 2000 nm with 95 % detection efficiency. The particle beam divergence was determined by measuring the detection efficiency at variable ALS positions along the laser cross sections and found to be minimal for PSL at about 800 nm. Compared to measurements of SPMS instruments using Liu-type ALSs, the minimum particle beam divergence is shifted towards larger particle sizes. However, there are no disadvantages compared to the Liu-type lenses for particle sizes down to 200 nm. Improvements achieved by using the DIE and an additional electric shielding could be evaluated by size-resolved measurements of the hit rate, which is the ratio of laser pulses yielding a detectable amount of ions to the total number of emitted laser pulses. In particular, the hit rate for multiply charged particles smaller 500 nm is significantly improved by preventing an undesired deflection of these particles in the ion extraction field. Moreover, it was found that by using the DIE the ion yield of the ablation, ionization and ion extraction process could be increased, resulting in up to seven times higher signal intensities of the cation spectra. The enhanced ion yield results in a larger effective width of the ablation laser beam, which in turn leads to a hit rate of almost 100 % for PSL particles in the size range from 350 nm to 2000 nm. Regarding cubic NaCl particles the modifications of the ALABMA result in a up to two times increased detection efficiency and a up to five times increased hit rate. The need for such instrument modifications arises in particular for measurements of particles that are present in low number concentrations such as ice nucleation particles (INP) in general, but also aerosol particles at high altitudes or in pristine environments. Especially for these low particle number concentrations improved efficiencies help to overcome statistical limitations of single particle mass spectrometer measurements. As an example laboratory INP measurements carried out in this study show that the application of the DIE alone increases the number of INP mass spectra per time unit by a factor of two to three for the sampled substances. Overall, the combination of instrument modifications presented here resulted in an increased measurement efficiency of the ALABAMA for different particle types, particles shapes and for highly charged particles.

The project MarParCloud (marine biological production, organic aerosol particles and marine clouds: a process chain) aims at achieving a better understanding of the biological production of organic matter (OM)in the oceans, its export into marine aerosol particles and finally its ability to act as ice and cloud condensation nuclei (INP and CCN). The core of MarParCloud comprised a field campaign at the Cape Verde Atmosphere Observatory (CVAO) in autumn 2017, where a variety of chemical, physical, biological and meteorological approaches were applied. The investigations included concerted measurements of the bulk water, the Sea Surface Microlayer (SML), ambient aerosol particles on the ground (30 m a.s.l.) and in mountain heights (744 m) as well as cloud water. Important aspects of the ocean atmosphere Interactions focusing on marine OM have been addressed through detailed observation and modeling approaches.Key variables comprised the chemical characterization of the atmospherically relevant OM components (e.g. lipids, proteins, sugars) in the ocean and the atmosphere as well as measurements of INP and CCN. Moreover, bacterial cell counts, mercury species and trace gases were analysed. To interpret the results, the measurements were accompanied by various auxiliary parameters such as air mass back trajectory analysis, vertical atmospheric profile analysis, cloud observations and pigment measurements in seawater. Additional modelling studies supported the experimental analysis.Here we show the proof of concept of the connection between organic matter emission from the ocean to the atmosphere and up to the cloud level. A link between the ocean and the atmosphere was clearly observed as (i) the particles measured at the surface are well mixed within the marine boundary layer up to cloud level and (ii) ocean-derived compounds can be found in the aerosol particles at mountain height and in the cloud water. The organic measurements will be implemented in a new source function for the oceanic emission of OM. However, from a perspective of particle number concentrations, the marine contributions to both CCN and INP are rather limited.

Ice-nucleating particles (INPs) associated with fresh waters are a neglected, but integral component of the water cycle. Abundant INPs were identified from surface waters of both the Maumee River and Lake Erie with ice nucleus spectra spanning a temperature range from −3 to −15 °C. The majority of river INPs were submicron in size and attributed to biogenic macromolecules, inferred from the denaturation of ice-nucleation activity by heat. In a watershed dominated by row-crop agriculture, higher concentrations of INPs were found in river samples compared to lake samples. Further, ice-nucleating temperatures differed between river and lake samples, which indicated different populations of INPs. Seasonal analysis of INPs that were active at warmer temperatures (≥−10 °C; INP–10) showed their concentration to correlate with river discharge, suggesting a watershed origin of these INPs. A terrestrial origin for INPs in the Maumee River was further supported by a correspondence between the ice-nucleation signatur...

Our current understanding of the importance of surface-active substances (SAS) on atmospheric aerosol cloud-forming efficiency is limited, as explicit data on the content of size-resolved ambient aerosol SAS, which are responsible for lowering the surface tension (σ) of activating droplets, are not available. We report on the first data comprising seasonal variability of size-segregated SAS concentrations in ambient aerosol particulate matter (PM). To assess the impact of SAS distribution within PM on cloud droplet activation and growth, a concept of surfactant activity was adopted and a parametrization developed ; i.e., surfactant activity factor (SAF) was defined, which allowed translation of experimental data for use in cloud parcel modeling. The results show that SAS-induced σ depression during cloud activation may affect droplet number ( Nd) as much as a 2-fold increase in particle number, whereas by considering also the size distribution of particulate SAS, Nd may increase for another 10%. This study underscores the importance of size-resolved SAS perspective on cloud activation, as data typically obtained from aqueous extracts of PM2.5 and PM10 may result in misleading conclusions about droplet growth due to large mass fractions of supermicron particles with SAS deficit and little or no influence on CCN and Nd.

Within the framework of the RACEPAC (Radiation–Aerosol–Cloud Experiment in the Arctic Circle) project, the Arctic aerosol, arriving at a ground-based station in Tuktoyaktuk (Mackenzie River delta area, Canada), was characterized during a period of 3 weeks in May 2014. Basic meteorological parameters and particle number size distributions (PNSDs) were observed and two distinct types of air masses were found. One type were typical Arctic haze air masses, termed accumulation-type air masses, characterized by a monomodal PNSD with a pronounced accumulation mode at sizes above 100 nm. These air masses were observed during a period when back trajectories indicate an air mass origin in the north-east of Canada. The other air mass type is characterized by a bimodal PNSD with a clear minimum around 90 nm and with an Aitken mode consisting of freshly formed aerosol particles. Back trajectories indicate that these air masses, termed Aitken-type air masses, originated from the North Pacific. In addition, the application of the PSCF receptor model shows that air masses with their origin in active fire areas in central Canada and Siberia, in areas of industrial anthropogenic pollution (Norilsk and Prudhoe Bay Oil Field) and the north-west Pacific have enhanced total particle number concentrations (NCN). Generally, NCN ranged from 20 to 500 cm−3, while cloud condensation nuclei (CCN) number concentrations were found to cover a range from less than 10 up to 250 cm−3 for a supersaturation (SS) between 0.1 and 0.7 %. The hygroscopicity parameter κ of the CCN was determined to be 0.23 on average and variations in κ were largely attributed to measurement uncertainties. Furthermore, simultaneous PNSD measurements at the ground station and on the Polar 6 research aircraft were performed. We found a good agreement of ground-based PNSDs with those measured between 200 and 1200 m. During two of the four overflights, particle number concentrations at 3000 m were found to be up to 20 times higher than those measured below 2000 m; for one of these two flights, PNSDs measured above 2000 m showed a different shape than those measured at lower altitudes. This is indicative of long-range transport from lower latitudes into the Arctic that can advect aerosol from different regions in different heights.

Ice crystal formation in atmospheric clouds has a strong effect on precipitation, cloud lifetime, cloud radiative properties, and thus the global energy budget. Primary ice formation above 235 K is initiated by nucleation on seed aerosol particles called ice-nucleating particles (INPs). Instruments that measure the ice-nucleating potential of aerosol particles in the atmosphere need to be able to accurately quantify ambient INP concentrations. In the last decade several instruments have been developed to investigate the ice-nucleating properties of aerosol particles and to measure ambient INP concentrations. Therefore, there is a need for intercomparisons to ensure instrument differences are not interpreted as scientific findings. In this study, we intercompare the results from parallel measurements using four online ice nucleation chambers. Seven different aerosol types are tested including untreated and acid-treated mineral dusts (microcline, which is a K-feldspar, and kaolinite), as well as birch pollen washing waters. Experiments exploring heterogeneous ice nucleation above and below water saturation are performed to cover the whole range of atmospherically relevant thermodynamic conditions that can be investigated with the intercompared chambers. The Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the Portable Immersion Mode Cooling chAmber coupled to the Portable Ice Nucleation Chamber (PIMCA-PINC) performed measurements in the immersion freezing mode. Additionally, two continuous-flow diffusion chambers (CFDCs) PINC and the Spectrometer for Ice Nuclei (SPIN) are used to perform measurements below and just above water saturation, nominally presenting deposition nucleation and condensation freezing. The results of LACIS and PIMCA-PINC agree well over the whole range of measured frozen fractions (FFs) and temperature. In general PINC and SPIN compare well and the observed differences are explained by the ice crystal growth and different residence times in the chamber. To study the mechanisms responsible for the ice nucleation in the four instruments, the FF (from LACIS and PIMCA-PINC) and the activated fraction, AF (from PINC and SPIN), are compared. Measured FFs are on the order of a factor of 3 higher than AFs, but are not consistent for all aerosol types and temperatures investigated. It is shown that measurements from CFDCs cannot be assumed to produce the same results as those instruments exclusively measuring immersion freezing. Instead, the need to apply a scaling factor to CFDCs operating above water saturation has to be considered to allow comparison with immersion freezing devices. Our results provide further awareness of factors such as the importance of dispersion methods and the quality of particle size selection for intercomparing online INP counters. ISSN:1680-7375 ISSN:1680-7367

Ice nucleating particles (INPs) in the troposphere can form ice in clouds via heterogeneous ice nucleation. Yet, atmospheric number concentrations of INPs (NINP) are not well characterized and although there is some understanding of their sources, it is still unclear to what extend different sources contribute, nor if all sources are known. In this work, we examined properties of INPs at Cape Verde from different sources, the oceanic sea surface microlayer (SML) and underlying water (ULW), the atmosphere close to both sea and cloud level as well as cloud water. Both enrichment and depletion of NINP in SML compared to ULW were observed. The enrichment factor (EF) varied from roughly 0.4 to 11, and there was no clear trend in EF with temperature. NINP in PM10 sampled at Cape Verde Atmospheric Observatory (CVAO) at any particular temperature spanned around 1 order of magnitude below −15 °C, and about 2 orders of magnitude at warmer temperatures (>−12 °C). NINP in PM1 were generally lower than those in PM10 at CVAO. About 83 ± 22 %, 67 ± 18 % and 77 ± 14 % (median ± standard deviation) of INPs had a diameter > 1 µm at ice activation temperatures of −12, −15, and −18 °C, respectively. Among the 17 PM10 samples at CVAO, three PM10 filters showed elevated NINP at warm temperatures, e.g., above 0.01 std L−1 at −10 °C. However, for NINP in PM1 at CVAO, this is not the case. At these higher temperatures, often biological particles have been found to be ice active. Consequently, the difference in NINP between PM1 and PM10 at CVAO, suggests that biological ice active particles were present in the super-micron size range. NINP in PM10 at CVAO was found to be similar to that on Monte Verde (MV, at 744 m a.s.l.) during non-cloud events. During cloud events, most INPs on MV were activated to cloud droplets. When highly ice active particles were present in PM10 filters at CVAO, they were not observed in PM10 filters on MV, but in cloud water samples, instead. This is direct evidence that these INPs which are likely biological are activated to cloud droplets during cloud events. In general, Cape Verde was often affected by dust from the Saharan desert during our measurement. For the observed air masses, atmospheric NINP in air fit well to the concentrations observed in cloud water. When comparing concentrations of both sea salt and INPs in both seawater and PM10 filters, it can be concluded that sea spray aerosol (SSA) only contributed a minor fraction to the atmospheric NINP. Therefore it can be said that, unless there would be a significant enrichment of NINP during the formation of SSA particles, NINP was mainly dominated by mineral dust at cold temperatures with few contributions from possible biological particles at warmer temperatures.

In a warming Arctic the increased occurrence of new particle formation (NPF) is believed to originate from the declining ice coverage during summertime. Understanding the physico-chemical properties of newly formed particles, as well as mechanisms that control both particle formation and growth in this pristine environment is important for interpreting aerosol-cloud interactions, to which the Arctic climate can be highly sensitive. In this investigation, we present the analysis of NPF and growth in the high summer Arctic. The measurements have been done on-board Research Vessel Polarstern during the PS106 Arctic expedition. Four distinctive NPF and subsequent particle growth events were observed, during which particle (diameter in a range 10–50 nm) number concentrations increased from background values of approx. 40 up to 4000 cm-3. Based on particle formation and growth rates, as well as hygroscopicity of nucleation and the Aitken mode particles, we distinguished two different types of NPF events. First, some NPF events were favored by negative ions, resulting in more-hygroscopic nucleation mode particles and suggesting sulfuric acid as a precursor gas. Second, other NPF events resulted in less-hygroscopic particles, indicating the influence of organic vapors on particle formation and growth. To test the climatic relevance of NPF and its influence on the cloud condensation nuclei (CCN) budget in the Arctic, we applied a zero-dimensional, adiabatic cloud parcel model. At an updraft velocity of 0.1 m s-1, the particle number size distribution (PNSD) generated during nucleation processes resulted in an increase of the CCN number concentration by a factor of 2 to 5, compared to the background CCN concentrations. This result was confirmed by the directly measured CCN number concentrations. Although particles did not grow beyond 50 nm in diameter and the activated fraction of 15–50 nm particles was on average below 10 %, it could be shown that the sheer number of particles produced by the nucleation process is enough to significantly influence the background CCN number concentration. It implies that NPF can be an important source of CCN in the Arctic. However, more studies should be conducted in the future to understand mechanisms of NPF, sources of precursor gases and condensable vapors, as well as the role of the aged nucleation mode particles on Arctic cloud formation.