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Ice-nucleating particles (INPs) have an important function in the freezing of clouds, but are rare in East Antarctica with concentrations between 6×10-6 L-1 and 5×10-3 L-1 observed at the Belgian Princess Elisabeth Station. These low concentrations offer a possible explanation for the occurrence of supercooled liquid water in clouds observed using the station's Micro Rain Radar and Ceilometer. 5 We used COSMO-CLM2 with an added aerosol-cycle module to test the cloud phase's sensitivity in response to varying prescribed INP concentrations. We tested two cases, one in austral summer, one in austral winter, and analysed the differences resulting from INP concentration changes for an area around the station and over the Southern Ocean within the selected domain. Our results show a strong influence of the INP concentration on the liquid water path in both regions, with higher concentrations reducing the amount of liquid water. Over the ocean, this effect is stronger during winter: During summer, a significant portion of water remains in liquid state regardless of INP concentration. Over the continent, this effect is stronger during summer: Temperatures in winter frequently fall below -37°C, allowing homogeneous freezing. The largest increase of the liquid water fraction of total cloud hydrometeor mass is simulated over the ocean in winter, from 9.8 % in the highest tested INP concentration to 50.3 % in the lowest. The radiative effects caused by the INP concentration changes are small with less than 3 Wm-2 difference in the averages between different concentrations. [ABSTRACT FROM AUTHOR]

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 consisting of a sampling unit and a powerful pump unit, and it 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 remote-controlled via software so that manual filter changes during 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 presenting the design and principle of operation of HERA, this paper describes 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 to 800 nm) or flow rate (10 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 collection 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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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-year-long 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. [ABSTRACT FROM AUTHOR]

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 life time 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, two-year-long INP measurements (from July 2018 to September 2020) at Villum 5 Research Station (VRS) in Northern Greenland are presented. A low-volume filter sampler was deployed to collect filter samples for off-line INP analysis. An annual cycle of INP concentration (NINP) was observed and the fraction of biogenic INPs was found to be higher in snow-free months and lower in months when the surface was snow-covered. 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 10 of the year. Winter and summer type 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. NINP in the case study period revealed no clear dependency on either meteorological parameters or different surface types which were passed 15 by the collected air masses. Overall, the results suggest that the coastal regions of Greenland were main sources of INPs in April 2019 and 2020, most likely including both local terrestrial and marine sources. 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. [ABSTRACT FROM AUTHOR]

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>500nm) from the global average overestimates the measured INP, but the parameterization representing biological particles from a forestry environment 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. [ABSTRACT FROM AUTHOR]

Transparent exopolymer particles (TEPs) exhibit the properties of gels and are ubiquitously found in the world oceans. TEPs may enter the atmosphere as part of sea-spray aerosol. Here, we report number concentrations of TEPs with a diameter > 4.5 µ m, hence covering a part of the supermicron particle range, 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 seawater. The ambient TEP concentrations ranged between 7×102 and 3×104 #TEP m -3 in the aerosol particles and correlations with 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 and, according to the measured cloud liquid water content, corresponding to equivalent air concentrations of 2– 4×103 #TEP m -3. Based on Na+ concentrations in seawater and in the atmosphere, the enrichment factors for TEPs in the atmosphere were calculated. The tank-generated TEPs were enriched by a factor of 50 compared with seawater and, therefore, in-line with published enrichment factors for supermicron organic matter in general and TEPs 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 a secondary 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, whereas 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 TEPs likely possess good properties to act as INPs, in future experiments it is worth studying if a certain part of TEPs contributes a fraction of the biogenic INP population. [ABSTRACT FROM AUTHOR]

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 Desert. 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 % were 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 were comparable. The long-term data presented here, together with the aerosol classification, can be used as a basis to improve our understanding of annual cycles of the atmospheric aerosol in the eastern tropical Atlantic Ocean and on aerosol-cloud interactions and it can be used as a basis for driving, evaluating and constraining atmospheric model simulations. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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 µ m 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 µ m. 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. [ABSTRACT FROM AUTHOR]

In the marine environment, measurements of lipids as representative species within different lipid classes have been performed to characterize their oceanic sources and their transfer from the ocean into the atmosphere to marine aerosol particles. The set of lipid classes includes 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); and phospholipids (PP) including phosphatidylglycerols (PG), phosphatidylethanolamine (PE), phosphatidylcholines (PC), as well as glycolipids (GL) which cover sulfoquinovosyldiacylglycerols (SQDG), monogalactosyl-diacylglycerols (MGDG), digalactosyldiacylglycerols (DGDG) and sterols (ST). These introduced lipid classes have been analyzed in the dissolved and particulate fraction of seawater, differentiating between underlying water (ULW) and the sea surface microlayer (SML) on the one hand. On the other hand, they have been examined on ambient submicrometer aerosol particle samples (PM 1) which were collected at the Cape Verde Atmospheric Observatory (CVAO) by applying concerted measurements. These different lipids are found in all marine compartments but in different compositions. Along the campaign, certain variabilities are observed for the concentration of dissolved (∑ DL ULW : 39.8–128.5 µgL-1 , ∑ DL SML : 55.7–121.5 µgL-1) and particulate (∑ PL ULW : 36.4–93.5 µgL-1 , ∑ PL SML : 61.0–118.1 µgL-1) lipids in the seawater of the tropical North Atlantic Ocean. Only slight SML enrichments are observed for the lipids with an enrichment factor EF SML of 1.1–1.4 (DL) and 1.0–1.7 (PL). On PM 1 aerosol particles, a total lipid concentration between 75.2–219.5 ng m -3 (averaged: 119.9 ng m -3) is measured. As also bacteria – besides phytoplankton sources – influence the lipid concentrations in seawater and on the aerosol particles, the lipid abundance cannot be exclusively explained by the phytoplankton tracer (chlorophyll a). The concentration and enrichment of lipids in the SML are not related to physicochemical properties which describe the surface activity. On the aerosol particles, an EF aer (the enrichment factor on the submicrometer aerosol particles compared to the SML) between 9×104 – 7×105 is observed. Regarding the individual lipid groups on the aerosol particles, a statistically significant correlation (R2=0.45 , p=0.028) was found between EF aer and lipophilicity (expressed by the KOW value), which was not present for the SML. But simple physicochemical descriptors are overall 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 extent of the enrichment of the lipid class constituents on the aerosol particles might be related to the distribution of the lipid within the bubble–air–water interface. The lipids TG and ALC which are preferably arranged within the bubble interface are transferred to the aerosol particles to the highest extent. Finally, the connection between ice nucleation particles (INPs) in seawater, which are already active at higher temperatures (-10 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 into the atmosphere. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The project MarParCloud (Marine biological production, organic aerosol Particles and marine Clouds: a process chain) aims to improve our understanding of the genesis, modification and impact of marine organic matter (OM) from its biological production, to its export to marine aerosol particles and, finally, to its ability to act as ice-nucleating particles (INPs) and cloud condensation nuclei (CCN). A field campaign at the Cape Verde Atmospheric Observatory (CVAO) in the tropics in September–October 2017 formed the core of this project that was jointly performed with the project MARSU (MARine atmospheric Science Unravelled). A suite of chemical, physical, biological and meteorological techniques was applied, and comprehensive measurements of bulk water, the sea surface microlayer (SML), cloud water and ambient aerosol particles collected at a ground-based and a mountain station took place. Key variables comprised the chemical characterization of the atmospherically relevant OM components in the ocean and the atmosphere as well as measurements of INPs and CCN. Moreover, bacterial cell counts, mercury species and trace gases were analyzed. 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 modeling studies supported the experimental analysis. During the campaign, the CVAO exhibited marine air masses with low and partly moderate dust influences. The marine boundary layer was well mixed as indicated by an almost uniform particle number size distribution within the boundary layer. Lipid biomarkers were present in the aerosol particles in typical concentrations of marine background conditions. Accumulation- and coarse-mode particles served as CCN and were efficiently transferred to the cloud water. The ascent of ocean-derived compounds, such as sea salt and sugar-like compounds, to the cloud level, as derived from chemical analysis and atmospheric transfer modeling results, denotes an influence of marine emissions on cloud formation. Organic nitrogen compounds (free amino acids) were enriched by several orders of magnitude in submicron aerosol particles and in cloud water compared to seawater. However, INP measurements also indicated a significant contribution of other non-marine sources to the local INP concentration, as (biologically active) INPs were mainly present in supermicron aerosol particles that are not suggested to undergo strong enrichment during ocean–atmosphere transfer. In addition, the number of CCN at the supersaturation of 0.30 % was about 2.5 times higher during dust periods compared to marine periods. Lipids, sugar-like compounds, UV-absorbing (UV: ultraviolet) humic-like substances and low-molecular-weight neutral components were important organic compounds in the seawater, and highly surface-active lipids were enriched within the SML. The selective enrichment of specific organic compounds in the SML needs to be studied in further detail and implemented in an OM source function for emission modeling to better understand transfer patterns, the mechanisms of marine OM transformation in the atmosphere and the role of additional sources. In summary, when looking at particulate mass, we see oceanic compounds transferred to the atmospheric aerosol and to the cloud level, while from a perspective of particle number concentrations, sea spray aerosol (i.e., primary marine aerosol) contributions to both CCN and INPs are rather limited. [ABSTRACT FROM AUTHOR]

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 or if all sources are known. In this work, we examined properties of INPs at Cabo Verde (a.k.a. Cape Verde) from different environmental compartments: the oceanic sea surface microlayer (SML), underlying water (ULW), cloud water and the atmosphere close to both sea level and cloud level. 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 ice-nucleation temperature. NINP values in PM 10 sampled at Cape Verde Atmospheric Observatory (CVAO) at any particular ice-nucleation temperature spanned around 1 order of magnitude below -15 ∘ C, and about 2 orders of magnitude at warmer temperatures (>-12 ∘ C). Among the 17 PM 10 samples at CVAO, three PM 10 filters showed elevated NINP at warm temperatures, e.g., above 0.01 L -1 at -10 ∘ C. After heating samples at 95 ∘ C for 1 h, the elevated NINP at the warm temperatures disappeared, indicating that these highly ice active INPs were most likely biological particles. INP number concentrations in PM 1 were generally lower than those in PM 10 at CVAO. About 83±22 %, 67±18 % and 77±14 % (median ± standard deviation) of INPs had a diameter >1 µ m at ice-nucleation temperatures of -12 , -15 and -18 ∘ C, respectively. PM 1 at CVAO did not show such elevated NINP at warm temperatures. Consequently, the difference in NINP between PM 1 and PM 10 at CVAO suggests that biological ice-active particles were present in the supermicron size range. NINP in PM 10 at CVAO was found to be similar to that on Monte Verde (MV, at 744 m a.s.l.) during noncloud events. During cloud events, most INPs on MV were activated to cloud droplets. When highly ice active particles were present in PM 10 filters at CVAO, they were not observed in PM 10 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. For the observed air masses, atmospheric NINP values in air fit well to the concentrations observed in cloud water. When comparing concentrations of both sea salt and INPs in both seawater and PM 10 filters, it can be concluded that sea spray aerosol (SSA) only contributed a minor fraction to the atmospheric NINP. This latter conclusion still holds when accounting for an enrichment of organic carbon in supermicron particles during sea spray generation as reported in literature. [ABSTRACT FROM AUTHOR]

In the framework of the MarParCloud (Marine biological production, organic aerosol particles and marine clouds: a Process Chain) project, measurements were carried out on the islands of Cabo Verde (a.k.a. Cape Verde) to investigate the abundance, properties and sources of aerosol particles in general, and cloud condensation nuclei (CCN) in particular, both close to sea level and at the cloud level. A thorough comparison of particle number concentration (PNC), particle number size distribution (PNSD) and CCN number concentration (NCCN) at the Cape Verde Atmospheric Observatory (CVAO, sea-level station) and Monte Verde (MV, cloud-level station) reveals that during times without clouds the aerosols at CVAO and MV are similar and the boundary layer is generally well mixed. Therefore, data obtained at CVAO can be used to describe the aerosol particles at cloud level. Cloud events were observed at MV during roughly 58 % of the time, and during these events a large fraction of particles was activated to cloud droplets. A trimodal parameterization method was deployed to characterize PNC at CVAO. Based on number concentrations in different aerosol modes, four well-separable types of PNSDs were found, which were named the marine type, mixture type, dust type1 and dust type2. Aerosol particles differ depending on their origins. When the air masses came from the Atlantic Ocean, sea spray can be assumed to be one source for particles besides new particle formation. For these air masses, PNSDs featured the lowest number concentration in Aitken, accumulation and coarse modes. Particle number concentrations for sea spray aerosol (SSA, i.e., the coarse mode for these air masses) accounted for about 3.7 % of NCCN,0.30% (CCN number concentration at 0.30 % supersaturation) and about 1.1 % to 4.4 % of Ntotal (total particle number concentration). When the air masses came from the Sahara, we observed enhanced Aitken, accumulation and coarse mode particle number concentrations and overall increased NCCN ; NCCN,0.30% during the strongest observed dust periods is about 2.5 times higher than that during marine periods. However, the particle hygroscopicity parameter κ for these two most different periods shows no significant difference and is generally similar, independent of air mass. Overall, κ averaged 0.28, suggesting the presence of organic material in particles. This is consistent with previous model work and field measurements. There is a slight increase in κ with increasing particle size, indicating the addition of soluble, likely inorganic, material during cloud processing. [ABSTRACT FROM AUTHOR]

The project MarParCloud (Marine biological production, organic aerosol Particles and marine Clouds: a process chain) aims at improving our understanding of the genesis, modification and impact of marine organic matter (OM), from its biological production, via its export to marine aerosol particles and, finally, towards its ability to act as ice nucleating particles (INP) and cloud condensation nuclei (CCN). A field campaign at the Cape Verde Atmospheric Observatory (CVAO) in the tropics in September/October 2017 formed the core of this project that was jointly performed with the project (MARine atmospheric Science Unravelled). A suite of chemical, physical, biological and meteorological techniques was applied and comprehensive measurements of bulk water, the sea surface microlayer (SML), cloud water and ambient aerosol particles collected at a ground-based and a mountain station took place. Key variables comprised the chemical characterization of the atmospherically relevant OM components 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. During the campaign, the CVAO exhibited marine air masses with low and partly moderate dust influences. The marine boundary layer was well mixed as indicated by an almost uniform particle number size distribution within the boundary layer. Lipid biomarkers were present in the aerosol particles in typical concentrations of marine background conditions. Accumulation and coarse mode particles served as CCN and were efficiently transferred to the cloud water. The ascent of ocean-derived compounds, such as sea salt and sugar-like compounds, to the cloud level as derived from chemical analysis and atmospheric transfer modelling results denote an influence of marine emissions on cloud formation. However, INP measurements indicated also a significant contribution of other non-marine sources to the local INP concentration or strong enrichment processes during upward transport. Lipids, sugar-like compounds, UV absorbing humic-like substances and low molecular weight neutral components were important organic compounds in the seawater and highly surface-active lipids were enriched within the SML. The selective enrichment of specific organic compounds in the SML needs to be studied in further detail and implemented in an OM source function for emission modelling to better understand transfer patterns, mechanisms of marine OM transformation in the atmosphere and the role of additional sources. In summary, when looking at particulate mass, we do see oceanic compounds transferred to the atmospheric aerosol and to the cloud level, while from a perspective of particle number concentrations, marine contributions to both CCN and INP are rather limited. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

As part of the A-LIFE (Absorbing aerosol layers in a changing climate: aging, LIFEtime and dynamics) campaign, ground-based measurements were carried out in Paphos, Cyprus, to characterize the abundance, properties, and sources of aerosol particles in general and cloud condensation nuclei (CCN) and ice-nucleating particles (INP) in particular. New particle formation (NPF) events with subsequent growth of the particles into the CCN size range were observed. Aitken mode particles featured κ values of 0.21 to 0.29, indicating the presence of organic materials. Accumulation mode particles featured a higher hygroscopicity parameter, with a median κ value of 0.57, suggesting the presence of sulfate and maybe sea salt particles mixed with organic carbon. A clear downward trend of κ with increasing supersaturation and decreasing dcrit was found. Super-micron particles originated mainly from sea-spray aerosol (SSA) and partly from mineral dust. INP concentrations (NINP) were measured in the temperature range from -6.5 to -26.5 ∘C , using two freezing array-type instruments. NINP at a particular temperature span around 1 order of magnitude below -20 ∘C and about 2 orders of magnitude at warmer temperatures (T>-18 ∘C). Few samples showed elevated concentrations at temperatures >-15 ∘C , which suggests a significant contribution of biological particles to the INP population, which possibly could originate from Cyprus. Both measured temperature spectra and NINP probability density functions (PDFs) indicate that the observed INP (ice active in the temperature range between -15 and -20 ∘C) mainly originate from long-range transport. There was no correlation between NINP and particle number concentration in the size range >500 nm (N>500nm). Parameterizations based on N>500nm were found to overestimate NINP by about 1 to 2 orders of magnitude. There was also no correlation between NINP and particle surface area concentration. The ice active surface site density (ns) for the polluted aerosol encountered in the eastern Mediterranean in this study is about 1 to 3 orders of magnitude lower than the ns found for dust aerosol particles in previous studies. This suggests that observed NINP PDFs such as those derived here could be a better choice for modeling NINP if the aerosol particle composition is unknown or uncertain. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

In the framework of the MarParCloud (Marine biological production, organic aerosol particles and marine clouds: a Process Chain) project, measurements were carried out on the islands of Cape Verde, to investigate the abundance, properties, and sources of aerosol particles in general and cloud condensation nuclei (CCN) in particular, both close to sea and cloud level heights. A thorough comparison of particle number concentration (PNC), particle number size distribution (PNSD) and CCN number concentration (NCCN) at the Cape Verde Atmospheric Observatory (CVAO, sea level station) and Monte Verde (MV, cloud level station) reveals that during times without clouds the aerosol at CVAO and MV are similar and the boundary layer is generally well mixed. Therefore, data obtained at CVAO can be used to describe the aerosol particles at cloud level. Cloud events were observed at MV during roughly 58 % of the time and during these, a large fraction of particles were activated to cloud droplets. A trimodal parameterization method was deployed to characterize PNC at CVAO. Based on number concentrations in different aerosol modes, four well separable types of PNSDs were found, which were named the marine type, mixture type, dust type1 and dust type2. Aerosol particles differ depending on their origins. When the air masses came from the Atlantic Ocean, sea spray can be assumed to be one source for particles, besides for new particle formation. For these air masses, PNSDs featured the lowest number concentration in Aitken, accumulation and coarse mode. Particle number concentrations for the sea spray aerosol (SSA, i.e., the coarse mode for these air masses) accounted for about 3.7 % of NCCN,0.30 % (CCN number concentration at 0.30 % supersaturation) and about 1.1 % to 4.4 % of Ntotal (total particle number concentration). When the air masses came from the Saharan desert, we observed enhanced Aitken, accumulation and coarse mode particle number concentrations and overall increased NCCN. NCCN,0.30 % during the strongest observed dust periods is about 2.5 times higher than that during marine periods. However, the particle hygroscopicity parameter κ for these two most different periods shows no significant difference and is generally similar, independent of air mass. Overall, κ averaged 0.28, suggesting the presence of organic material in particles. This is consistent with previous model work and field measurement. There is a slight increase of κ with increasing particle size, indicating the addition of soluble, likely inorganic material during cloud processing. [ABSTRACT FROM AUTHOR]

Number concentrations of ice-nucleating particles (NINP) in the Arctic were derived from ground-based filter samples. Examined samples had been collected in Alert (Nunavut, northern Canadian archipelago on Ellesmere Island), Utqiaġvik, formerly known as Barrow (Alaska), Ny-Ålesund (Svalbard), and at the Villum Research Station (VRS; northern Greenland). For the former two stations, examined filters span a full yearly cycle. For VRS, 10 weekly samples, mostly from different months of one year, were included. Samples from Ny-Ålesund were collected during the months from March until September of one year. At all four stations, highest concentrations were found in the summer months from roughly June to September. For those stations with sufficient data coverage, an annual cycle can be seen. The spectra of NINP observed at the highest temperatures, i.e., those obtained for summer months, showed the presence of INPs that nucleate ice up to -5 ∘ C. Although the nature of these highly ice-active INPs could not be determined in this study, it often has been described in the literature that ice activity observed at such high temperatures originates from the presence of ice-active material of biogenic origin. Spectra observed at the lowest temperatures, i.e., those derived for winter months, were on the lower end of the respective values from the literature on Arctic INPs or INPs from midlatitude continental sites, to which a comparison is presented herein. An analysis concerning the origin of INPs that were ice active at high temperatures was carried out using back trajectories and satellite information. Both terrestrial locations in the Arctic and the adjacent sea were found to be possible source areas for highly active INPs. [ABSTRACT FROM AUTHOR]

As part of the A-LIFE (Absorbing aerosol layers in a changing climate: aging, lifetime and dynamics) campaign, ground-based measurements were carried out in Paphos, Cyprus, for characterizing the abundance, properties and sources of aerosol particles in general, and cloud condensation nuclei (CCN) and ice nucleating particles (INP), in particular. New particle formation (NPF) events with subsequent growth of the particles into the CCN size range were observed. Aitken mode particles featured κ values of 0.21 to 0.29, indicating the presence of organic materials. Accumulation mode particles featured a higher hygroscopicity parameter, with a median κ value of 0.57, suggesting the presence of sulfate. A clear downward trend of κ with increasing supersaturation and decreasing dcrit was found. Super-micron particles originated mainly from sea spray aerosol (SSA) and partly from mineral dust. INP concentrations (NINP) were measured in the temperature range from −6.5 to −26.5 ℃, using two freezing array type instruments. NINP at a particular temperature span around 1 order of magnitude below −20 ℃, and about 2 orders of magnitude at warmer temperatures (T > −18 ℃). Few samples showed elevated concentrations at temperatures > −15 ℃, which suggests a significant contribution of biological particles to the INP population, which possibly could originate from Cyprus. Both measured temperature spectra and NINP probability density functions (PDFs) indicate that the observed INP (ice active in the temperature range between −15 and −20 ℃) mainly originate from long-range transport. There was no correlation between NINP and particle number concentration in the size range > 500 nm (N> 500 nm). Parameterizations based on N> 500 nm were found to overestimate NINP by about 1 to 2 orders of magnitude. There was also no correlation between NINP and particle surface area concentration. The ice active surface site density (ns) for the anthropogenically polluted aerosol encountered in this study is about 1 to 3 orders of magnitude lower than the ns found for dust aerosol particles in previous studies. This suggests that observed NINP-PDFs as those derived here could be a better choice for modelling NINP if the aerosol particle composition is unknown or uncertain. [ABSTRACT FROM AUTHOR]

For three austral summer seasons (2013–2016, each from December to February) aerosol particles arriving at the Belgian Antarctic research station Princess Elisabeth (PE) in Dronning Maud Land in East Antarctica were characterized. This included number concentrations of total aerosol particles (NCN) and cloud condensation nuclei (NCCN), the particle number size distribution (PNSD), the aerosol particle hygroscopicity, and the influence of the air mass origin on NCN and NCCN. In general NCN was found to range from 40 to 6700 cm -3 , with a median of 333 cm -3 , while NCCN was found to cover a range between less than 10 and 1300 cm -3 for supersaturations (SSs) between 0.1 % and 0.7 %. It is shown that the aerosol is dominated by the Aitken mode, being characterized by a significant amount of small, and therefore likely secondarily formed, aerosol particles, with 94 % and 36 % of the aerosol particles smaller than 90 and ≈35 nm, respectively. Measurements of the basic meteorological parameters as well as the history of the air masses arriving at the measurement station indicate that the station is influenced by both marine air masses originating from the Southern Ocean and coastal areas around Antarctica (marine events – MEs) and continental air masses (continental events – CEs). CEs, which were defined as instances when the air masses spent at least 90 % of the time over the Antarctic continent during the last 10 days prior to arrival at the measurements station, occurred during 61 % of the time during which measurements were done. CEs came along with rather constant NCN and NCCN values, which we denote as Antarctic continental background concentrations. MEs, however, cause large fluctuations in NCN and NCCN , with low concentrations likely caused by scavenging due to precipitation and high concentrations likely originating from new particle formation (NPF) based on marine precursors. The application of HYSPLIT back trajectories in form of the potential source contribution function (PSCF) analysis indicate that the region of the Southern Ocean is a potential source of Aitken mode particles. On the basis of PNSDs, together with NCCN measured at an SS of 0.1 %, median values for the critical diameter for cloud droplet activation and the aerosol particle hygroscopicity parameter κ were determined to be 110 nm and 1, respectively. For particles larger than ≈110 nm the Southern Ocean together with parts of the Antarctic ice shelf regions were found to be potential source regions. While the former may contribute sea spray particles directly, the contribution of the latter may be due to the emission of sea salt aerosol particles, released from snow particles from surface snow layers, e.g., during periods of high wind speed, leading to drifting or blowing snow. The region of the Antarctic inland plateau, however, was not found to feature a significant source region for aerosol particles in general or for cloud condensation nuclei measured at the PE station in the austral summer. [ABSTRACT FROM AUTHOR]

To date, only a few studies have investigated the potential of coal fly ash particles to trigger heterogeneous ice nucleation in cloud droplets. The presented measurements aim at expanding the sparse dataset and improving process understanding of how physicochemical particle properties can influence the freezing behavior of coal fly ash particles immersed in water. Firstly, immersion freezing measurements were performed with two single particle techniques, i.e., the Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the SPectrometer for Ice Nuclei (SPIN). The effect of suspension time on the efficiency of the coal fly ash particles when immersed in a cloud droplet is analyzed based on the different residence times of the two instruments and employing both dry and wet particle generation. Secondly, two cold-stage setups, one using microliter sized droplets (Leipzig Ice Nucleation Array) and one using nanoliter sized droplets (WeIzmann Supercooled Droplets Observation on Microarray setup) were applied. We found that coal fly ash particles are comparable to mineral dust in their immersion freezing behavior when being dry generated. However, a significant decrease in immersion freezing efficiency was observed during experiments with wet-generated particles in LACIS and SPIN. The efficiency of wet-generated particles is in agreement with the cold-stage measurements. In order to understand the reason behind the deactivation, a series of chemical composition, morphology, and crystallography analyses (single particle mass spectrometry, scanning electron microscopy coupled with energy dispersive X-ray microanalysis, X-ray diffraction analysis) were performed with dry- and wet-generated particles. From these investigations, we conclude that anhydrous CaSO4 and CaO -- which, if investigated in pure form, show the same qualitative immersion freezing behavior as observed for dry-generated coal fly ash particles -- contribute to triggering heterogeneous ice nucleation at the particle--water interface. The observed deactivation in contact with water is related to changes in the particle surface properties which are potentially caused by hydration of CaSO4 and CaO. The contribution of coal fly ash to the ambient population of ice-nucleating particles therefore depends on whether and for how long particles are immersed in cloud droplets. [ABSTRACT FROM AUTHOR]

To date, only a few studies have investigated the potential of coal fly ash particles to trigger heterogeneous ice nucleation in cloud droplets. The presented measurements aim at expanding the sparse dataset and improving process understanding of how physico-chemical particle properties influence the freezing behavior of coal fly ash particles immersed in water. Firstly, immersion freezing measurements were performed with two single particle techniques, i.e., the Leipzig Aerosol Cloud Interaction Simulator and the Spectrometer for Ice Nuclei. The effect of suspension time on the efficiency of the coal fly ash particles when immersed in a cloud droplet is analyzed based on the different residence times of the two instruments and employing both dry and wet particle generation. Secondly, two cold stage setups, one using microliter sized droplets (Leipzig Ice Nucleation Array) and one using nanoliter sized droplets (Weizman Supercooled Droplets Observation on Microarray setup) were applied. We found that coal fly ash particles are comparable to mineral dust in their immersion freezing behavior when being dry-generated. However, a significant decrease in immersion freezing efficiency was observed during experiments with wet-generated particles in LACIS and SPIN. The efficiency of wet-generated particles is in agreement with the cold stage measurements. In order to understand the reason behind the deactivation, a series of chemical composition, morphology, and crystallography analyses (single particle mass spectrometry, scanning electron microscopy coupled with energy dispersive X-ray microanalysis, X-ray diffraction analysis) was performed with dry- and wet-generated particles. From these investigations, we conclude that anhydrous CaSO4 and CaO, which, if investigated in pure form, show the same qualitative immersion freezing behavior as observed for dry-generated coal fly ash particles, contribute to triggering heterogeneous ice nucleation at the particle-water interface. The observed deactivation in contact with water is related to changes of the particle surface propertieswhich are potentially caused by hydration of CaSO4 and CaO. The contribution of coal fly ash to the ambient population of ice nucleating particles therefore depends on whether and for how long particles are immersed in cloud droplets. [ABSTRACT FROM AUTHOR]

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 90nm 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 3000m were found to be up to 20 times higher than those measured below 2000 m; for one of these two flights, PNSDs measured above 2000m 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. [ABSTRACT FROM AUTHOR]

For three austral summer seasons (2013–2016, each from December to February) aerosol particles arriving at the Belgian Antarctic research station Princess Elisabeth (PE), in Dronning Maud Land in East Antarctica were characterized in terms of number concentrations of total aerosol particles (NCN) and cloud condensation nuclei (NCCN), the particle number size distribution (PNSD), the aerosol particle hygroscopicity and the influence of the air mass origin on NCN and NCCN. In general NCN was found to range from 40 to 6700 cm−3 with a median of 333 cm−3, while NCCN was found to cover a range between less than 10 and 1300 cm−3 for supersaturations (SS) between 0.1 and 0.7 %. It is shown that the aerosol is Aitken mode dominated and is characterized by a significant amount of freshly, secondarily formed aerosol particles, with 94 % and 36 % of the aerosol particles are smaller than 90 nm and ≈ 35 nm, respectively. Measurements of the basic meteorological parameters as well as the history of the air masses arriving at the measurement station indicate that the station is influenced by both, continental air masses originating from the Antarctic inland ice sheet (continental events – CE) and marine air masses originating from the Southern Ocean (marine events – ME). CEs came along with rather constant NCN and NCCN values, which we denote to be Antarctic continental background concentrations. MEs however cause large fluctuations in NCN and NCCN caused by scavenging due to precipitation or new particle formation based on marine precursors. The application of Hysplit back trajectories in form of the potential source contribution function (PSCF) analysis indicate, that the region of the Southern Ocean is a potential source of Aitken mode particles. For particles larger than ≈ 110 nm (CCN measured at SS of 0.1 %) the Antarctic ice shelf regions were found to be a potential source region, most likely due to the emission of sea salt aerosol particles, released from snow particles from surface snow layers by sublimation, e.g., during periods of high wind speed, leading to drifting or blowing snow. On the basis of the PNSDs and NCCN, the critical diameter for cloud droplet activation and the aerosol particle hygroscopicity parameter κ were determined to be 110 nm and 1, respectively, for a SS of 0.1 %. The region of the Antarctic inland plateau however was not found to feature a significant source region for CN and CCN measured at the PE station in austral summer. [ABSTRACT FROM AUTHOR]

Exceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated whether anthropogenic PM2.5 may significantly contribute to ice-nucleating particles (INP). However, few studies have focused on the ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the atmospheric number concentration of INP (NINP) in the range from -6 to -25° in Beijing. No correlations between NINP and either PM2.5 or black carbon mass concentrations were found, although both varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between NINP and either total particle number concentration or number concentrations for particles with diameters > 500 nm. Furthermore, there was no clear difference between day and night samples. All these results indicate that Beijing air pollution did not increase or decrease INP concentrations in the examined temperature range above values observed in nonurban areas; hence, the background INP concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined temperature range. [ABSTRACT FROM AUTHOR]

The degree of glaciation of mixed-phase clouds constitutes one of the largest uncertainties in climate prediction. In order to better understand cloud glaciation, cloud spectrometer observations are presented in this paper, which were made in the mixed-phase temperature regime between 0 and -38 °C (273 to 235 K), where cloud particles can either be frozen or liquid. The extensive data set covers four airborne field campaigns providing a total of 139 000 1 Hz data points (38.6 h within clouds) over Arctic, midlatitude and tropical regions. We develop algorithms, combining the information on number concentration, size and asphericity of the observed cloud particles to classify four cloud types: liquid clouds, clouds in which liquid droplets and ice crystals coexist, fully glaciated clouds after the Wegener–Bergeron–Findeisen process and clouds where secondary ice formation occurred. We quantify the occurrence of these cloud groups depending on the geographical region and temperature and find that liquid clouds dominate our measurements during the Arctic spring, while clouds dominated by the Wegener–Bergeron–Findeisen process are most common in midlatitude spring. The coexistence of liquid water and ice crystals is found over the whole mixed-phase temperature range in tropical convective towers in the dry season. Secondary ice is found at midlatitudes at -5 to -10 °C (268 to 263 K) and at higher altitudes, i.e. lower temperatures in the tropics. The distribution of the cloud types with decreasing temperature is shown to be consistent with the theory of evolution of mixed-phase clouds. With this study, we aim to contribute to a large statistical database on cloud types in the mixed-phase temperature regime. [ABSTRACT FROM AUTHOR]

Exceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated if anthropogenic PM2.5 may significantly contribute ice nucleating particles (INP). However, few studies have focused on the ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the atmospheric number concentration of INP (NINP) in the range from -6 ºC to -25 ºC in Beijing. No correlations between NINP and neither PM2.5 nor black carbon mass concentrations were found, although both varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between NINP and either total particle number concentration or number concentrations for particles with diameters > 500 nm. Furthermore, there was no clear difference between day and night samples. All these indicate that Beijing air pollution did not increase or decrease INP concentrations in the examined temperature range above values observed in non-urban areas, hence, the background INP concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined temperature range. [ABSTRACT FROM AUTHOR]

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. The observations of basic meteorological parameters and particle number size distributions (PNSDs) were indicative for the rapid transition from Arctic spring to summer that took place during the measurement period. Two distinct types of air masses were found. One type were typical Arctic haze air masses, termed as spring-type air masses, characterized by a mono-modal 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 bi-modal 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 as summer-type air masses, originated from the northern Pacific. Generally total particle number concentrations (NCN) ranged from 20 to 500 cm-3, while cloud condensation nuclei (CCN) number concentrations were found to cover a range between 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 kappa 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 twenty times higher than those measured below 2000 m, and for one of these two flights, PNSDs measured above 2000 m showed a different shape than those measured at lower altitudes. This is indicative for long range transport from lower latitudes into the Arctic that can advect aerosol from different regions in different heights. [ABSTRACT FROM AUTHOR]

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 inter-comparisons to ensure instrument differences are not interpreted as scientific findings. In this study, we inter-compare the results from parallel measurements using four online ice nucleation chambers. Seven different aerosol types are tested including untreated and acid treated mineral dust (microcline - 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 thermodynamic conditions that can be investigated with the inter-compared 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 ice crystal growth and different residence times in the chamber. To study the mechanisms responsible for ice nucleation in the four instruments, FF (from LACIS and PIMCA-PINC) and activated fraction, AF (from PINC and SPIN) are compared. Measured FFs are up to a factor of three higher than AFs, but not consistent for all aerosol types and temperatures investigated. It showed 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 on factors such as the importance of dispersion methods and the quality of particle size-selection for inter-comparing online INP counters. [ABSTRACT FROM AUTHOR]

The degree of glaciation of mixed-phase clouds constitutes one of the largest uncertainties in climate prediction. In order to better understand cloud glaciation, cloud spectrometer observations are presented in this paper that were made in the mixed-phase temperature regime between 0 #176;C and -38 #176;C, where cloud particles can either be frozen or liquid. The extensive dataset covers four airborne field campaigns providing a total of 139,000 1 Hz data points (38.6 hours within clouds) over Arctic, mid-latitude and tropical regions. We develop algorithms combining the information on number concentration, size and asphericity of the observed cloud particles to classify four cloud types associated with liquid clouds, clouds where liquid droplets and ice crystals coexist, fully glaciated clouds after the Wegener-Bergeron-Findeisen process, and clouds where secondary ice formation occurred. We quantify the occurrence of these cloud groups depending on the geographical region and temperature and find that liquid clouds dominate in our measurements during the Arctic spring, while clouds dominated by the Wegener-Bergeron-Findeisen process are most common in mid-latitude spring. Coexistence of liquid water and ice crystals is found over the whole mixed-phase temperature range in tropical convective towers in the dry season. Secondary ice is found at mid-latitudes at -5 #176;C to -10 #176;C and at higher altitudes, i.e. lower temperatures in the tropics. The distribution of the cloud types with decreasing temperatures is shown to be consistent with the theory of evolution of mixed-phase clouds. With this study, we aim to contribute to a large statistical database on cloud types in the mixed-phase temperature regime. [ABSTRACT FROM AUTHOR]

The marine aerosol arriving at Barbados (Ragged Point) was characterized during two 3-week long measurement periods in November 2010 and April 2011, in the context of the measurement campaign CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados). Through a comparison between groundbased and airborne measurements it was shown that the former are representative of the marine boundary layer at least up to cloud base. In general, total particle number concentrations (Ntotal) ranged from as low as 100 up to 800 cm-3, while number concentrations for cloud condensation nuclei (NCCN) at a supersaturation of 0.26% ranged from some 10 to 600 cm-3. Ntotal and NCCCN depended on the air mass origin. Three distinct types of air masses were found. One type showed elevated values for both Ntotal and NCCCN and could be attributed to long-range transport from Africa, by which biomass burning particles from the Sahel region and/or mineral dust particles from the Sahara were advected. The second and third type both had values for NCCCN below 200 cm-3 and a clear minimum in the particle number size distribution (NSD) around 70 to 80 nm (Hoppel minimum). While for one of these two types the accumulation mode was dominating (albeit less so than for air masses advected from Africa), the Aitken mode dominated the other and contributed more than 50% of all particles. These Aitken mode particles likely were formed by new particle formation no more than 3 days prior to the measurements. Hygroscopicity of particles in the CCN size range was determined from CCN measurements to be κ =0.66 on average, which suggests that these particles contain mainly sulfate and do not show a strong influence from organic material, which might generally be the case for the months during which measurements were made. The average κ could be used to derive NCCCN from measured number size distributions, showing that this is a valid approach to obtain NCCCN. Although the total particulate mass sampled on filters was found to be dominated by Na+ and Cl-, this was found to be contributed by a small number of large particles (>500 nm, mostly even in the super-micron size range). Based on a three-modal fit, a sea spray mode observed in the NSDs was found to contribute 90% to the total particulate mass but only 4 to 10% to Ntotal and up to 15% to NCCCN. This is in accordance with finding no correlation between Ntotal and wind speed. [ABSTRACT FROM AUTHOR]

The SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nucleating particle (INP) counter manufactured by Droplet Measurement Technologies in Boulder, CO. The SPIN is a continuous flow diffusion chamber with parallel plate geometry based on the Zurich Ice Nucleation Chamber and the Portable Ice Nucleation Chamber. This study presents a standard description for using the SPIN instrument and also highlights methods to analyze measurements in more advanced ways. It characterizes and describes the behavior of the SPIN chamber, reports data from laboratory measurements, and quantifies uncertainties associated with the measurements. Experiments with ammonium sulfate are used to investigate homogeneous freezing of deliquesced haze droplets and droplet breakthrough. Experiments with kaolinite, NX illite, and silver iodide are used to investigate heterogeneous ice nucleation. SPIN nucleation results are compared to those from the literature. A machine learning approach for analyzing depolarization data from the SPIN optical particle counter is also presented (as an advanceduse). Overall, we report that the SPIN is able to reproduce previous INP counter measurements. [ABSTRACT FROM AUTHOR]

Biological particles such as bacteria, fungal spores or pollen are known to be efficient ice nucleating particles. Their ability to nucleate ice is due to ice nucleation active macromolecules (INMs). It has been suggested that these INMs maintain their nucleating ability even when they are separated from their original carriers. This opens the possibility of an accumulation of such INMs in soils, resulting in an internal mixture of mineral dust and INMs. If particles from such soils which contain biological INMs are then dispersed into the atmosphere due to wind erosion or agricultural processes, they could induce ice nucleation at temperatures typical for biological substances, i.e., above -20 up to almost 0 °C, while they might be characterized as mineral dust particles due to a possibly low content of biological material. We conducted a study within the research unit INUIT (Ice Nucleation research UnIT), where we investigated the ice nucleation behavior of mineral dust particles internally mixed with INM. Specifically, we mixed a pure mineral dust sample (illite-NX) with ice active biological material (birch pollen washing water) and quantified the immersion freezing behavior of the resulting particles utilizing the Leipzig Aerosol Cloud Interaction Simulator (LACIS). A very important topic concerning the investigations presented here as well as for atmospheric application is the characterization of the mixing state of aerosol particles. In the present study we used different methods like single-particle aerosol mass spectrometry, Scanning Electron Microscopy (SEM), Energy Dispersive X-ray analysis (EDX), and a Volatility- Hygroscopicity Tandem Differential Mobility Analyser (VHTDMA) to investigate the mixing state of our generated aerosol. Not all applied methods performed similarly well in detecting small amounts of biological material on the mineral dust particles. Measuring the hygroscopicity/volatility of the mixed particles with the VH-TDMA was the most sensitive method. We found that internally mixed particles, containing ice active biological material, follow the ice nucleation behavior observed for the pure biological particles. We verified this by modeling the freezing behavior of the mixed particles with the Soccerball model (SBM). It can be concluded that a single INM located on a mineral dust particle determines the freezing behavior of that particle with the result that freezing occurs at temperatures at which pure mineral dust particles are not yet ice active. [ABSTRACT FROM AUTHOR]

It is generally known that ash particles from coal combustion can trigger ice nucleation. However, data on the ice nucleation of ash particles from different sources, including both anthropogenic and natural combustion processes, is still scarce. As coal combustion still fuels the biggest proportion of electric power production worldwide and biomass burning contributes significantly to the global aerosol loading, further data is needed to better assess the ice nucleating efficiency of ash particles. In the framework of this study, we found that ash particles from brown coal (i.e., lignite) burning are more ice active than those from wood burning, with fly ash from a coal-fired power-plant being the most efficient at nucleating ice. Furthermore the effect of particle generation on the freezing behavior was studied. For this, particles were generated either by dispersion of dry sample material, or by atomization of ash-water suspensions, and then led into the Leipzig Aerosol Cloud Interaction Simulator (LACIS) where the immersion freezing behavior was examined. Whereas the immersion freezing behavior of ashes from wood burning was not affected by the particle generation method, it depended on the type of particle generation for ash from brown coal. It was also found that the common practice of treating prepared suspensions in an ultrasonic bath to avoid aggregation of particles led to an enhanced ice nucleation activity. The findings of this study suggest a) that ash from brown coal burning may influence heterogeneous ice nucleation on at least a regional scale and b) that the freezing behavior of ash particles may be altered by a change in sample preparation and/or particle generation. [ABSTRACT FROM AUTHOR]

Ice nucleating particles (INP) in the troposphere can form ice in clouds via heterogeneous ice nucleation. Number concentrations of ice in clouds significantly affect cloud lifetime, the formation of precipitation and radiative properties. Still up to date, atmospheric number concentrations of INP are not well characterized and although there is some understanding of their sources, it is not known to which extend different sources contribute, nor if all sources are known. In this work, we are examining properties of INP that are known to occur in the oceanic sea surface microlayer (SML) and in bulk seawater, as well as the contribution of sea spray aerosol (SSA) to INP in clouds.The measurements to be presented here were carried out from 13 September to 12 October 2017 at Cape Verde. Besides for a thorough analysis of the atmospheric aerosol, samples collected for INP analysis include: bulk seawater and SML from the ocean upwind of the island; polycarbonate filter samples of atmospheric aerosol, collected on a tower installed at the island shore and on a 700 m high mountain top; cloud water collected during cloud events on the mountain top. INP concentrations were measured offline with two types of cold stages, based on well known techniques (see Chen et al., 2018), yielding results in the temperature range from roughly -5°C to -25°C.There were two main findings. Firstly, both enrichment and depletion of INP in the SML were observed compared to the bulk seawater, with an enrichment factor (EF) of INP number concentrations at -22 °C varying from 0.58 to 3.88. Secondly, the INP concentrations of the cloud water were around one order of magnitude higher than those of the SML and bulk seawater. When accounting for measured aerosol parameters (concentrations of total particles and cloud condensation nuclei) and assuming cloud droplet sizes in a range from 5 to 20 micrometer, it can be estimated that only a low fraction of all atmospheric INP were from the SSA.The authors acknowledge the Leibniz Association SAW funding for the MarParCloud project, SAW-2016-TROPOS-2.Literature: Chen, Jie, et al. "Ice-nucleating particle concentrations unaffected by urban air pollution in Beijing, China." Atmospheric Chemistry and Physics 18.5 (2018): 3523-3539. [ABSTRACT FROM AUTHOR]