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Data from both laboratory studies and atmospheric measurements are used to develop an empirical parameterization for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RHw) are taken as a measure of the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. The parameterization developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A calibration factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RHw of 105% vs. maximum fractions active at higher RHw. Instrumental factors that affect activation behavior vs. RHw in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this calibration factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization, including calibration correction, to predictions of the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first-order approximation in numerical modeling investigations.

Bioaerosols are relevant for public health and may play an important role in the climate system, but their atmospheric abundance, properties, and sources are not well understood. Here we show that the concentration of airborne biological particles in a North American forest ecosystem increases significantly during rain and that bioparticles are closely correlated with atmospheric ice nuclei (IN). The greatest increase of bioparticles and IN occurred in the size range of 2–6 μm, which is characteristic for bacterial aggregates and fungal spores. By DNA analysis we found high diversities of airborne bacteria and fungi, including groups containing human and plant pathogens (mildew, smut and rust fungi, molds, Enterobacteriaceae, Pseudomonadaceae). In addition to detecting known bacterial and fungal IN (Pseudomonas sp., Fusarium sporotrichioides), we discovered two species of IN-active fungi that were not previously known as biological ice nucleators (Isaria farinosa and Acremonium implicatum). Our findings suggest that atmospheric bioaerosols, IN, and rainfall are more tightly coupled than previously assumed.

The Arctic is warming at more than twice the rate of the global average. This warming is influenced by clouds, which modulate the solar and terrestrial radiative fluxes and, thus, determine the surface energy budget. However, the interactions among clouds, aerosols, and radiative fluxes in the Arctic are still poorly understood. To address these uncertainties, the Ny-Ålesund Aerosol Cloud Experiment (NASCENT) study was conducted from September 2019 to August 2020 in Ny-Ålesund, Svalbard. The campaign’s primary goal was to elucidate the life cycle of aerosols in the Arctic and to determine how they modulate cloud properties throughout the year. In situ and remote sensing observations were taken on the ground at sea level, at a mountaintop station, and with a tethered balloon system. An overview of the meteorological and the main aerosol seasonality encountered during the NASCENT year is introduced, followed by a presentation of first scientific highlights. In particular, we present new findings on aerosol physicochemical and molecular properties. Further, the role of cloud droplet activation and ice crystal nucleation in the formation and persistence of mixed-phase clouds, and the occurrence of secondary ice processes, are discussed and compared to the representation of cloud processes within the regional Weather Research and Forecasting Model. The paper concludes with research questions that are to be addressed in upcoming NASCENT publications.

Kaolinite particles from two different sources (Fluka and Clay Minerals Society (CMS)) were examined with respect to their ability to act as ice nuclei (IN). This was done in the water-subsaturated regime where often deposition ice nucleation is assumed to occur, and for water-supersaturated conditions, i.e., in the immersion freezing mode. Measurements were done using a flow tube (the Leipzig Aerosol Cloud Interaction Simulator, LACIS) and a continuous-flow diffusion chamber (CFDC). Pure and coated particles were used, with coating thicknesses of a few nanometers or less, where the coating consisted of levoglucosan, succinic acid or sulfuric acid. In general, it was found that the coatings strongly reduced deposition ice nucleation. Remaining ice formation in the water-subsaturated regime could be attributed to immersion freezing, with particles immersed in concentrated solutions formed by the coatings. In the immersion freezing mode, ice nucleation rate coefficients jhet from both instruments agreed well with each other, particularly when the residence times in the instruments were accounted for. Fluka kaolinite particles coated with either levoglucosan or succinic acid showed the same IN activity as pure Fluka kaolinite particles; i.e., it can be assumed that these two types of coating did not alter the ice-active surface chemically, and that the coatings were diluted enough in the droplets that were formed prior to the ice nucleation, so that freezing point depression was negligible. However, Fluka kaolinite particles, which were either coated with pure sulfuric acid or were first coated with the acid and then exposed to additional water vapor, both showed a reduced ability to nucleate ice compared to the pure particles. For the CMS kaolinite particles, the ability to nucleate ice in the immersion freezing mode was similar for all examined particles, i.e., for the pure ones and the ones with the different types of coating. Moreover, jhet derived for the CMS kaolinite particles was comparable to jhet derived for Fluka kaolinite particles coated with sulfuric acid. This is suggestive for the Fluka kaolinite possessing a type of ice-nucleating surface feature which is not present on the CMS kaolinite, and which can be destroyed by reaction with sulfuric acid. This might be potassium feldspar.

Heterogeneous ice nucleation is a crucial process for forming ice-containing clouds and subsequent ice-induced precipitation. The importance for ice nucleation by airborne desert soil dusts composed predominantly of minerals is widely acknowledged. However, the potential influence of agricultural soil dusts on ice nucleation has been poorly recognized, despite recent estimates that they may account for up to 20–25% of the global atmospheric dust load. We have conducted freezing experiments with various dusts, including agricultural soil dusts derived from the largest dust-source region in North America. Here we show evidence for the significant role of soil organic matter (SOM) in particles acting as ice nuclei (IN) under mixed-phase cloud conditions. We find that the ice-nucleating ability of the agricultural soil dusts is similar to that of desert soil dusts, but is clearly reduced after either H2O2 digestion or dry heating to 300 °C. In addition, based on chemical composition analysis, we demonstrate that organic-rich particles are more important than mineral particles for the ice-nucleating ability of the agricultural soil dusts at temperatures warmer than about −36 °C. Finally, we suggest that such organic-rich particles of agricultural origin (namely, SOM particles) may contribute significantly to the ubiquity of organic-rich IN in the global atmosphere.

The Arctic region is sensitive to climate change and is warming faster than the global average. Aerosol particles change cloud properties by acting as cloud condensation nuclei and ice-nucleating particles, thus influencing the Arctic climate system. Therefore, understanding the aerosol particle properties in the Arctic is needed to interpret and simulate their influences on climate. In this study, we collected ambient aerosol particles using whole-air and PM10 inlets and residual particles of cloud droplets and ice crystals from Arctic low-level clouds (typically, all-liquid or mixed-phase clouds) using a counterflow virtual impactor inlet at the Zeppelin Observatory near Ny-Ålesund, Svalbard, within a time frame of 4 years. We measured the composition and mixing state of individual fine-mode particles in 239 samples using transmission electron microscopy. On the basis of their composition, the aerosol and cloud residual particles were classified as mineral dust, sea salt, K-bearing, sulfate, and carbonaceous particles. The number fraction of aerosol particles showed seasonal changes, with sulfate dominating in summer and sea salt increasing in winter. There was no measurable difference in the fractions between ambient aerosol and cloud residual particles collected at ambient temperatures above 0 ∘C. On the other hand, cloud residual samples collected at ambient temperatures below 0 ∘C had several times more sea salt and mineral dust particles and fewer sulfates than ambient aerosol samples, suggesting that sea spray and mineral dust particles may influence the formation of cloud particles in Arctic mixed-phase clouds. We also found that 43 % of mineral dust particles from cloud residual samples were mixed with sea salt, whereas only 18 % of mineral dust particles in ambient aerosol samples were mixed with sea salt. This study highlights the variety in aerosol compositions and mixing states that influence or are influenced by aerosol–cloud interactions in Arctic low-level clouds.

We investigated the association of marine biological indicators (polysaccharides, protein-like gel particles, and chl a) with the formation of fluorescent aerosol particles, cloud condensation nuclei (CCNs), and ice-nucleating particles (INPs) over the North Pacific Ocean, Bering Sea, and Arctic Ocean during September–November 2019. The abundance of bioindicators was high in the North Pacific Ocean and the Bering Sea (e.g., up to 1.3 mg m−3 of chl a), suggesting high biological activity due to a phytoplankton bloom. In the North Pacific Ocean, particles were characterized by high mass fractions of organics and sulfate with a predominance of terrestrial air masses. Conversely, in the Bering Sea and the Arctic Ocean, particles were characterized by high mass fractions of sea salt and sulfate with a predominance of maritime air masses. The averaged range/value of the CCN concentration at 0.4 % supersaturation were 99–151, 43–139, and 36 cm−3 over the North Pacific Ocean with terrestrial influences, over the Bering Sea with marine biogenic influences, and over the Arctic Ocean with marine influences, respectively, and the corresponding range/value of the hygroscopicity parameter κ were 0.17–0.59, 0.42–0.68, and 0.66, respectively. The averaged INP concentration (NINP) measured at temperatures of −18 and −24 ∘C with marine sources in the North Pacific and Bering Sea was 0.01–0.09 and 0.1–2.5 L−1, respectively, and that over the Arctic Ocean was 0.001–0.016 and 0.012–0.27 L−1, respectively. When marine sources were dominant, fluorescent bioaerosols in the fine mode were strongly correlated with all bioindicator types (R: 0.81–0.88) when the effect of wind-induced uplift from the sea surface to the atmosphere was considered. Correlations between NINP measured at −18 and −24 ∘C and all bioindicator types (R: 0.58–0.95 and 0.79–0.93, respectively) were positive, even when the extreme outlier point was omitted, as were those between NINP and fluorescent bioaerosols (R: 0.50 and 0.60, respectively), suggesting that marine bioindicators contributed substantially as sources of bioaerosols and to cloud formation.

Soil organic matter (SOM) may be a significant source of atmospheric ice nucleating particles (INPs), especially of those active  >  −15 °C. However, due to both a lack of investigations and the complexity of the SOM itself, the identities of these INPs remain unknown. To more comprehensively characterize organic INPs we tested locally representative soils in Wyoming and Colorado for total organic INPs, INPs in the heat-labile fraction, ice nucleating (IN) bacteria, IN fungi, IN fulvic and humic acids, IN plant tissue, and ice nucleation by monolayers of aliphatic alcohols. All soils contained  ≈  106 to  ≈  5 × 107 INPs g−1 dry soil active at −10 °C. Removal of SOM with H2O2 removed  ≥  99 % of INPs active  >  −18 °C (the limit of testing), while heating of soil suspensions to 105 °C showed that labile INPs increasingly predominated  >  −12 °C and comprised  ≥  90 % of INPs active  >  −9 °C. Papain protease, which inactivates IN proteins produced by the fungus Mortierella alpina, common in the region's soils, lowered INPs active at  ≥  −11 °C by  ≥  75 % in two arable soils and in sagebrush shrubland soil. By contrast, lysozyme, which digests bacterial cell walls, only reduced INPs active at  ≥  −7.5 or  ≥  −6 °C, depending on the soil. The known IN bacteria were not detected in any soil, using PCR for the ina gene that codes for the active protein. We directly isolated and photographed two INPs from soil, using repeated cycles of freeze testing and subdivision of droplets of dilute soil suspensions; they were complex and apparently organic entities. Ice nucleation activity was not affected by digestion of Proteinase K-susceptible proteins or the removal of entities composed of fulvic and humic acids, sterols, or aliphatic alcohol monolayers. Organic INPs active colder than −10 to −12 °C were resistant to all investigations other than heat, oxidation with H2O2, and, for some, digestion with papain. They may originate from decomposing plant material, microbial biomass, and/or the humin component of the SOM. In the case of the latter then they are most likely to be a carbohydrate. Reflecting the diversity of the SOM itself, soil INPs have a range of sources which occur with differing relative abundances.

Long-range transport of atmospheric microbiota with Asian dust (Kosa) particles is of great concern in Northeast Asia in view of the health effect of Kosa particles on human being, disturbance of ecosystems caused through invasion of new microbe, contribution of microorganisms to biogeochemical cycle on global/regional scales, and others. Information on atmospheric microbes over the desert areas has been desired for a long time. Detection of atmospheric microbiota on the desert regions, on the base of balloon-borne measurements, has been made at Dunhuang, China (40°00′ N, 94°30′ E; east end of Taklamakan desert) in the summer of 2007. The measurements showed that microbiota mixed internally with Kosa particles were frequently floating from the ground to about 2-km heights (above sea level), and possible long-range transport of atmospheric microbiota with dust particles taking local circulations is strongly suggested, causing active mixing of atmospheric dust over the Taklamakan desert from the ground to the free troposphere where westerly jet dominates (Iwasaka et al. in J Geophys Res 108:8652, 2003a , J Geophys Res 108:8644, b ). The concentration of the mixed particles of Kosa and microbiota having a size larger than about 1 μm in diameter is estimated to be about 1 particle/cm 3 at those heights on the basis of measurements of particle concentration with an optical particle counter and analysis of particles having fluorescence light due to dye of DAPI (4′6-diamidino-2 phenylindole) with an epifluorescence microscope. The mixing situation of microbiota and Kosa particles is the important factor controlling atmospheric lifetime of floating microbiota, since the mixing state certainly can protect microbiota from stressful environments [dryness, solar ultraviolet (UV) radiation, low temperature] in the atmosphere, and therefore, it is useful to discuss the data of the first description of microbiota in the atmosphere on the Taklamakan desert.

The chemical history of dust particles in the atmosphere is crucial for assessing their impact on both the Earth’s climate and ecosystem. So far, a number of studies have shown that, in the vicinity of strong anthropogenic emission sources, Ca-rich dust particles can be converted into aqueous droplets mainly by the reaction with gaseous HNO₃ to form Ca(NO₃)₂. Here we show that other similar processes have the potential to be activated under typical remote marine atmospheric conditions. Based on field measurements at several sites in East Asia and thermodynamic predictions, we examined the possibility for the formation of two highly soluble calcium salts, Ca(NO₃)₂ and CaCl₂, which can deliquesce at low relative humidity. According to the results, the conversion of insoluble CaCO₃ to Ca(NO₃)₂ tends to be dominated over urban and industrialized areas of the Asian continent, where the concentrations of HNO₃ exceed those of HCl ([HNO₃/HCl] > ∼1). In this regime, CaCl₂ is hardly detected from dust particles. However, the generation of CaCl₂ becomes detectable around the Japan Islands, where the concentrations of HCl are much higher than those of HNO₃ ([HNO₃/HCl] < ∼0.3). We suggest that elevated concentrations of HCl in the remote marine boundary layer are sufficient to modify Ca-rich particles in dust storms and can play a more important role in forming a deliquescent layer on the particle surfaces as they are transported toward remote ocean regions.