Regionally sourced bioaerosols drive high-temperature ice nucleating particles in the Arctic.

Primary biological aerosol particles (PBAP) play an important role in the climate system, facilitating the formation of ice within clouds, consequently PBAP may be important in understanding the rapidly changing Arctic. Within this work, we use single-particle fluorescence spectroscopy to identify and quantify PBAP at an Arctic mountain site, with transmission electronic microscopy analysis supporting the presence of PBAP. We find that PBAP concentrations range between 10-3-10-1 L-1 and peak in summer. Evidences suggest that the terrestrial Arctic biosphere is an important regional source of PBAP, given the high correlation to air temperature, surface albedo, surface vegetation and PBAP tracers. PBAP clearly correlate with high-temperature ice nucleating particles (INP) (>-15 °C), of which a high a fraction (>90%) are proteinaceous in summer, implying biological origin. These findings will contribute to an improved understanding of sources and characteristics of Arctic PBAP and their links to INP.

Visualization of the seasonal shift of a variety of airborne pollens in western Tokyo.

Airborne pollens cause pollinosis and have the potential to affect microphysics in clouds; however, the number of monitored species has been very limited due to technical difficulties for the morphotype identification. In this study, we applied an eDNA approach to the airborne pollen communities in the suburbs of the Tokyo metropolitan area in Japan, within a mixed urban, rural, and mountain landscape, revealing pollen seasonality of various taxa (a total of 78 families across the period) in the spring season (February to May). Those taxa distinctly shifted in the season, especially in the beginning of February and the middle of April. Air temperature shift was an obvious key factor to affect the airborne pollen community, while the influence of other meteorological factors, such as wind speed, humidity, and precipitation, was not clear. Taxonomic classification of major Amplicon Sequence Variants (ASVs) indicates multiple pollen sources, including natural forest, planted forest, roadside, park lands, and horticultural activities. Most major ASV belongs to Japanese cedar (Cryptomeria japonica), which is the most notable allergen that causes pollinosis in Japan, peaking in mid-February to March. Backward trajectory analysis of air masses suggests that the Japanese cedar and other Cupressaceae plantation forests in the western mountains were a significant source of airborne pollen communities detected at our sampling site. Other major plant pollen sources, including Japanese zelkova (Zelkova serrata) and ginkgo (Ginkgo biloba), emanated from the nearby parks or roadside regions. This study's approach enables us to visualize the phenology of multiple pollen, including timing and duration. Long-term monitoring of this type would provide additional insight into understanding the role of climate change on pollen transmission and links to flowering events.

Seasonal Changes of Airborne Bacterial Communities Over Tokyo and Influence of Local Meteorology.

In order to study airborne bacterial community dynamics over Tokyo, including fine-scale correlations between airborne microorganisms and meteorological conditions, and the influence of local versus long-range transport of microbes, air samples were collected on filters for periods ranging from 48 to 72 h. The diversity of the microbial community was assessed by next generation sequencing. Predicted source regions of airborne particles, from back trajectory analyses, changed abruptly from the Pacific Ocean to the Eurasian Continent in the beginning of October. However, the microbial community composition and the alpha and beta diversities were not affected by this shift in meteorological regime, suggesting that long-range transport from oceanic or continental sources was not the principal determinant controlling the local airborne microbiome. By contrast, we found a significant correlation between the local meteorology, especially relative humidity and wind speed, and both alpha diversity and beta diversity. Among four potential local source categories (soil, bay seawater, river, and pond), bay seawater and soil were identified as constant and predominant sources. Statistical analyses point toward humidity as the most influential meteorological factor, most likely because it is correlated with soil moisture and hence negatively correlated with the dispersal of particles from the land surface. In this study, we have demonstrated the benefits of fine-scale temporal analyses for understanding the sources and relationships with the meteorology of Tokyo's "aerobiome."

Ice nucleation by particles containing long-chain fatty acids of relevance to freezing by sea spray aerosols.

Heterogeneous ice nucleation in the atmosphere regulates cloud properties, such as phase (ice versus liquid) and lifetime. Aerosol particles of marine origin are relevant ice nucleating particle sources when marine aerosol layers are lifted over mountainous terrain and in higher latitude ocean boundary layers, distant from terrestrial aerosol sources. Among many particle compositions associated with ice nucleation by sea spray aerosols are highly saturated fatty acids. Previous studies have not demonstrated their ability to freeze dilute water droplets. This study investigates ice nucleation by monolayers at the surface of supercooled droplets and as crystalline particles at temperatures exceeding the threshold for homogeneous freezing. Results show the poor efficiency of long chain fatty acid (C16, C18) monolayers in templating freezing of pure water droplets and seawater subphase to temperatures of at least -30 °C, consistent with theory. This contrasts with freezing of fatty alcohols (C22 used here) at nearly 20 °C warmer. Evaporation of µL-sized droplets to promote structural compression of a C19 acid monolayer did not favor warmer ice formation of drops. Heterogeneous ice nucleation occurred for nL-sized droplets condensed on 5 to 100 µm crystalline particles of fatty acid (C12 to C20) at a range of temperatures below -28 °C. These experiments suggest that fatty acids nucleate ice at warmer than -36 °C only when the crystalline phase is present. Rough estimates of ice active site densities are consistent with those of marine aerosols, but require knowledge of the proportion of surface area comprised of fatty acids for application.

An improved approach for measuring immersion freezing in large droplets over a wide temperature range.

Immersion freezing (ice nucleation by particles immersed in supercooled water) is a key process for forming ice in mixed-phase clouds. Immersion freezing experiments with particles in microliter-sized (millimeter-sized) water droplets are often applied to detecting very small numbers of ice nucleating particles (INPs). However, the application of such large droplets remains confined to the detection of INPs active at temperatures much higher than the homogeneous freezing limit, because of artifacts related to freezing of water droplets without added INPs at temperatures of -25 °C or higher on a supporting substrate. Here I report a method for measuring immersion freezing in super-microliter-sized droplets over a wide temperature range. To reduce possible artifacts, droplets are pipetted onto a thin layer of Vaseline and cooled in a clean booth. In the Cryogenic Refrigerator Applied to Freezing Test (CRAFT) system, freezing of pure (Milli-Q) water droplets are limited at temperatures above -30 °C. An intercomparison of various techniques for immersion freezing experiments with reference particles (Snomax and illite NX) demonstrates that despite the use of relatively large droplets, the CRAFT setup allows for evaluating the immersion freezing activity of the particles over almost the entire temperature range (about -30 °C to 0 °C) relevant for mixed-phase cloud formation.

Asian dust particles converted into aqueous droplets under remote marine atmospheric conditions.

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 HNO(3) to form Ca(NO(3))(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(NO(3))(2) and CaCl(2), which can deliquesce at low relative humidity. According to the results, the conversion of insoluble CaCO(3) to Ca(NO(3))(2) tends to be dominated over urban and industrialized areas of the Asian continent, where the concentrations of HNO(3) exceed those of HCl ([HNO(3)/HCl] >  âˆ¼ 1). In this regime, CaCl(2) is hardly detected from dust particles. However, the generation of CaCl(2) becomes detectable around the Japan Islands, where the concentrations of HCl are much higher than those of HNO(3) ([HNO(3)/HCl] <  âˆ¼ 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.

Phylogenetic analysis of atmospheric halotolerant bacterial communities at high altitude in an Asian dust (KOSA) arrival region, Suzu City.

The microbial communities transported by Asian desert dust (KOSA) events have attracted much attention as bioaerosols because the transported microorganisms are thought to influence the downwind ecosystems in Korea and Japan. However, the atmospheric microbial community has not been investigated at high altitude in the KOSA arrival area. In this study, to estimate the viability and diversity of atmospheric halotolerant bacteria, which are expected to resist to various environmental stresses as well as high salinities, bioaerosol samples were collected at 10 and 600 m above the ground within the KOSA arrival area, Suzu City, Japan, during KOSA events. During the sampling period, the particle numbers at 600 m were higher than those at 10 m, suggesting that large particles of aerosol fall from the high altitude of 600 m to the ground surface. The microorganisms in bioaerosol samples grew in media containing up to 15% NaCl concentrations demonstrating the viability of the halotolerant bacteria in bioaerosol samples. The PCR-DGGE analysis using 16S rDNA revealed that the bacterial species in NaCl-amended cultures were similar to the bacteria detected from the genomic DNA directly extracted from the bioaerosol samples. The 16S rDNA sequences of bacterial communities in bioaerosol samples were classified into 4 phylotypes belonging to the Bacilluscereus or Bacillussubtilis group. The bioaerosol samples collected at 600 m included 2 phylotypes belonging to B. subtilis, and one phylotype among all 4 phylotypes was identical between the samples at 10 and 600 m. In the atmosphere at 600 m, the halotolerant bacterial community was expected to remain viable, and the species composition was expected to include a few species of the genus Bacillus. During this investigation period, these atmospheric bacteria may have been vertically transported to the ground surface, where the long-range KOSA particle transport from China is frequently observed.