Aerosol particles, including airborne microorganisms, are transported through the free troposphere from the Asian continental area to the downwind area in East Asia and can influence climate changes, ecosystem dynamics, and human health. However, the variations present in airborne bacterial communities in the free troposphere over downwind areas are poorly understood, and there are few studies that provide an in-depth examination of the effects of long-range transport of aerosols (natural and anthropogenic particles) on bacterial variations. In this study, the vertical distributions of airborne bacterial communities at high altitudes were investigated and the bacterial variations were compared between dust events and non-dust events. Aerosols were collected at three altitudes from ground level to the free troposphere (upper level: 3000 or 2500 m; middle level: 1200 or 500 m; and low level: 10 m) during Asian dust events and non-dust events over the Noto Peninsula, Japan, where westerly winds carry aerosols from the Asian continental areas. During Asian dust events, air masses at high altitudes were transported from the Asian continental area by westerly winds, and laser imaging detection and ranging (lidar) data indicated high concentrations of non-spherical particles, suggesting that dust-sand particles were transported from the central desert regions of Asia. The air samples collected during the dust events contained 10–100 times higher concentrations of microscopic fluorescent particles and optical particle counter (OPC) measured particles than in non-dust events. The air masses of non-dust events contained lower amounts of dust-sand particles. Additionally, some air samples showed relatively high levels of black carbon, which were likely transported from the Asian continental coasts. Moreover, during the dust events, microbial particles at altitudes of > 1200 m increased to the concentrations ranging from 1. 2 × 10⁶ to 6. 6 × 10⁶ particles m⁻³. In contrast, when dust events disappeared, the microbial particles at > 1200 m decreased slightly to microbial-particle concentrations ranging from 6. 4 × 10⁴ to 8. 9 × 10⁵ particles m⁻³. High-throughput sequencing technology targeting 16S rRNA genes (16S rDNA) revealed that the bacterial communities collected at high altitudes (from 500 to 3000 m) during dust events exhibited higher diversities and were predominantly composed of natural-sand/terrestrial bacteria, such as Bacillus members. During non-dust periods, airborne bacteria at high altitudes were mainly composed of anthropogenic/terrestrial bacteria (Actinobacteria), marine bacteria (Cyanobacteria and Alphaproteobacteria), and plant-associated bacteria (Gammaproteobacteria), which shifted in composition in correspondence with the origins of the air masses and the meteorological conditions. The airborne bacterial structures at high altitudes suggested remarkable changes in response to air mass sources, which contributed to the increases in community richness and to the domination of a few bacterial taxa.

In order to better characterize ice nucleating (IN) aerosol particles in the atmosphere, we investigated the chemical composition, mixing state, and morphology of atmospheric aerosols that nucleate ice under conditions relevant for mixed-phase clouds. Five standard mineral dust samples (quartz, K-feldspar, Na-feldspar, Arizona test dust, and Asian dust source particles) were compared with actual aerosol particles collected from the west coast of Japan (the city of Kanazawa) during Asian dust events in February and April 2016. Following droplet activation by particles deposited on a hydrophobic Si (silicon) wafer substrate under supersaturated air, individual IN particles were located using an optical microscope by gradually cooling the temperature to −30 °C. For the aerosol samples, both the IN active particles and non-active particles were analyzed individually by atomic force microscopy (AFM), micro-Raman spectroscopy, and scanning electron microscopy (SEM) coupled with energy dispersive X-ray spectroscopy (EDX). Heterogeneous ice nucleation in all standard mineral dust samples tested in this study was observed at consistently higher temperatures (e.g., −22.2 to −24.2 °C with K-feldspar) than the homogeneous freezing temperature (−36.5 °C). Meanwhile, most of the IN active atmospheric particles formed ice below −28 °C, i.e., at lower temperatures than the standard mineral dust samples of pure components. The most abundant IN active particles above −30 °C were predominantly irregular solid particles that showed clay mineral characteristics (or mixtures of several mineral components). Other than clay, Ca-rich particles internally mixed with other components, such as sulfate, were also regarded as IN active particle types. Moreover, sea salt particles were predominantly found in the non-active fraction, and internal mixing with sea salt clearly acted as a significant inhibiting agent for the ice nucleation activity of mineral dust particles. Also, relatively pure or fresh calcite, Ca(NO₃)₂, and (NH₄)₂SO₄ particles were more often found in the non-active fraction. In this study, we demonstrated the capability of the combined single droplet freezing method and thorough individual particle analysis to characterize the ice nucleation activity of atmospheric aerosols. We also found that dramatic changes in the particle mixing states during long-range transport had a complex effect on the ice nucleation activity of the host aerosol particles. A case study in the Asian dust outflow region highlighted the need to consider particle mixing states, which can dramatically influence ice nucleation activity.

Dithiothreitol-measured oxidative potential (OP^DTT) can chemically quantify the adverse health effects of atmospheric aerosols. Some chemical species are characterized with DTT activities, and the particle diameter and surface area control DTT oxidizability; however, the physical contribution to OP^DTT by atmospheric aerosols is controversial. Therefore, we performed field observations and aerosol sampling at urban and rural sites in Japan to investigate the effect of both physical and chemical properties on the variation in OP^DTT of atmospheric aerosols. The shifting degree of the representative diameter to the ultrafine range (i.e., the predominance degree of ultrafine particles) was retrieved from the ratio between the lung-deposited surface area and mass concentrations. The chemical components and OP^DTT were also elucidated. We discerned strong positive correlations of K, Mn, Pb, NH₄⁺, SO₄²⁻, and pyrolyzable organic carbon with OP^DTT. Hence, anthropogenic combustion, the iron–steel industry, and secondary organic aerosols were the major emission sources governing OP^DTT variations. The increased specific surface area did not lead to the increase in the OP^DTT of atmospheric aerosols, despite the existing relevance of the surface area of water-insoluble particles to DTT oxidizability. Overall, the OP^DTT of atmospheric aerosols can be estimated by the mass of chemical components related to OP^DTT variation, owing to numerous factors controlling DTT oxidizability (e.g., strong contribution of water-soluble particles). Our findings can be used to estimate OP^DTT via several physicochemical parameters without its direct measurement.

Iron (Fe), the main component of non-exhaust particulates, is known to have variable health effects that depend on the chemical species of iron. This study characterized the possible contribution of iron oxides and hydroxides to airborne brake wear particles under realistic vehicle driving and braking conditions with different brake pad friction materials. We found significant differences in wear factors and PM₁₀ and PM_2.5 emissions between non-asbestos organic (NAO) and European performance (ECE) brake pads. Iron was the dominant contributor to PM₁₀ and PM_2.5 brake wear particles for both NAO and ECE. The iron concentration ratio in the particle mass (PM) was comparable to the disc-to-pads ratio measured by wear mass. The fact that magnetite, which is of interest with respect to health effects, was less abundant in NAO than in ECE suggested that tribo-oxidations occurred in NAO. Metallic iron is generated not only from abrasive wear but also from tribo-chemical reduction with magnetite as the starting material. We found that there were differences in PM emissions between brake friction materials, and that the phase transformations of iron differed between friction materials. These differences were apparent in the distribution of iron oxides and hydroxides. Heat, tribo-oxidation, and tribo-reduction are intricately involved in these reactions.

Biological particles may play an important role in the climate system by efficiently acting as ice nucleating particles (INPs) at a higher temperature range (e.g., above −20 °C where representative INPs such as mineral dust remain inactive), but there is an obvious lack of direct evidence that these particles serve in this manner. Here, we collected ambient particles under different weather conditions for identifying INPs that are active above −22 °C. The abundance of such efficient INPs increased during or following rainfall events. The extensive characterization of individual particles by three different analyses (particle morphology and composition, heat sensitivity of ice nucleation activities, and biological fingerprinting by DNA staining) revealed that efficient INPs have distinctly biological characteristics, which differ significantly from more abundant, representative, and relatively less active INPs, such as mineral dust. Additionally, by combining the heat-sensitivity experiments and DNA staining techniques, efficient INPs were found to contain heat-sensitive biomaterials and biological cells. Our findings provide direct evidence that biological particles are preferentially released into the atmosphere during rainfall events and act as important atmospheric INPs at higher temperature ranges (warmer than −22 °C), where typical INPs remain inactive.

A new method, namely, force–distance curve mapping, was developed to directly measure the adhesion force of individual aerosol particles by atomic force microscopy. The proposed method collects adhesion force from multiple points on a single particle. It also takes into account the spatial distribution of the adhesion force affected by topography (e.g., the variation in the tip angle relative to the surface, as well as the force imposed upon contact), thereby enabling the direct and quantitative measurement of the adhesion force representing each particle. The topographic effect was first evaluated by measuring Polystyrene latex (PSL) standard particles, and the optimized method was then applied on atmospherically relevant model dust particles (quartz, ATD, and CJ-1) and inorganic particles (ammonium sulfate and artificial sea salt) to inter-compare the adhesion forces among different aerosol types. The method was further applied on the actual ambient aerosol particles collected on the western coast of Japan, when the region was under the influence of Asian dust plume. The ambient particles were classified into sea salt (SS), silicate dust, and Ca-rich dust particles based on individual particle analysis (micro-Raman or Scanning Electron Microscope/Energy Dispersive X-ray Spectroscopy (SEM-EDX)). Comparable adhesion forces were obtained from the model and ambient particles for both SS and silicate dust. Although dust particles tended to show smaller adhesion forces, the adhesion force of Ca-rich dust particles was larger than the majority of silicate dust particles and was comparable with the inorganic salt particles. These results highlight that the original chemical composition, as well as the aging process in the atmosphere, can create significant variation in the adhesion force among individual particles. This study demonstrates that force–distance curve mapping can be used as a new tool to quantitatively characterize the physical properties of aerosol particles on an individual basis.