No abstract

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.

The chemical speciation of nanoparticles is technically challenging because of the minute mass of the particles. There is a constant need for more sensitive collection methods and chemical analyses. In this study, we demonstrated the applicability of a surface enhanced Raman scattering (SERS) technique on the rapid and sensitive chemical analysis of individual nanoparticles. SERS technique provides a significant enhancement of the scattering efficiency over traditional Raman spectroscopy. The novelty of the proposed technique is that the SERS substrate is used directly as the sampling substrate of a condensational growth tube (CGT) sampler, which can activate nanoparticles into water droplets and ensure simultaneous inertial sampling and SERS pretreatment. First, we investigated applicability of the method on mono-dispersed (20 nm, 50 nm, or 100 nm) ammonium sulfate (AS) and levoglucosan (LG) particles as model aerosols. The method was then applied to ambient nanoparticles. The successful detection of peaks corresponding to sulfate (SO 4 2-) and organics (C-H) indicates that our proposed method to combine a CGT sampler and SERS showed a sensitivity high enough to provide deep insights into the chemical speciation of atmospheric nanoparticles as small as 20 nm in diameter.