Assessment of the Sphericity of Submicrometer Particles Using a Single-particle Polar Nephelometer at an Urban Site in Japan

he sphericity of particles must be considered when evaluating their effects on the climate and human health. Thus, to examine this property and its controlling factors, this study measured the scattering angular distributions of both thermodenuded and non-thermodenuded individual particles with a diameter of 500 nm in real time using a home-made polar nephelometer in Nagoya, Japan. Estimating the sphericities based on the depths of the local minima in the scattering angular distributions, we found the ambient aerosols to be external mixtures of at least two types of particles, one with relatively high and the other with relatively low sphericity. Although most of the particles exhibiting high sphericity were removed as they passed through the thermodenuder, approximately one-third of the fraction exhibiting low sphericity remained. During the daytime, the proportion of the low-sphericity particles decreased, whereas the average sphericity of the high-sphericity particles increased, which can be attributed to photochemical formation and/or aging processes. On days with extremely high relative humidity, the diurnal variation in the average sphericity displayed another peak during the early morning, which may have been due to the secondary formation of nitrate

Offline analysis of the chemical composition and hygroscopicity of sub-micrometer aerosol at an Asian outflow receptor site and comparison with online measurements

Filter-based offline analysis of atmospheric aerosol hygroscopicity coupled to composition analysis provides information complementary to that obtained from online analysis. However, its application itself and comparison to online analysis have remained limited to date. In this study, daily submicrometer aerosol particles (PM0.95, 50 % cutoff diameter 0.95 µm) were collected onto quartz fiber filters on Okinawa Island, a receptor of East Asian outflow, in the autumn of 2015. The chemical composition of water-soluble matter (WSM) in PM0.95, PM0.95 itself, and their respective hygroscopicities were characterized through the offline use of an aerosol mass spectrometer and a hygroscopicity tandem differential mobility analyzer. Thereafter, results were compared with those obtained from online analyses. Sulfate dominated the WSM mass (59 %), followed by water-soluble organic matter (WSOM, 20 %) and ammonium (13 %). WSOM accounted for most (91 %) of the mass of extracted organic matter (EOM) and the atomic O-to-C ratios (O : C) of WSOM and EOM were high (mean ± standard deviation were 0.84 ± 0.08 and 0.78 ± 0.08, respectively), both of which indicate highly aged characteristics of the observed aerosol. The hygroscopic growth curves showed clear hysteresis for most samples. At 85 % relative humidity (RH), the calculated hygroscopicity parameter κ values of the WSM (κWSM), WSOM, EOM, andPM0.95 (κPM0.95 ) were 0.50 ± 0.03, 0.22 ± 0.12, 0.20 ± 0.11, and 0.47 ± 0.03, respectively. An analysis using the thermodynamic Extended Aerosol Inorganics Model (E-AIM) shows, on average, that inorganic salts and WSOM contributed 88 % and 12 %, respectively, of the κWSM (or κPM0.95 ). High similarities were found between offline and online analysis for chemical compositions that are related to particle hygroscopicity (the mass fractions and O : C of organics and the degree of neutralization) and also for aerosol hygroscopicity. As possible factors governing the variation in κWSM, the influences of WSOM abundance and the neutralization of inorganic salts were assessed. At high RH (70 %–90 %), the hygroscopicity of WSM and PM0.95 was affected considerably by the presence of organic components; at low RH (20 %–50 %), the degree of neutralization could be important.This study not only characterized aerosol hygroscopicity at the receptor site of East Asian outflow but also shows that offline hygroscopicity analysis is an appropriate method, at least for aerosols of the studied type. The results encourage further applications to other environments and to more in-depth hygroscopicity analysis, in particular for organic fractions