Chromophoric water-soluble organic matter in atmospheric aerosols potentially plays an important role in aqueous reactions and light absorption by organics. The fluorescence and chemical-structural characteristics of the chromophoric water-soluble organic matter in submicron aerosols collected in urban, forest, and marine environments (Nagoya, Kii Peninsula, and the tropical Eastern Pacific) were investigated using excitation-emission matrices (EEMs) and a high-resolution aerosol mass spectrometer. A total of three types of water-soluble chromophores, two with fluorescence characteristics similar to those of humiclike substances (HULIS-1 and HULIS-2) and one with fluorescence characteristics similar to those of protein compounds (PLOM), were identified in atmospheric aerosols by parallel factor analysis (PARAFAC) for EEMs. We found that the chromophore components of HULIS-1 and -2 were associated with highly and less-oxygenated structures, respectively, which may provide a clue to understanding the chemical formation or loss of organic chromophores in atmospheric aerosols. Whereas HULIS-1 was ubiquitous in water-soluble chromophores over different environments, HULIS-2 was abundant only in terrestrial aerosols, and PLOM was abundant in marine aerosols. These findings are useful for further studies regarding the classification and source identification of chromophores in atmospheric aerosols.

A suite of advanced instruments were employed to measure aerosol hygroscopicity, volatility and chemical composition at a suburban site in the Pearl River Delta (PRD) Region and at a marine site in Okinawa, respectively. The results showed that the particle number concentration in PRD is approximately ten times higher than that in Okinawa. Organics contributes about one half of the total NR-PM 1 concentration in PRD, while sulfate is the dominant component (about 60%) in Okinawa. Diurnal variation of the chemical species demonstrated that the site in PRD was affected by trafficrelated sources and industrial emissions, while the one in Okinawa is mainly affected by regional emissions. The V-TDMA measurements showed that a large fraction (20-45%) of particles in Okinawa volatilized at about 200°C and nearly all particles volatilized at about 300°C, indicating that the particles were almost volatile in Okinawa. In contrast, a fraction (15-21%) of particles in PRD did not evaporate even when heated to about 300°C, implying that these particles might contain black carbon or low-volatile organics. For 40-200 nm particles in Okinawa, the hygroscopicity parameter κ is around 0.5, significantly higher than that of PRD particles (κ ≈ 0.26). Particles tend to have bimodal distribution in PRD and unimodal in Okinawa, indicating that the former is externally mixed while the latter is internally mixed.

The formation of biogenic secondary organic aerosols (BSOAs) in forest environments is potentially important to cloud formation via changes of the cloud condensation nuclei (CCN) activity of aerosols. In this study, the CCN activation of submicrometer aerosols and their chemical compositions and size distributions were measured at a midlatitude forest site in Japan during the summer of 2014 to assess the hygroscopicity of the organic aerosols and their contributions to the local CCN concentrations. The mean number concentrations of the condensation nuclei and CCN at supersaturation (SS) conditions of 0.11–0.80% were 1,238 and 166–740 cm−3, respectively. Organic aerosols and sulfate dominated the submicrometer aerosol mass concentrations. The particle hygroscopicity increased with increases in particle diameters. The hygroscopicity parameter for the organics, κorg, was positively correlated with the atomic O to C ratio. The product of κorg and the volume fraction of OA was 0.12, accounting for 38% of the water uptake by aerosol particles. The hygroscopicity parameter of the locally formed fresh BSOA was estimated to be 0.09. The contribution of OA to the CCN number concentration, which was assessed by subtracting the CCN concentration of the hypothetical inorganic aerosols from that of the ambient aerosols, was 50–182 cm−3 for the SS range of 0.11–0.80%. The increase of the CCN number concentrations per 1‐μg/m3 increase of the BSOA was 23–299 cm−3 at 0.11–0.80% SS. The contribution of the BSOA to the CCN number concentration can be enhanced by new particle formation.

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