Abstract. A hygroscopic tandem differential mobility analyzer (HTDMA), a scanning mobility cloud condensation nuclei (CCN) analyzer (SMCA), and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) were used to, respectively, measure the hygroscopicity, condensation nuclei activation, and chemical composition of aerosol particles at the Panyu site in the Pearl River Delta region during wintertime 2014. The distribution of the size-resolved CCN at four supersaturations (SSs of 0.1 %, 0.2 %, 0.4 %, and 0.7 %) and the aerosol particle size distribution were obtained by the SMCA. The hygroscopicity parameter κ (κCCN, κHTDMA, and κAMS) was, respectively, calculated based upon the SMCA, HTDMA, and AMS measurements. The results showed that the κHTDMA value was slightly smaller than the κCCN one at all diameters and for particles larger than 100 nm, and the κAMS value was significantly smaller than the others (κCCN and κHTDMA), which could be attributed to the underestimated hygroscopicity of the organics (κorg). The activation ratio (AR) calculated from the growth factor – probability density function (Gf-PDF) without surface tension correction was found to be lower than that from the CCN measurements, due most likely to the uncorrected surface tension (σs∕a) that did not consider the surfactant effects of the organic compounds. We demonstrated that better agreement between the calculated and measured ARs could be obtained by adjusting σs∕a. Various schemes were proposed to predict the CCN number concentration (NCCN) based on the HTDMA and AMS measurements. In general, the predicted NCCN agreed reasonably well with the corresponding measured ones using different schemes. For the HTDMA measurements, the NCCN value predicted from the real-time AR measurements was slightly smaller (∼6.8 %) than that from the activation diameter (D50) method due to the assumed internal mixing in the D50 prediction. The NCCN values predicted from bulk chemical composition of PM1 were higher (∼11.5 %) than those from size-resolved composition measured by the AMS because a significant fraction of PM1 was composed of inorganic matter. The NCCN values calculated from AMS measurement were underpredicted at 0.1 % and 0.2 % supersaturations, which could be due to underestimation of κorg and overestimation of σs∕a. For SS values of 0.4 % and 0.7 %, slight overpredicted NCCN values were found because of the internal mixing assumption. Our results highlight the need for accurately evaluating the effects of organics on both the hygroscopic parameter κ and the surface tension σ in order to accurately predict CCN activity.
Abstract. Simultaneous measurements of aerosol hygroscopicity and particle-phase chemical composition were performed at a suburban site over the Pearl River Delta region in the late summer of 2016 using a self-assembled hygroscopic tandem differential mobility analyzer (HTDMA) and an Aerodyne quadruple aerosol chemical speciation monitor (ACSM), respectively. The hygroscopic growth factor (HGF) of the Aitken mode (30 nm, 60 nm) and accumulation mode (100 nm, 145 nm) particles were obtained under 90 % relative humidity (RH). An external mixture was observed for particles of every size during this study, with a dominant mode of more-hygroscopic (MH) particles, as aged aerosols dominated due to the anthropogenic influence. The HGF of less-hygroscopic (LH) mode particles increased, while their number fractions decreased during the daytime due to a reduced degree of external mixing that probably resulted from the condensation of gaseous species. These LH mode particles in the early morning or late afternoon could be possibly dominated by carbonaceous material emitted from local automobile exhaust during rush hours. During polluted days with air masses flowing mainly from the coastal areas, the chemical composition of aerosols had a clear diurnal variation and a strong correlation with the mean HGF. Closure analysis was carried out between the HTDMA-measured HGF and the ACSM-derived hygroscopicity using various approximations for the hygroscopic growth factor of organic compounds (HGForg). Considering the assumptions regarding the differences in the mass fraction of each component between PM1 and 145 nm particles, the hygroscopicity-composition closure was achieved using an HGForg of 1.26 for the organic material in the 145 nm particles and a simple linear relationship between the HGForg and the oxidation level inferred from the O:C ratio of the organic material was suggested. Compared with the results from other environments, HGForg obtained from our measurements appeared to be less sensitive to the variation of its oxidation level, which is, however, similar to the observations in the urban atmosphere of other megacities in China. This finding suggests that the anthropogenic precursors or the photooxidation mechanisms might differ significantly between the suburban and urban atmosphere in China and those in other background environments. This may lead to different characteristics of the oxidation products in secondary organic aerosols (SOA) and therefore to a different relationship between the HGForg and its O:C ratio.
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.
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