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  • Hansen, A. M. K.; Hong, J.; Raatikainen, T.; Kristensen, K.; Ylisirnio, A.; Virtanen, A.; Petäjä, T.; Glasius, M.; Prisle, N. L. (2015)
    Organosulfates have been observed as constituents of atmospheric aerosols in a wide range of environments; however their hygroscopic properties remain uncharacterised. Here, limonene-derived organosulfates with a molecular weight of 250 Da (L-OS 250) were synthesised and used for simultaneous measurements with a hygroscopicity tandem differential mobility analyser (H-TDMA) and a cloud condensation nuclei counter (CCNC) to determine the hygroscopicity parameter, kappa, for pure L-OS 250 and mixtures of L-OS 250 with ammonium sulfate (AS) over a wide range of humidity conditions. The kappa values derived from measurements with H-TDMA decreased with increasing particle dry diameter for all chemical compositions investigated, indicating that kappa H-TDMA depends on particle diameter and/or surface effects; however, it is not clear if this trend is statistically significant. For pure L-OS 250, kappa was found to increase with increasing relative humidity, indicating dilution/solubility effects to be significant. Discrepancies in kappa between the sub-and supersaturated measurements were observed for LOS 250, whereas kappa of AS and mixed L-OS 250/AS were similar. This discrepancy was primarily ascribed to limited dissolution of L-OS 250 at subsaturated conditions. In general, hygroscopic growth factor, critical particle diameter and kappa for the mixed L-OS 250/AS particles converged towards the values of pure AS for mixtures with >= 20% w/w AS. Surface tension measurements of bulk aqueous L-OS 250/AS solutions showed that L-OS 250 was indeed surface active, as expected from its molecular structure, decreasing the surface tension of solutions with 24% from the pure water value at a L-OS 250 concentration of 0.0025 mol L-1. Based on these surface tension measurements, we present the first concentration-dependent parametrisation of surface tension for aqueous L-OS 250, which was implemented to different process-level models of L-OS 250 hygroscopicity and CCN activation. The values of kappa obtained from the measurements were compared with kappa calculated applying the volume additive Zdanovskii-Stokes-Robinson mixing rule, as well as kappa modelled from equilibrium Kohler theory with different assumptions regarding L-OS 250 bulk-to-surface partitioning and aqueous droplet surface tension. This study is to our knowledge the first to investigate the hygroscopic properties and surface activity of L-OS 250; hence it is an important first step towards understanding the atmospheric impact of organosulfates.
  • Hong, Juan; Xu, Hanbing; Tan, Haobo; Yin, Changqing; Hao, Liqing; Li, Fei; Cai, Mingfu; Deng, Xuejiao; Wang, Nan; Su, Hang; Cheng, Yafang; Wang, Lin; Petäjä, Tuukka; Kerminen, Veli-Matti (2018)
    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 lesshygroscopic (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 (HGF(org)). 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 HGF(org) 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, HGF(org) 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 HGF(org) and its O : C ratio.
  • Sihto, Sanna-Liisa; Mikkilä, Jyri; Vanhanen, Joonas; Ehn, Mikael; Liao, Li; Lehtipalo, Katrianne; Aalto, Pasi; Duplissy, Jonathan; Petäjä, Tuukka; Kerminen, Veli-Matti; Boy, Michael; Kulmala, Markku (2011)
    As a part of EUCAARI activities, the annual cycle of cloud condensation nuclei (CCN) concentrations and critical diameter for cloud droplet activation as a function of supersaturation were measured using a CCN counter and a HTDMA (hygroscopicity tandem differential mobility analyzer) at SMEAR II station, Hyytiälä, Finland. The critical diameters for CCN activation were estimated from (i) the measured CCN concentration and particle size distribution data, and (ii) the hygroscopic growth factors by applying κ-Köhler theory, in both cases assuming an internally mixed aerosol. The critical diameters derived by these two methods were in good agreement with each other. The effect of new particle formation on the diurnal variation of CCN concentration and critical diameters was studied. New particle formation was observed to increase the CCN concentrations by 70–110%, depending on the supersaturation level. The average value for the κ-parameter determined from hygroscopicity measurements was κ = 0.18 and it predicted well the CCN activation in boreal forest conditions in Hyytiälä. The derived critical diameters and κ-parameter confirm earlier findings with other methods, that aerosol particles at CCN sizes in Hyytiälä are mostly organic, but contain also more hygrosopic, probably inorganic salts like ammonium sulphate, making the particles more CCN active than pure secondary organic aerosol.