Publications (2)0 Total impact
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Article: Size-resolved and bulk activation properties of aerosols in the North China plain: the importance of aerosol size distribution in the prediction of CCN number concentration
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ABSTRACT: Size-resolved and bulk activation properties of aerosols were measured at a regional/suburban site in the North China Plain (NCP), which is occasionally heavily polluted by anthropogenic aerosol particles and gases. A CCN (Cloud Condensation Nuclei) closure study is conducted with bulk CCN number concentration (NCCN) and calculated NCCN based on the aerosol number size distribution and size-resolved activation properties. The observed NCCN are higher than those observed in other locations than China, with average NCCN of roughly 2000, 3000, 6000, 10 000 and 13 000 cm−3 at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.70%, respectively. An inferred critical dry diameter (Dm) is calculated based on the measured NCCN and aerosol number size distribution assuming homogeneous chemical composition. This inferred cut off diameter varies in a wide range, indicating that it is impossible to predict NCCN with a fixed critical diameter. Size-resolved activation measurements show that most of the 300 nm particles are activated at the investigated supersaturations, while almost no particles of 30 nm are activated even at the highest supersaturation of 0.72%. The activation ratio increases with increasing supersaturation and particle size. The slopes of the activation curves for ambient aerosols are not as steep as those observed in calibrations with ammonium sulfate suggesting that the observed aerosols is an external mixture of more hygroscopic and hydrophobic particles. This conclusion is confirmed by hygroscopicity measurements performed during two intensive field studies in 2009. The calculated NCCN based on the size-resolved activation ratio and aerosol number size distribution correlate well with the measured NCCN, and show an average overestimation of 19%. Sensitivity studies of the CCN closure show that the NCCN for each supersaturation is well predicted with the campaign average of size-resolved activation curves. These results indicate that the aerosol number size distribution is critical in the prediction of possible CCN. The NCCN can be estimated with average activation curve, along with a well described aerosol number size distribution.Atmospheric Chemistry and Physics Discussions. 01/2011; -
Article: Hygroscopic properties of aerosol particles at high relative humidity and their diurnal variations in the North China Plain
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ABSTRACT: The hygroscopic properties of submicron aerosol particles were determined at a suburban site (Wuqing) in the North China Plain among a cluster of cities during the period 17 July to 12 August 2009. A High Humidity Tandem Differential Mobility Analyser (HH-TDMA) instrument was applied to measure the hygroscopic growth factor (GF) at 90%, 95% and 98.5% relative humidity (RH) for particles with dry diameter between 50–250 nm. The probability distribution of GF (GF-PDF) averaged over the period shows a distinct bimodal pattern, namely, a dominant more-hygroscopic (MH) group and a smaller nearly-hydrophobic (NH) group. The MH group particles were highly hygroscopic, and their GF was relatively constant during the period with average values of 1.54±0.02, 1.81±0.04 and 2.45±0.07 at 90%, 95% and 98.5% RH ( D 0=100 nm), respectively. The NH group particles grew very slightly when exposed to high RH, with GF values of 1.08±0.02, 1.13±0.06 and 1.24±0.13, respectively at 90%, 95% and 98.5% RH ( D 0=100 nm). The hygroscopic growth behaviours at different RHs were well represented by the hygroscopicity parameter κ with a single-parameter Köhler model. Thus, the calculation of GF as a function of RH and dry diameter could be facilitated by an empirical parameterization of κ as function of dry diameter. A strong diurnal pattern in number fraction of different hygroscopic groups was observed, indicating a diurnal variation of aerosol mixing state and/or chemical composition. The average number fraction of NH particles during the day was about 8%, while during the nighttime fractions up to 20% were reached. Correspondingly, the state of mixing in terms of water uptake varied significantly during a day. The high fraction of NH particles measured during the night denotes a high degree of external mixing of ambient aerosols, while during the day the degree of external mixing decreased. Simulations using a particle-resolved aerosol box model (PartMC-MOSAIC) suggest that the diurnal variations of aerosol hygroscopicity and mixing state were mainly caused by the evolution of the atmospheric mixing layer. The shallow nocturnal boundary layer during the night facilitated the accumulation of freshly emitted carbonaceous particles (mainly hydrophobic) near the surface while in the morning turbulence entrained the more aged and more hygroscopic particles from aloft and diluted the NH particles near the surface resulting in a decrease in the fraction of NH particles.Atmospheric Chemistry and Physics Discussions. 01/2011;