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- ItemThe impact of aerosol hygroscopic growth on the single-scattering albedo and its application on the NO2 photolysis rate coefficient(München : European Geopyhsical Union, 2014) Tao, J.C.; Zhao, C.S.; Ma, N.; Liu, P.F.Hygroscopic growth of aerosol particles can significantly affect their single-scattering albedo (ω), and consequently alters the aerosol effect on tropospheric photochemistry. In this study, the impact of aerosol hygroscopic growth on ω and its application to the NO2 photolysis rate coefficient (JNO2) are investigated for a typical aerosol particle population in the North China Plain (NCP). The variations of aerosol optical properties with relative humidity (RH) are calculated using a Mie theory aerosol optical model, on the basis of field measurements of number–size distribution and hygroscopic growth factor (at RH values above 90%) from the 2009 HaChi (Haze in China) project. Results demonstrate that ambient ω has pronouncedly different diurnal patterns from ω measured at dry state, and is highly sensitive to the ambient RHs. Ambient ω in the NCP can be described by a dry state ω value of 0.863, increasing with the RH following a characteristic RH dependence curve. A Monte Carlo simulation shows that the uncertainty of ω from the propagation of uncertainties in the input parameters decreases from 0.03 (at dry state) to 0.015 (RHs > 90%). The impact of hygroscopic growth on ω is further applied in the calculation of the radiative transfer process. Hygroscopic growth of the studied aerosol particle population generally inhibits the photolysis of NO2 at the ground level, whereas accelerates it above the moist planetary boundary layer. Compared with dry state, the calculated JNO2 at RH of 98% at the height of 1 km increases by 30.4%, because of the enhancement of ultraviolet radiation by the humidified scattering-dominant aerosol particles. The increase of JNO2 due to the aerosol hygroscopic growth above the upper boundary layer may affect the tropospheric photochemical processes and this needs to be taken into account in the atmospheric chemical models.
- ItemHygroscopic properties of aerosol particles at high relative humidity and their diurnal variations in the North China Plain(München : European Geopyhsical Union, 2011) Liu, P.F.; Zhao, C.S.; Göbel, T.; Hallbauer, E.; Nowak, A.; Ran, L.; Xu, W.Y.; Deng, Z.Z.; Ma, N.; Mildenberger, K.; Henning, S.; Stratmann, F.; Wiedensohler, A.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 diameters between 50 and 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 (D0 = 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 (D0 = 100 nm). The hygroscopic growth behaviours at different RHs were well represented by 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. 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. 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.
- ItemA parameterization of low visibilities for hazy days in the North China Plain(München : European Geopyhsical Union, 2012) Chen, J.; Zhao, C.S.; Ma, N.; Liu, P.F.; Göbel, T.; Hallbauer, E.; Deng, Z.Z.; Ran, L.; Xu, W.Y.; Liang, Z.; Liu, H.J.; Yan, P.; Zhou, X.J.; Wiedensohler, A.Visibility degradation is a pervasive and urgent environmental problem in China. The occurrence of low visibility events is frequent in the North China Plain, where the aerosol loading is quite high and aerosols are strongly hygroscopic. A parameterization of light extinction (Kex) for low visibilities on hazy days is proposed in this paper, based on visibility, relative humidity (RH), aerosol hygroscopic growth factors and particle number size distributions measured during the Haze in China (HaChi) Project. Observational results show that a high aerosol volume concentration is responsible for low visibility at RH <90%; while for RH >90%, decrease of visibility is mainly influenced by the increase of RH. The parameterization of Kex is developed on the basis of aerosol volume concentrations and RH, taking into accounts the sensitivity of visibility to the two factors and the availability of corresponding data. The extinction coefficients calculated with the parameterization schemes agree well with the directly measured values.
- ItemAerosol hygroscopicity parameter derived from the light scattering enhancement factor measurements in the North China Plain(Göttingen : Copernicus, 2014) Chen, J.; Zhao, C.S.; Ma, N.; Yan, P.The relative humidity (RH) dependence of aerosol light scattering is an essential parameter for accurate estimation of the direct radiative forcing induced by aerosol particles. Because of insufficient information on aerosol hygroscopicity in climate models, a more detailed parameterization of hygroscopic growth factors and resulting optical properties with respect to location, time, sources, aerosol chemistry and meteorology are urgently required. In this paper, a retrieval method to calculate the aerosol hygroscopicity parameter, κ, is proposed based on the in situ measured aerosol light scattering enhancement factor, namely f(RH), and particle number size distribution (PNSD) obtained from the HaChi (Haze in China) campaign. Measurements show that f(RH) increases sharply with increasing RH, and that the time variance of f(RH) is much greater at higher RH. A sensitivity analysis reveals that the f(RH) is more sensitive to the aerosol hygroscopicity than PNSD. f(RH) for polluted cases is distinctly higher than that for clean periods at a specific RH. The derived equivalent κ, combined with the PNSD measurements, is applied in the prediction of the cloud condensation nuclei (CCN) number concentration. The predicted CCN number concentration with the derived equivalent κ agrees well with the measured ones, especially at high supersaturations. The proposed calculation algorithm of κ with the f(RH) measurements is demonstrated to be reasonable and can be widely applied.
- ItemA study of aerosol liquid water content based on hygroscopicity measurements at high relative humidity in the North China Plain(München : European Geopyhsical Union, 2014) Bian, Y.X.; Zhao, C.S.; Ma, N.; Chen, J.; Xu, W.Y.Water can be a major component of aerosol particles, also serving as a medium for aqueous-phase reactions. In this study, a novel method is presented to calculate the aerosol liquid water content at high relative humidity based on measurements of aerosol hygroscopic growth factor, particle number size distribution and relative humidity in the Haze in China (HaChi) summer field campaign (July–August 2009) in the North China Plain. The aerosol liquid water content calculated using this method agreed well with that calculated using a thermodynamic equilibrium model (ISORROPIA II) at high relative humidity (>60%) with a correlation coefficient of 0.96. At low relative humidity (<60%), an underestimation was found in the calculated aerosol liquid water content by the thermodynamic equilibrium model. This discrepancy mainly resulted from the ISORROPIA II model, which only considered limited aerosol chemical compositions. The mean and maximum values of aerosol liquid water content during the HaChi campaign reached 1.69 × 10−4 g m−3 and 9.71 × 10−4 g m−3, respectively. A distinct diurnal variation of the aerosol liquid water content was found, with lower values during daytime and higher ones at night. The aerosol liquid water content depended strongly on the relative humidity. The aerosol liquid water content in the accumulation mode dominated the total aerosol liquid water content.