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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.
- ItemTropospheric aerosol scattering and absorption over central Europe: A closure study for the dry particle state(München : European Geopyhsical Union, 2014) Ma, N.; Birmili, W.; Müller, T.; Tuch, T.; Cheng, Y.F.; Xu, W.Y.; Zhao, C.S.; Wiedensohler, A.This work analyses optical properties of the dry tropospheric aerosol measured at the regional Global Atmosphere Watch (GAW) observation site Melpitz in East Germany. For a continuous observation period between 2007 and 2010, we provide representative values of the dry-state scattering coefficient, hemispheric backscattering coefficient, absorption coefficient, single scattering albedo, and scattering Ångström exponent. Besides the direct measurement, the aerosol scattering coefficient was alternatively computed from experimental particle number size distributions using a Mie model. Within pre-defined limits, a closure could be achieved with the direct measurement. The achievement of closure implies that such calculations can be used as a high-level quality control measure for data sets involving multiple instrumentation. All dry-state optical properties show pronounced annual and diurnal variations, which are attributed to the corresponding variations in the regional emission fluxes, the intensity of secondary particle formation, and the mixing layer height. Air mass classification shows that atmospheric stability is a major factor influencing the dry aerosol properties at the GAW station. In the cold season, temperature inversions limit the volume available for atmospheric mixing, so that the dry-state aerosol optical properties near the ground proved quite sensitive to the geographical origin of the air mass. In the warm season, when the atmosphere is usually well-mixed during daytime, considerably less variability was observed for the optical properties between different air masses. This work provides, on the basis of quality-checked in situ measurements, a first step towards a climatological assessment of direct aerosol radiative forcing in the region under study.
- ItemA new method to determine the mixing state of light absorbing carbonaceous using the measured aerosol optical properties and number size distributions(München : European Geopyhsical Union, 2012) Ma, N.; Zhao, C.S.; Müller, T.; Cheng, Y.F.; Liu, P.F.; Deng, Z.Z.; Xu, W.Y.; Ran, L.; Nekat, B.; van Pinxteren, D.; Gnauk, T.; Müller, K.; Herrmann, H.; Yan, P.; Zhou, X.J.; Wiedensohler, A.In this paper, the mixing state of light absorbing carbonaceous (LAC) was investigated with a two-parameter aerosol optical model and in situ aerosol measurements at a regional site in the North China Plain (NCP). A closure study between the hemispheric backscattering fraction (HBF) measured by an integrating nephelometer and that calculated with a modified Mie model was conducted. A new method was proposed to retrieve the ratio of the externally mixed LAC mass to the total mass of LAC (rext-LAC) based on the assumption that the ambient aerosol particles were externally mixed and consisted of a pure LAC material and a core-shell morphology in which the core is LAC and the shell is a less absorbing material. A Monte Carlo simulation was applied to estimate the overall influences of input parameters of the algorithm to the retrieved rext-LAC. The diurnal variation of rext-LAC was analyzed and the PartMC-MOSAIC model was used to simulate the variation of the aerosol mixing state. Results show that, for internally mixed particles, the assumption of core-shell mixture is more appropriate than that of homogenous mixture which has been widely used in aerosol optical calculations. A significant diurnal pattern of the retrieved rext-LAC was found, with high values during the daytime and low values at night. The consistency between the retrieved rext-LAC and the model results indicates that the diurnal variation of LAC mixing state is mainly caused by the diurnal evolution of the mixing layer.
- 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.