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- ItemHygroscopic properties of atmospheric aerosol particles over the Eastern Mediterranean: Implications for regional direct radiative forcing under clean and polluted conditions(München : European Geopyhsical Union, 2011) Stock, M.; Cheng, Y.F.; Birmili, W.; Massling, A.; Wehner, B.; Müller, T.; Leinert, S.; Kalivitis, N.; Mihalopoulos, N.; Wiedensohler, A.This work examines the effect of direct radiative forcing of aerosols in the eastern Mediterranean troposphere as a function of air mass composition, particle size distribution and hygroscopicity, and relative humidity (RH). During intensive field measurements on the island of Crete, Greece, the hygroscopic properties of atmospheric particles were determined using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Hygroscopicity Differential Mobility Analyzer-Aerodynamic Particle Sizer (H-DMA-APS). Similar to former studies, the H-TDMA identified three hygroscopic sub-fractions of particles in the sub-μm range: a more hygroscopic group, a less hygroscopic group and a nearly hydrophobic particle group. The average hygroscopic particle growth factors at 90 % RH were a significant function of particle mobility diameter (Dp): 1.42 (± 0.05) at 30 nm compared to 1.63 (± 0.07) at 250 nm. The H-DMA-APS identified up to three hygroscopic sub-fractions at mobility diameters of 1.0 and 1.2 μm. The data recorded between 12 August and 20 October 2005 were classified into four distinct synoptic-scale air mass types distinguishing between different regions of origin (western Mediterranean vs. the Aegean Sea) as well as the degree of continental pollution (marine vs. continentally influenced). The hygroscopic properties of particles with diameter Dp≥150 nm showed the most pronounced dependency on air mass origin, with growth factors in marine air masses exceeding those in continentally influenced air masses. Particle size distributions and hygroscopic growth factors were used to calculate aerosol light scattering coefficients at ambient RH using a Mie model. A main result was the pronounced enhancement of particle scattering over the eastern Mediterranean due to hygroscopic growth, both in the marine and continentally influenced air masses. When RH reached its summer daytime values around 70–80 %, up to 50–70 % of the calculated visibility reduction was due to the hygroscopic growth of the particles by water compared to the effect of the dry particles alone. The estimated aerosol direct radiative forcings for both, marine and continentally influenced air masses were negative indicating a net cooling of the atmosphere due to the aerosol. The radiative forcing ΔFr was nevertheless governed by the total aerosol concentration most of the time: ΔFr was typically more negative for continentally influenced aerosols (ca. −4 W m−2) compared to rather clean marine aerosols (ca. −1.5 W m−2). When RH occasionally reached 90 % in marine air masses, ΔFr even reached values down to −7 W m−2. Our results emphasize, on the basis of explicit particle hygroscopicity measurements, the relevance of ambient RH for the radiative forcing of regional atmospheres.
- 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.
- ItemAerosol optical properties in the North China Plain during HaChi campaign: An in-situ optical closure study(München : European Geopyhsical Union, 2011) Ma, N.; Zhao, C.S.; Nowak, A.; Müller, T.; Pfeifer, S.; Cheng, Y.F.; Deng, Z.Z.; Liu, P.F.; Xu, W.Y.; Ran, L.; Yan, P.; Göbel, T.; Hallbauer, E.; Mildenberger, K.; Henning, S.; Yu, J.; Chen, L.L.; Zhou, X.J.; Stratmann, F.; Wiedensohler, A.The largest uncertainty in the estimation of climate forcing stems from atmospheric aerosols. In early spring and summer of 2009, two periods of in-situ measurements on aerosol physical and chemical properties were conducted within the HaChi (Haze in China) project at Wuqing, a town between Beijing and Tianjin in the North China Plain (NCP). Aerosol optical properties, including the scattering coefficient (σsp), the hemispheric back scattering coefficient (σbsp), the absorption coefficient (σap), as well as the single scattering albedo (ω), are presented. The diurnal and seasonal variations are analyzed together with meteorology and satellite data. The mean values of σsp, 550 nm of the dry aerosol in spring and summer are 280±253 and 379±251 Mm−1, respectively. The average σap for the two periods is respectively 47±38 and 43±27 Mm−1. The mean values of ω at the wavelength of 637 nm are 0.82±0.05 and 0.86±0.05 for spring and summer, respectively. The relative high levels of σsp and σbsp are representative of the regional aerosol pollution in the NCP. Pronounced diurnal cycle of $σsp, σap and ω are found, mainly influenced by the evolution of boundary layer and the accumulation of local emissions during nighttime. The pollutants transported from the southwest of the NCP are more significant than that from the two megacities, Beijing and Tianjin, in both spring and summer. An optical closure experiment is conducted to better understand the uncertainties of the measurements. Good correlations (R>0.98) are found between the values measured by the nephelometer and the values calculated with a modified Mie model. The Monte Carlo simulation shows an uncertainty of about 30 % for the calculations. Considering all possible uncertainties of measurements, calculated σsp and σbsp agree well with the measured values, indicating a stable performance of instruments and thus reliable aerosol optical data.