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 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 (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 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 accumuCorrespondence to: C. S. Zhao (zcs@pku.edu.cn) lation 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.

Abstract. North China Plain (NCP) is one of the most densely populated regions in China and has experienced enormous economic growth in the past decades. Its regional trace gas pollution has also become one of the top environmental concerns in China. Measurements of surface trace gases, including O 3 , NO x , SO 2 and CO were carried out within the HaChi (Haze in China) project at Wuqing Meteorology Station, located between 2 mega-cities (Beijing and Tianjin) in the NCP, from 9 July 2009 to 21 January 2010. Detailed statistical analyses were made in order to provide information on the levels of the measured air pollutants and their characteristics. Gaseous air pollutant concentrations were also studied together with meteorological data and satellite data to help us better understand the causes of the observed variations in the trace gases during the field campaign. In comparison to measurements from other rural and background stations in the NCP, relatively high concentrations were detected in Wuqing, presumably due to regional mixing and transport of pollutants. Local meteorology had deterministic impacts on air pollution levels, which have to be accounted for when evaluating other effects on pollutant concentrations. Trace gas concentrations showed strong dependence on wind, providing information on regional pollution characteristics. O 3 mixing ratio also showed clear dependencies on temperature and relative humidity.

[1] Ozone and its precursors were measured from 15 June 2006 to 14 June 2007 at an urban site in Shanghai and used to characterize photochemical oxidant production in this region. During the observation period, ozone displays a seasonal variation with a maximum in spring. Observed nitrogen oxides (NOx) and carbon monoxide (CO) reached a maximum in winter and a minimum in summer. NOx and CO has a similar double-peak diurnal cycle, implying that they are largely of motor vehicle origin. Total nonmethane organic compounds (NMOC) concentrations averaged over the morning, and the 24-hour periods have a large day-to-day variation with no apparent seasonal cycle. Aromatics play a dominant role in contributing to total NMOC reactivity and ozone-forming potential. Anthropogenic NMOC of diverse sources are major components of total NMOC and consist mainly of moderate and low reactivity species. In contrast, relatively low levels of biogenic NMOC concentrations were observed in urban Shanghai. The early morning NMOC/NOx ratios are typically below 8:1 with an average of around 4:1, indicating that the sampling location is situated in a NMOC-limited regime. Model simulations confirm that potential photochemical ozone production in Shanghai is NMOC-sensitive. It is presently difficult to predict the impact of future human activities, such as the increase of automobiles and vegetation-covered landscapes and the reduction of aerosol on ozone pollution in the fast developing megacities of China, and additional studies are needed to better understand the highly nonlinear ozone problem.

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 Cloud Condensation Nuclei (CCN) closure study is conducted with bulk CCN number concentration (N CCN ) and calculated CCN number concentration based on the aerosol number size distribution and size-resolved activation properties.The observed CCN number concentration (N CCN-obs ) are higher than those observed in other locations than China, with average N CCN-obs of roughly 2000, 3000, 6000, 10 000 and 13 000 cm 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 particleCorrespondence to: C. S. Zhao (zcs@pku.edu.cn) 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.The calculated CCN number concentrations (N CCN-calc ) based on the size-resolved activation ratio and aerosol number size distribution correlate well with the N CCN-obs , and show an average overestimation of 19%. Sensitivity studies of the CCN closure show that the N CCN at each supersaturation is well predicted with the campaign average of sizeresolved activation curves. These results indicate that the aerosol number size distribution is critical in the prediction of possible CCN. The CCN number concentration can be reliably estimated using time-averaged, size-resolved activation efficiencies without accounting for the temporal variations.

Abstract. 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 (K ex ) 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 K ex 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.

Abstract. 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 (σ sp ), the hemispheric back scattering coefficient (σ bsp ), the absorption coefficient (σ ap ), 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 σ sp, 550nm of the dry aerosol in spring and summer are 280±253 and 379±251 Mm −1 , respectively. The average σ ap 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 σ sp and σ bsp are representative of the regional aerosol pollution in the NCP. Pronounced diurnal cycle of σ sp , σ ap 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 under-

Abstract. 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 (r ext-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 r ext-LAC . The diurnal variation of r ext-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 r ext-LAC was found, with high values during the daytime and low values at night. The consistency between the retrieved r ext-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.

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