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Size-resolved chemical composition, mixing state, and cloud condensation nucleus (CCN) activity of aerosol particles in polluted mega-city air and biomass burning smoke were measured during the PRIDE-PRD2006 campaign near Guangzhou, China, using an aerosol mass spectrometer (AMS), a volatility tandem differential mobility analyzer (VTDMA), and a continuous-flow CCN counter (DMT-CCNC). The size-dependence and temporal variations of the effective average hygroscopicity parameter for CCN-active particles (κa) could be parameterized as a function of organic and inorganic mass fractions (forg, finorg) determined by the AMS: κa,p=κorg·forg + κinorg·finorg. The characteristic κ values of organic and inorganic components were similar to those observed in other continental regions of the world: κorg≈0.1 and κinorg≈0.6. The campaign average κa values increased with particle size from ~0.25 at ~50 nm to ~0.4 at ~200 nm, while forg decreased with particle size. At ~50 nm, forg was on average 60% and increased to almost 100% during a biomass burning event. The VTDMA results and complementary aerosol optical data suggest that the large fractions of CCN-inactive particles observed at low supersaturations (up to 60% at S≤0.27%) were externally mixed weakly CCN-active soot particles with low volatility (diameter reduction <5% at 300 °C) and effective hygroscopicity parameters around κLV≈0.01. A proxy for the effective average hygroscopicity of the total ensemble of CCN-active particles including weakly CCN-active particles (κt) could be parameterized as a function of κa,p and the number fraction of low volatility particles determined by VTDMA (φLV): κt,p=κa,p−φLV·(κa,p−κLV). Based on κ values derived from AMS and VTDMA data, the observed CCN number concentrations (NCCN,S≈102–104 cm−3 at S = 0.068–0.47%) could be efficiently predicted from the measured particle number size distribution. The mean relative deviations between observed and predicted CCN concentrations were ~10% when using κt,p, and they increased to ~20% when using only κa,p. The mean relative deviations were not higher (~20%) when using an approximate continental average value of κ≈0.3, although the constant κ value cannot account for the observed temporal variations in particle composition and mixing state (diurnal cycles and biomass burning events). Overall, the results confirm that on a global and climate modeling scale an average value of κ≈0.3 can be used for approximate predictions of CCN number concentrations in continental boundary layer air when aerosol size distribution data are available without information about chemical composition. Bulk or size-resolved data on aerosol chemical composition enable improved CCN predictions resolving regional and temporal variations, but the composition data need to be highly accurate and complemented by information about particle mixing state to achieve high precision (relative deviations <20%).

This study was part of the international field measurement Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing‐2006). We investigated a new particle formation event in a highly polluted air mass at a regional site south of the megacity Beijing and its impact on the abundance and properties of cloud condensation nuclei (CCN). During the 1‐month observation, particle nucleation followed by significant particle growth on a regional scale was observed frequently (∼30%), and we chose 23 August 2006 as a representative case study. Secondary aerosol mass was produced continuously, with sulfate, ammonium, and organics as major components. The aerosol mass growth rate was on average 19 μg m−3 h−1 during the late hours of the day. This growth rate was observed several times during the 1‐month intensive measurements. The nucleation mode grew very quickly into the size range of CCN, and the CCN size distribution was dominated by the growing nucleation mode (up to 80% of the total CCN number concentration) and not as usual by the accumulation mode. At water vapor supersaturations of 0.07–0.86%, the CCN number concentrations reached maximum values of 4000–19,000 cm−3 only 6–14 h after the nucleation event. During particle formation and growth, the effective hygroscopicity parameter κ increased from about 0.1–0.3 to 0.35–0.5 for particles with diameters of 40–90 nm, but it remained nearly constant at ∼0.45 for particles with diameters of ∼190 nm. This result is consistent with aerosol chemical composition data, showing a pronounced increase of sulfate.

Soot particles are the most efficient light absorbing aerosol species in the atmosphere, playing an important role as a driver of global warming. Their climate effects strongly depend on their mixing state, which significantly changes their light absorbing capability and cloud condensation nuclei (CCN) activity. Therefore, knowledge about the mixing state of soot and its aging mechanism becomes an important topic in the atmospheric sciences. The size-resolved (30–320 nm diameter) mixing state of soot particles in polluted megacity air was measured at a suburban site (Yufa) during the CAREBeijing 2006 campaign in Beijing, using a volatility tandem differential mobility analyzer (VTDMA). Particles in this size range with non-volatile residuals at 300 °C were considered to be soot particles. On average, the number fraction of internally mixed soot in total soot particles (Fin), decreased from 0.80 to 0.57 when initial Dp increased from 30 to 320 nm. Further analysis reveals that: (1) Fin was well correlated with the aerosol hygroscopic mixing state measured by a CCN counter. More externally mixed soot particles were observed when particles showed more heterogeneous features with regard to hygroscopicity. (2) Fin had pronounced diurnal cycles. For particles in the accumulation mode (Dp at 100–320 nm), largest Fin were observed at noon time, with \"apparent\" turnover rates (kex → in) up to 7.8% h−1. (3) Fin was subject to competing effects of both aging and emissions. While aging increases Fin by converting externally mixed soot particles into internally mixed ones, emissions tend to reduce Fin by emitting more fresh and externally mixed soot particles. Similar competing effects were also found with air mass age indicators. (4) Under the estimated emission intensities, actual turnover rates of soot (kex → in) up to 20% h−1 were derived, which showed a pronounced diurnal cycle peaking around noon time. This result confirms that (soot) particles are undergoing fast aging/coating with the existing high levels of condensable vapors in the megacity Beijing. (5) Diurnal cycles of Fin were different between Aitken and accumulation mode particles, which could be explained by the faster growth of smaller Aitken mode particles into larger size bins. To improve the Fin prediction in regional/global models, we suggest parameterizing Fin by an air mass aging indicator, i.e., Fin = a + bx, where a and b are empirical coefficients determined from observations, and x is the value of an air mass age indicator. At the Yufa site in the North China Plain, fitted coefficients (a, b) were determined as (0.57, 0.21), (0.47, 0.21), and (0.52, 0.0088) for x (indicators) as [NOz]/[NOy], [E]/[X] ([ethylbenzene]/[m,p-xylene]) and ([IM] + [OM])/[EC] ([inorganic + organic matter]/[elemental carbon]), respectively. Such a parameterization consumes little additional computing time, but yields a more realistic description of Fin compared with the simple treatment of soot mixing state in regional/global models.

An aerosol optical closure study was performed using the observed high time‐ and size‐resolved soot mixing states determined by a Volatility Tandem Differential Mobility Analyzer (VTDMA) at a polluted regional site, Yufa, in the south of Beijing during the summer of 2006. Good agreement was found between the simulated and measured aerosol absorption (σap, R = 0.9) and scattering (σsp, R ≥ 0.95). The soot mixing state at Yufa can be generally determined by VTDMA, in terms of properly predicting the σap using a simple optical model combined with spherical homogeneous and core‐shell coated Mie codes. The possible uncertainties in the modeled σap were discussed. Rapid soot aging was observed, which led to large variations in the fractional contributions to σap by externally mixed and coated soot. On average, about 37% of the σap (∼10–60%) arose by the coated soot. The coating enhancement in σap and σsp of the coated soot can reach up to a factor of 8–10 within several hours owing to the secondary processing during daytime. It was contributed not only by the increased thickness of coating shell, but also the transition of soot from externally mixed to coated one. Hence, assuming constant soot mixing state for the regional climate model is not realistic and may lead to uncertainties. In the highly polluted region in northeastern China, the aerosol single scattering albedo may increase very fast owing to the rapid secondary particle formation and condensation (up to 0.90–0.95). This increase took place although the concurrent coating processing enhanced the light absorption capability of soot.

The droplet aerosol analyzer (DAA) was developed to study the influence of aerosol properties on clouds. It measures the ambient particle size of individual droplets and interstitial particles, the size of the dry (residual) particles after the evaporation of water vapor and the number concentration of the dry (residual) particles. A method was developed for the evaluation of DAA data to obtain the three-parameter data set: ambient particle diameter, dry (residual) particle diameter and number concentration. First results from in-cloud measurements performed on the summit of Mt. Brocken in Germany are presented. Various aspects of the cloud–aerosol data set are presented, such as the number concentration of interstitial particles and cloud droplets, the dry residue particle size distribution, droplet size distributions, scavenging ratios due to cloud droplet formation and size-dependent solute concentrations. This data set makes it possible to study clouds and the influence of the aerosol population on clouds.

We describe a general-purpose dryer designed for continuous sampling of atmospheric aerosol, where a specified relative humidity (RH) of the sample flow (lower than the atmospheric humidity) is required. It is often prescribed to measure the properties of dried aerosol, for instance for monitoring networks. The specific purpose of our dryer is to dry cloud droplets (maximum diameter approximately 25 μm, highly charged, up to 5 × 102 charges). One criterion is to minimise losses from the droplet size distribution entering the dryer as well as on the residual dry particle size distribution exiting the dryer. This is achieved by using a straight vertical downwards path from the aerosol inlet mounted above the dryer, and removing humidity to a dry, closed loop airflow on the other side of a semi-permeable GORE-TEX membrane (total area 0.134 m2). The water vapour transfer coefficient, k, was measured to be 4.6 × 10-7 kg m−2 s−1% RH−1 in the laboratory (temperature 294 K) and is used for design purposes. A net water vapour transfer rate of up to 1.2 × 10-6 kg s−1 was achieved in the field. This corresponds to drying a 5.7 L min−1 (0.35 m3 h−1) aerosol sample flow from 100% RH to 27% RH at 293 K (with a drying air total flow of 8.7 L min−1). The system was used outdoors from 9 May until 20 October 2010, on the mountain Brocken (51.80° N, 10.67° E, 1142 m a.s.l.) in the Harz region in central Germany. Sample air relative humidity of less than 30% was obtained 72% of the time period. The total availability of the measurement system was >94% during these five months.

In Chinese megacities the problems of air pollution are frequently obvious as hazy layers covering large areas combined with low visibility. To estimate the aerosol effect on regional and global climate, the knowledge of light‐absorbing and light‐scattering compounds as well as their mixing state is essential. A Volatility Tandem DMA (VTDMA) was used to measure nonvolatile fractions (at 300°C) of submicrometer aerosol particles. The remaining size distributions were divided into three fractions, corresponding to particles with a low‐volatile, medium‐volatile, and high‐volatile fraction. The particles with a low‐volatile fraction are equivalent with externally mixed nonvolatile (refractory) material; in the observed size range, this fraction is assumed to consist mainly of soot. Combined with number size distributions, the number and volume concentrations of externally and internally mixed nonvolatile particles were calculated. In a parallel study by Cheng et al. (2009) the results were used in a Mie model and compared with measured absorption coefficients showing a good agreement. During Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing‐2006), large variations in the mixing state were found, especially between new particle formation and heavily polluted days. The fraction of externally mixed soot decreased from ∼37% during clean to 18% during heavily polluted periods, parallel to an increase in particle mass concentration mainly caused by the production of secondary aerosol material. In the nucleation mode, high particle number fractions with high‐volatile fractions were found (∼64% in contrast to ∼24% on a nonevent day); that is, refractory material is produced during nucleation and growth.