To assess the primary and secondary sources of fine organic aerosols after the aggressive implementation of air pollution controls during the 2008 Beijing Olympic Games, 12 h PM2.5 values were measured at an urban site at Peking University (PKU) and an upwind rural site at Yufa during the CAREBEIJING-2008 (Campaigns of Air quality REsearch in BEIJING and surrounding region) summer field campaign. The average PM2.5 concentrations were 72.5 +/- 43.6 mu g m(-3) and 64.3 +/- 36.2 mu g m(-3) (average +/- standard deviation, below as the same) at PKU and Yufa, respectively, showing the lowest concentrations in recent years. Combining the results from a CMB (chemical mass balance) model and secondary organic aerosol (SOA) tracer-yield model, five primary and four secondary fine organic aerosol sources were compared with the results from previous studies in Beijing. The relative contribution of mobile sources to PM2.5 concentrations was increased in 2008, with diesel engines contributing 16.2 +/- 5.9% and 14.5 +/- 4.1% and gasoline vehicles contributing 10.3 +/- 8.7% and 7.9 +/- 6.2% to organic carbon (OC) at PKU and Yufa, respectively. Due to the implementation of emission controls, the absolute OC concentrations from primary sources were reduced during the Olympics, and the contributions from secondary formation of OC represented a larger relative source of fine organic aerosols. Compared with the non-controlled period prior to the Olympics, primary vehicle contributions were reduced by 30% at the urban site and 24% at the rural site. The reductions in coal combustion contributions were 57% at PKU and 7% at Yufa. Our results demonstrate that the emission control measures implemented in 2008 significantly alleviated the primary organic particle pollution in and around Beijing. However, additional studies are needed to provide a more comprehensive assessment of the emission control effectiveness on SOA formation.

Radiocarbon (C-14) has become a powerful tracer in source apportionments of atmospheric carbonaceous particles. Fine particles (PM2.5) were collected at a rural site of Beijing in the summer and winter of 2007. The fractions of contemporary carbon (f(C)) in total carbon (TC) and elemental carbon (EC) are presented using C-14 measurements. This value directly represents the contemporary biogenic contribution, since recently living biomass and biogenic organic compound emissions have f(C) = 1, whereas anthropogenic emissions from fossil carbon have f(C) = 0 because the C-14 in the latter has completely decayed. The measured f(C) (TC) values range from 0.30 to 0.38 (n = 12) in winter and 0.31 to 0.44 (n = 12) in summer, respectively. The levels of f(C) values are lower than those from other rural sites in the world, indicating that the Yufa site was heavily influenced by anthropogenic emissions. The high TC concentrations in winter with the lower average f(C) (TC) suggest that coal burning for residential heating was significant contributors to the TC concentrations. The sources of contemporary carbon are primary emissions due to biomass burning, and biogenic secondary organic aerosol. Biomass burning was a dominant contributor in the winter. Fossil fuels represented 80-87% of EC in both seasons. (C) 2012 Elsevier Ltd. All rights reserved.

Both organic carbon (OC) and elemental carbon (EC) were measured during PRIDE-PRD 2006 summer campaign by using a semi-continuous thermal-optical carbon analyzer at a rural site, Back Garden (BG), which is located 50 km to the northwest of Guangzhou City. Together with the online EC/OC analyzer, various kinds of instruments related to aerosol chemical properties were employed here, which provided a good opportunity to check data quality. The concentrations of OC correlated well with the mass of organic matter (OM) and water soluble organic carbon (WSOC), implying the reliability of the data measured in this campaign. The average OC concentrations in fine particle for three typical periods during the campaign (local emission influence, typhoon and precipitation and normal days) were 28.1 mu gC m(-3), 4.0 mu gC m(-3) and 5.7 mu gC m(-3), respectively; and EC were 11.6 mu gC m(-3), 1.8 mu gC m(-3), and 3.3 mu gC m(-3), respectively. The diurnal patterns of EC and OC during the campaign were higher at night and in early morning than daytime, which was probably caused by the primary emission and accumulation in the occurrence of low boundary layer. Compared with the constant diurnal enhancement ratios of EC, the enhancement ratio of OC (OC versus (CO-CObackground)) kept in a relative high level in the afternoon, with a similar diurnal profile to oxygenated organic aerosol (OOA), due to the strong photochemical formation of OC. Here, a modified EC tracer method was used to estimate the formation of secondary organic carbon (SOC). These results showed that the average SOC concentration (normal days) at BG site was about 2.0 +/- 2.3 mu gC m(-3), and the SOC fraction in OC could reach up to 80% with the average of 47 %. The modified approach in this study proved to be effective and reliable for SOC estimation based on good correlations between estimated SOC versus OOA or WSOC, and estimated POC versus hydrocarbon-like organic aerosol (HOA).

Simultaneous measurements of aerosol size, distribution of number, mass, and chemical compositions were conducted in the winter of 2007 in Beijing using a Twin Differential Mobility Particle Sizer and a Micro Orifice Uniform Deposit Impactor. Both material density and effective density of ambient particles were estimated to be 1.61 +/- 0.13 g cm(-3) and 1.62 +/- 0.38 g cm(-3) for PM1.8 and 1.73 +/- 0.14 g cm(-3) and 1.67 +/- 0.37 g cm(-3) for PM10. Effective density decreased in the nighttime, indicating the primary particles emission from coal burning influenced the density of ambient particles. Size-resolved material density and effective density showed that both values increased with diameter from about 1.5 g cm(-3) at the size of 0.1 mu m to above 2.0 g cm(-3) in the coarse mode. Material density was significantly higher for particles between 0.56 and 1.8 mu m during clean episodes. Dynamic Shape Factors varied within the range of 0.95-1.13 and decreased with particle size, indicating that coagulation and atmospheric aging processes may change the shape of particles.

Ambient aerosol samples were collected at an urban site and an upwind rural site of Beijing during the CAREBEIJING-2008 (Campaigns of Air quality REsearch in BEIJING and surrounding region) summer field campaign. Contributions of primary particles and secondary organic aerosols (SOA) were estimated by chemical mass balance (CMB) modeling and tracer-yield method. The apportioned primary and secondary sources explain 73.8% +/- 9.7% and 79.6% +/- 10.1% of the measured OC at the urban and rural sites, respectively. Secondary organic carbon (SOC) contributes to 32.5 +/- 15.9% of the organic carbon (OC) at the urban site, with 17.4 7.6% from toluene, 9.7 +/- 5.4% from isoprene, 5.1 +/- 2.0% from alpha-pinene, and 2.3 +/- 1.7% from beta-caryophyllene. At the rural site, the secondary sources are responsible for 38.4 +/- 14.4% of the OC, with the contributions of 17.3 +/- 6.9%, 13.9 9.1%, 5.6 1.9%, and 1.7 1.0% from toluene, isoprene, alpha-pinene, and beta-caryophyllene, respectively. Compared with other regions in the world, SOA in Beijing is less aged, but the concentrations are much higher; between the sites, SOA is more aged and affected by regional transport at the urban site. The high SOA loading in Beijing is probably attributed to the high regional SOC background (similar to 2 mu g m(-3)). The toluene SOC concentration is high and comparable at the two sites, implying that some anthropogenic components, at least toluene SOA, are widespread in Beijing and represents a major factor in affecting the regional air quality. The aerosol gaseous precursor concentrations and temperature correlate well with SOA, both affecting SOA formation. The significant SOA enhancement with increasing water uptake and acidification indicates that the aqueous-phase reactions are largely responsible SOA formation in Beijing.

In order to characterize the features of particulate pollution in the Pearl River Delta (PRD) in the summer, continuous measurements of particle number size distributions and chemical compositions were simultaneously performed at Guangzhou urban site (GZ) and Back-garden downwind regional site (BG) in July 2006. Particle number concentration from 20 nm to 10 mu m at BG was (1.7 +/- 0.8) x 10(4) cm(-3), about 40% lower than that at GZ, (2.9 +/- 1.1) x 10(4) cm(-3). The total particle volume concentration at BG was 94 +/- 34 mu m(3) cm(-3), similar to that at GZ, 96 +/- 43 mu m(3) cm(-3). More 20-100 nm particles, significantly affected by the traffic emissions, were observed at GZ, while 100-660 nm particle number concentrations were similar at both sites as they are more regional. PM(2.5) values were similar at GZ (69 +/- 43 mu g m(-3)) and BG (69 +/- 58 mu g m(-3)) with R(2) of 0.71 for the daily average PM(2.5) at these two sites, indicating the fine particulate pollution in the PRD region to be regional. Two kinds of pollution episodes, the accumulation pollution episode and the regional transport pollution episode, were observed. Fine particles over 100 nm dominated both number and volume concentrations of total particles during the late periods of these pollution episodes. Accumulation and secondary transformation are the main reasons for the nighttime accumulation pollution episode. SO(4)(2-), NO(3)(-), and NH(4)(+) accounted for about 60% in 100-660 nm particle mass and PM(2.5) increase. When south or southeast wind prevailed in the PRD region, regional transport of pollutants took place. Regional transport contributed about 30% to fine particulate pollution at BG during a regional transport case. Secondary transformation played an important role during regional transport, causing higher increase rates of secondary ions in PM(1.0) than other species and shifting the peaks of sulfate and ammonium mass size distributions to larger sizes. SO(4)(2-), NO(3)(-), and NH(4)(+) accounted for about 70% and 40% of PM(1.0) and PM(2.5), respectively.

To characterize aerosol pollution in Beijing, size-resolved aerosols were collected by MOUDIs during CAREBEIJING-2006 field campaign at Peking University (urban site) and Yufa (upwind rural site). Fine particle concentrations (PM1.8 by MOUDI) were 99.8 +/- 77.4 mu g/m(3) and 78.2 +/- 58.4 mu g/m(3), with PM1.8/PM10 ratios of 0.64 +/- 0.08 and 0.76 +/- 0.08 at PKU and Yufa, respectively, and secondary compounds accounted for more than 50% in fine particles. PMF model analysis was used to resolve the particle modes. Three modes were resolved at Yufa, representing condensation, droplet and coarse mode. However, one more droplet mode with bigger size was resolved, which was considered probably from regional transport. Condensation mode accounted for 10%-60% of the total mass at both sites, indicating that the gas-to-particle condensation process was important in summer. The formation of sulfate was mainly attributed to in-cloud or aerosol droplet process (PKU 80%, Yufa 70%) and gas condensation process (PKU 14%, Yufa 22%). According to the thermodynamic instability of NH4NO3, size distributions of nitrate were classified as three categories by RH. The existence of Ca(NO3)(2) in droplet mode indicated the reaction of HNO3 with crustal particles was also important in fine particles. A rough estimation was given that 69% of the PM10 and 87% of the PM1.8 in Beijing urban were regional contributions. Sulfate, ammonium and oxalate were formed regionally, with the regional contributions of 90%, 87% and 95% to PM1.8. Nitrate formation was local dominant. In summary regional secondary formation led to aerosol pollution in the summer of Beijing.

Aerosol mass spectrometry has proved to be a powerful tool to measure submicron particulate composition with high time resolution. Factor analysis of mass spectra (MS) collected worldwide by aerosol mass spectrometer (AMS) demonstrates that submicron organic aerosol (OA) is usually composed of several major components, such as oxygenated (OOA), hydrocarbon-like (HOA), biomass burning (BBOA), and other primary OA. In order to help interpretation of component MS from factor analysis of ambient OA datasets, AMS measurements of different primary sources is required for comparison. Such work, however, has been very scarce in the literature, especially for high resolution MS (HR-MS) measurements, which performs improved characterization by separating the ions of different elemental composition at each m/z in comparison with unit mass resolution MS (UMR-MS) measurements. In this study, primary emissions from four types of Chinese cooking (CC) and six types of biomass burning (BB) were simulated systematically and measured using an Aerodyne High-Resolution Time-of-Flight AMS (HR-ToF-AMS). The MS of the CC emissions show high similarity, with m/z 41 and m/z 55 being the highest signals; the MS of the BB emissions also show high similarity, with m/z 29 and m/z 43 being the highest signals. The MS difference between the CC and BB emissions is much bigger than that between different CC (or BB) types, especially for the HR-MS. The O/C ratio of OA ranges from 0.08 to 0.13 for the CC emissions and from 0.18 to 0.26 for the BB emissions. The UMR ions of m/z 43, m/z 44, m/z 57, and m/z 60, usually used as tracers in AMS measurements, were examined for their HR-MS characteristics in the CC and BB emissions. In addition, the MS of the CC and BB emissions are also compared with component MS from factor analysis of ambient OA datasets observed in China, as well as with other AMS measurements of primary sources in the literature. The MS signatures of cooking and biomass burning emissions revealed in this study can be used as important reference for factor analysis of ambient OA datasets, especially for the relevant studies in East Asia.

The Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing-2006) were mainly focused on the influence of the regional aerosol on the air pollution in Beijing. The urban aerosol was characterized in detail. The particle size distributions were also compared to those measured at a regional site (Yufa) approximately 50 km south of the urban site at Peking University (PKU). At PKU, total particle number and volume concentrations were (1.8 +/- 0.8) x 10(4) cm(-3) and 83.5 +/- 57.9 mu m(3) cm(-3), respectively. Days in three consecutive summers of 2004, 2005, and 2006 were classified as polluted days with PM10 over 150 mu g m(-3) and nonpolluted days with lower PM10. On nonpolluted days, particle number size distributions showed a maximum at about 60 nm with Aitken mode particles dominating number concentration. On polluted days, the contribution of accumulation mode particles increased, shifting the maximum of the number size distribution to over 80 nm. On polluted days with stagnant meteorological conditions, secondary aerosol dominated, with SO42-, NO3-, and NH4+ accounting for over 60% of accumulation mode particle mass. Particle number size distributions at both sites were similar. Number and volume concentrations of total particles at Yufa were 6% and 12% lower, respectively; those of accumulation mode particles were 2% and 15% lower. This means that air pollution in Beijing is mainly a regional problem. The regional accumulation mode particles are a metric for assessing the air quality since they influence most the visibility and total mass concentration. Their number and volume concentrations on polluted days were 5 x 10(3) cm(-3) and 30 mu m(3) cm(-3), respectively. Five new particle formation (NPF) events with continuous smooth growth were observed at both PKU and Yufa during CAREBeijing-2006. These NPF events are regional or semiregional. Growth rates at PKU ranged from 1.2 to 5.6 nm h(-1), and formation rates ranged from 1.1 to 22.4 cm(-3) s(-1). SO42-, NH4+, and oxalate might be important contributors to NPF events.

Fine particles (PM2.5, i.e., particles with an aerodynamic diameter of <= 2.5 mu m) were collected from the air in August 2005, August-September 2006, and January-February 2007, in Beijing, China. The chemical compositions of particulate organic matter in the ambient samples were quantified by gas chromatography/mass spectrometry. The dominant compounds identified in summertime were n-alkanoic acids, followed by dicarboxylic acids and sugars, while sugars became the most abundant species in winter, followed by polycyclic aromatic hydrocarbons, n-alkanes, and n-alkanoic acids. The contributions of seven emission sources (i.e., gasoline/diesel vehicles, coal burning, wood/straw burning, cooking, and vegetative detritus) to particulate organic matter in PM2.5 were estimated using a chemical mass balance receptor model. The model results present the seasonal trends of source contributions to organic aerosols. Biomass burning (straw and wood) had the highest contribution in winter, followed by coal burning, vehicle exhaust, and cooking. The contribution of cooking was the highest in summer, followed by vehicle exhaust and biomass burning, while coal smoke showed only a minor contribution to ambient organic carbon.

To further understand and improve air quality for the 2008 Beijing Olympic Games, the Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing-2006) were carried out in an urban and a suburban area from 10 August to 12 September 2006. As a part of an intensive series of measurements, the optical and physical properties of the aerosol were monitored together with identification of the chemical species involved. A method to calculate the hygroscopic factor for aerosol scattering f(RH), defined as the ratio of the aerosol scattering coefficient at given relative humidity (RH) to that at 35% RH, is proposed on the basis of the optical parameters. Over the course of the study f(80%) = 1.63 +/- 0.19. The observation that the molar ratio of NH4+ to (2*SO42- plus NO3-) was very close to 1 implies that the chemical form of the sulfate aerosol may be ammonium sulfate (NH4)(2)SO4 and that nitrate possibly existed as NH4NO3. On the basis of the measurements of size-resolved chemistry, RH, and published functional relationships between the chemical composition and water uptake, the aerosol scattering coefficients could be calculated by the Mie theory for the major particle species (ammonium sulfate, ammonium nitrate, sodium chloride, particulate organic matter, elemental carbon, and residual material). This retrieval method synthesizes the high temporal resolution of mass concentration measurements and low temporal resolution size distribution for water soluble ionic components and carbonaceous aerosols. A local closure experiment is obtained by comparing the measured f(RH) with model calculations using aerosol chemical composition and chemical thermodynamics. Results from the closure study show that the measured and the predicted values of f(RH) agree within measurement uncertainties.