Abstract. In this study, 121 daily PM2.5 (aerosol particle with aerodynamic diameter less than 2.5 μm) samples were collected from an urban site in Beijing in four months between April 2009 and January 2010 representing the four seasons. The samples were determined for various compositions, including elements, ions, and organic/elemental carbon. Various approaches, such as chemical mass balance, positive matrix factorization (PMF), trajectory clustering, and potential source contribution function (PSCF), were employed for characterizing aerosol speciation, identifying likely sources, and apportioning contributions from each likely source. Our results have shown distinctive seasonality for various aerosol speciations associated with PM2.5 in Beijing. Soil dust waxes in the spring and wanes in the summer. Regarding the secondary aerosol components, inorganic and organic species may behave in different manners. The former preferentially forms in the hot and humid summer via photochemical reactions, although their precursor gases, such as SO2 and NOx, are emitted much more in winter. The latter seems to favorably form in the cold and dry winter. Synoptic meteorological and climate conditions can overwhelm the emission pattern in the formation of secondary aerosols. The PMF model identified six main sources: soil dust, coal combustion, biomass burning, traffic and waste incineration emission, industrial pollution, and secondary inorganic aerosol. Each of these sources has an annual mean contribution of 16, 14, 13, 3, 28, and 26%, respectively, to PM2.5. However, the relative contributions of these identified sources significantly vary with changing seasons. The results of trajectory clustering and the PSCF method demonstrated that regional sources could be crucial contributors to PM pollution in Beijing. In conclusion, we have unraveled some complex aspects of the pollution sources and formation processes of PM2.5 in Beijing. To our knowledge, this is the first systematic study that comprehensively explores the chemical characterizations and source apportionments of PM2.5 aerosol speciation in Beijing by applying multiple approaches based on a completely seasonal perspective.

Aerosol‐planetary boundary layer (PBL) interactions have been found to enhance air pollution in megacities in China. We show that black carbon (BC) aerosols play the key role in modifying the PBL meteorology and hence enhancing the haze pollution. With model simulations and data analysis from various field observations in December 2013, we demonstrate that BC induces heating in the PBL, particularly in the upper PBL, and the resulting decreased surface heat flux substantially depresses the development of PBL and consequently enhances the occurrences of extreme haze pollution episodes. We define this process as the “dome effect” of BC and suggest an urgent need for reducing BC emissions as an efficient way to mitigate the extreme haze pollution in megacities of China.

Abstract. During winter 2013–2014 aerosol mass spectrometer (AMS) measurements were conducted for the first time with a novel PM2.5 (particulate matter with aerodynamic diameter  ≤ 2.5 µm) lens in two major cities of China: Xi'an and Beijing. We denote the periods with visibility below 2 km as extreme haze and refer to the rest as reference periods. During the measurements in Xi'an an extreme haze covered the city for about a week and the total non-refractory (NR)-PM2.5 mass fraction reached peak concentrations of over 1000 µg m−3. During the measurements in Beijing two extreme haze events occurred, but the temporal extent and the total concentrations reached during these events were lower than in Xi'an. Average PM2.5 concentrations of 537 ± 146 and 243 ± 47 µg m−3 (including NR species and equivalent black carbon, eBC) were recorded during the extreme haze events in Xi'an and Beijing, respectively. During the reference periods the measured average concentrations were 140 ± 99 µg m−3 in Xi'an and 75 ± 61 µg m−3 in Beijing. The relative composition of the NR-PM2.5 evolved substantially during the extreme haze periods, with increased contributions of the inorganic components (mostly sulfate and nitrate). Our results suggest that the high relative humidity present during the extreme haze events had a strong effect on the increase of sulfate mass (via aqueous phase oxidation of sulfur dioxide). Another relevant characteristic of the extreme haze is the size of the measured particles. During the extreme haze events, the AMS showed much larger particles, with a volume weighted mode at about 800 to 1000 nm, in contrast to about 400 nm during reference periods. These large particle sizes made the use of the PM2.5 inlet crucial, especially during the severe haze events, where 39 ± 5 % of the mass would have been lost in the conventional PM1 (particulate matter with aerodynamic diameter ≤ 1 µm) inlet. A novel positive matrix factorization procedure was developed to apportion the sources of organic aerosols (OA) based on their mass spectra using the multilinear engine (ME-2) controlled via the source finder (SoFi). The procedure allows for an effective exploration of the solution space, a more objective selection of the best solution and an estimation of the rotational uncertainties. Our results clearly show an increase of the oxygenated organic aerosol (OOA) mass during extreme haze events. The contribution of OOA to the total OA increased from the reference to the extreme haze periods from 16.2 ± 1.1 to 31.3 ± 1.5 % in Xi'an and from 15.7 ± 0.7 to 25.0 ± 1.2 % in Beijing. By contrast, during the reference periods the total OA mass was dominated by domestic emissions of primary aerosols from biomass burning in Xi'an (42.2 ± 1.5 % of OA) and coal combustion in Beijing (55.2 ± 1.6 % of OA). These two sources are also mostly responsible for extremely high polycyclic aromatic hydrocarbon (PAH) concentrations measured with the AMS (campaign average of 2.1 ± 2.0 µg m−3 and frequent peak concentrations above 10 µg m−3). To the best of our knowledge, this is the first data set where the simultaneous extraction of these two primary sources could be achieved in China by conducting on-line AMS measurements at two areas with contrasted emission patterns.