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Regional severe haze represents an enormous environmental problem in China, influencing air quality, human health, ecosystem, weather, and climate. These extremes are characterized by exceedingly high concentrations of fine particulate matter (smaller than 2.5 µm, or PM2.5) and occur with extensive temporal (on a daily, weekly, to monthly timescale) and spatial (over a million square kilometers) coverage. Although significant advances have been made in field measurements, model simulations, and laboratory experiments for fine PM over recent years, the causes for severe haze formation have not yet to be systematically/comprehensively evaluated. This review provides a synthetic synopsis of recent advances in understanding the fundamental mechanisms of severe haze formation in northern China, focusing on emission sources, chemical formation and transformation, and meteorological and climatic conditions. In particular, we highlight the synergetic effects from the interactions between anthropogenic emissions and atmospheric processes. Current challenges and future research directions to improve the understanding of severe haze pollution as well as plausible regulatory implications on a scientific basis are also discussed.

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Abstract. We simulated elemental carbon (EC) and organic carbon (OC) aerosols in China and compared model results to surface measurements at Chinese rural and background sites, with the goal of deriving "top-down" emission estimates of EC and OC, as well as better quantifying the secondary sources of OC. We included in the model state-of-the-science Chinese "bottom-up" emission inventories for EC (1.92 TgC yr −1 ) and OC (3.95 TgC yr −1 ), as well as updated secondary OC formation pathways. The average simulated annual mean EC concentration at rural and background sites was 1.1 µgC m −3 , 56 % lower than the observed 2.5 µgC m −3 . The average simulated annual mean OC concentration at rural and background sites was 3.4 µgC m −3 , 76 % lower than the observed 14 µgC m −3 . Multiple regression to fit surface monthly mean EC observations at rural and background sites yielded the best estimate of Chinese EC source of 3.05 ± 0.78 TgC yr −1 . Based on the topdown EC emission estimate and observed seasonal primary OC/EC ratios, we estimated Chinese OC emissions to be 6.67 ± 1.30 TgC yr −1 . Using these top-down estimates, the simulated average annual mean EC concentration at rural and background sites was significantly improved to 1.9 µgC m −3 . However, the model still significantly underestimated observed OC in all seasons (simulated average annual mean OC at rural and background sites was 5.4 µgC m −3 ), with little skill in capturing the spatiotemporal variability. Secondary formation accounts for 21 % of Chinese annual mean surface OC in the model, with isoprene being the most important precursor. In summer, as high as 62 % of the observed surface OC may be due to secondary formation in eastern China. Our analysis points to four shortcomings in the current bottom-up inventories of Chinese carbonaceous aerosols: (1) the anthropogenic source is underestimated on a national scale, particularly for OC; (2) the spatiotemporal distributions of emissions are misrepresented; (3) there is a missing source in western China, likely associated with the use of biofuels or other low-quality fuels for heating; and (4) sources in fall are not well represented, either because the seasonal shifting of Published by Copernicus Publications on behalf of the European Geosciences Union. T.-M. Fu et al.: Carbonaceous aerosols in Chinaemissions and/or secondary formation are poorly captured or because specific fall emission events are missing. In addition, secondary production of OC in China is severely underestimated. More regional measurements with better spatiotemporal coverage are needed to resolve these shortcomings.

Abstract. During winter 2013, extremely high concentrations (i.e., 4–20 times higher than the World Health Organization guideline) of PM2.5 (particulate matter with an aerodynamic diameter < 2.5 μm) mass concentrations (24 h samples) were found in four major cities in China including Xi'an, Beijing, Shanghai and Guangzhou. Statistical analysis of a combined data set from elemental carbon (EC), organic carbon (OC), 14C and biomass-burning marker measurements using Latin hypercube sampling allowed a quantitative source apportionment of carbonaceous aerosols. Based on 14C measurements of EC fractions (six samples each city), we found that fossil emissions from coal combustion and vehicle exhaust dominated EC with a mean contribution of 75 ± 8% across all sites. The remaining 25 ± 8% was exclusively attributed to biomass combustion, consistent with the measurements of biomass-burning markers such as anhydrosugars (levoglucosan and mannosan) and water-soluble potassium (K+). With a combination of the levoglucosan-to-mannosan and levoglucosan-to-K+ ratios, the major source of biomass burning in winter in China is suggested to be combustion of crop residues. The contribution of fossil sources to OC was highest in Beijing (58 ± 5%) and decreased from Shanghai (49 ± 2%) to Xi'an (38 ± 3%) and Guangzhou (35 ± 7%). Generally, a larger fraction of fossil OC was from secondary origins than primary sources for all sites. Non-fossil sources accounted on average for 55 ± 10 and 48 ± 9% of OC and total carbon (TC), respectively, which suggests that non-fossil emissions were very important contributors of urban carbonaceous aerosols in China. The primary biomass-burning emissions accounted for 40 ± 8, 48 ± 18, 53 ± 4 and 65 ± 26% of non-fossil OC for Xi'an, Beijing, Shanghai and Guangzhou, respectively. Other non-fossil sources excluding primary biomass burning were mainly attributed to formation of secondary organic carbon (SOC) from non-fossil precursors such as biomass-burning emissions. For each site, we also compared samples from moderately to heavily polluted days according to particulate matter mass. Despite a significant increase of the absolute mass concentrations of primary emissions from both fossil and non-fossil sources during the heavily polluted events, their relative contribution to TC was even decreased, whereas the portion of SOC was consistently increased at all sites. This observation indicates that SOC was an important fraction in the increment of carbonaceous aerosols during the haze episode in China.

Abstract. Numerous definitions and analytical techniques for elemental (or black) carbon (EC) have been published in the scientific literature, but still no generally accepted interdisciplinary definition exists. EC is not a single chemical compound, but is mainly composed of two parts of carbon contents: combustion residues from pyrolysis and combustion emissions formed via gas-to-particle conversion. Accordingly EC is subdivided into two classes: char and soot. Char is defined as carbonaceous materials obtained by heating organic substances and formed directly from pyrolysis, or as an impure form of graphitic carbon obtained as a residue when carbonaceous material is partially burned or heated with limited access of air. Soot is defined as only those carbon particles that form at high temperature via gasphase processes. Since the different classes of EC have different chemical and physical properties, their optical lightabsorbing properties differ, so that it is essential to differentiate them in the environment. The thermal optical reflectance (TOR) method was used to differentiate between char-EC and soot-EC according to its stepwise thermal evolutional oxidation of different carbon fractions under different temperatures and atmosphere. Char-EC and soot-EC are operationally defined as EC1-OP and EC2+EC3 (EC1, EC2 and EC3 corresponding to carbon fractions evolved at 550, 700 and 800 • C in a 98% He/2% O 2 atmosphere, respectively), respectively. One year of observations of the daily and seasonal variations of carbonaceous particles were conducted in Xi'an, China in 2004 to demonstrate the different characteristics of char and soot in the atmosphere. Total carbon (TC), organic carbon (OC), EC and char-EC showed Correspondence to: Y. M. Han (yongming@ieecas.cn) similar seasonal trends, with high concentrations in winter and low concentrations in summer, while soot-EC revealed relatively small seasonal variations, with maximum concentration (1.85±0.72 µg m −3 ) in spring and minimum concentration (1.15±0.47 µg m −3 ) in summer. The strong correlation between EC and char-EC (R 2 = 0.99) and poor correlation between EC and soot-EC (R 2 = 0.31) indicate that previously reported total EC in the literature reflected the distribution characteristics of char only, while overlooking that of soot. However, soot exhibits stronger light-absorbing characteristics than char, and merits greater focus in climate research. The small seasonal variation of soot-EC indicates that soot may be the background fraction in total EC, and is likely to have an even longer lifetime in the atmosphere than previously estimated for total EC, which suggests that soot may has a greater contribution to global warming. While both char-EC/soot-EC and primary OC/EC ratios vary with emission sources, only OC/EC ratio is affected by SOA. Thus char-EC/soot-EC may be a more effective indicator than OC/EC in source identification of carbonaceous aerosol. Comparison of seasonal variations of OC/EC and char-EC/soot-EC ratios in Xi'an confirms this point. ...

at Lulang, a high-altitude (>3300m above sea level) site on the southeast Tibetan Plateau (TP); objectives were to determine chemical characteristics of the aerosol and identify its major sources. We report aerosol (total suspended particulate, TSP) mass levels and the concentrations of selected elements, carbonaceous species, and water-soluble inorganic ions. Significant buildup of aerosol mass and chemical species (organic carbon, element carbon, nitrate, and sulfate) occurred during the premonsoon, while lower concentrations were observed during the monsoon. Seasonal variations in aerosol and chemical species were driven by precipitation scavenging and atmospheric circulation. Two kinds of high-aerosol episodes were observed: one was enriched with dust indicators (Fe and Ca , and Fe. The TSP loadings during the latter were 3 to 6 times those on normal days. The greatest aerosol optical depths (National Centers for Environmental Protection/National Center for Atmospheric Research reanalysis) occurred upwind, in eastern India and Bangladesh, and trajectory analysis indicates that air pollutants were transported from the southwest. Northwesterly winds brought high levels of natural emissions (Fe, Ca 2+ ) and low levels of pollutants (SO 4 2À , NO 3 À , K + , and EC); this was consistent with high aerosol optical depths over the western deserts and Gobi. Our work provides evidence that both geological and pollution aerosols from surrounding regions impact the aerosol population of the TP.