Significance We illustrate the similarity and difference in particulate matter (PM) formation between Beijing and other world regions. The periodic cycle of PM events in Beijing is regulated by meteorological conditions. While the particle chemical compositions in Beijing are similar to those commonly measured worldwide, efficient nucleation and growth over an extended period in Beijing are distinctive from the aerosol formation typically observed in other global areas. Gaseous emissions of volatile organic compounds and nitrogen oxides from urban transportation and sulfur dioxide from regional industry are responsible for large secondary PM formation, while primary emissions and regional transport of PM are insignificant. Reductions in emissions of the aerosol precursor gases from transportation and industry are essential to mediate severe haze pollution in China.
Sulfate aerosols exert profound impacts on human and ecosystem health, weather, and climate, but their formation mechanism remains uncertain. Atmospheric models consistently underpredict sulfate levels under diverse environmental conditions. From atmospheric measurements in two Chinese megacities and complementary laboratory experiments, we show that the aqueous oxidation of SO 2 by NO 2 is key to efficient sulfate formation but is only feasible under two atmospheric conditions: on fine aerosols with high relative humidity and NH 3 neutralization or under cloud conditions. Under polluted environments, this SO 2 oxidation process leads to large sulfate production rates and promotes formation of nitrate and organic matter on aqueous particles, exacerbating severe haze development. Effective haze mitigation is achievable by intervening in the sulfate formation process with enforced NH 3 and NO 2 control measures. In addition to explaining the polluted episodes currently occurring in China and during the 1952 London Fog, this sulfate production mechanism is widespread, and our results suggest a way to tackle this growing problem in China and much of the developing world.sulfate aerosol | severe haze | pollution | human health | climate
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Project Description and Overview: Objectives: Determining the overall impact of atmospheric aerosols on radiative balance requires knowledge of the relative amounts of scattering and absorbing aerosols, their distributions, and their chemical and optical properties. This proposal was a continuation of measurements of aerosol scattering and absorption begun in Mexico City in 2003 in collaboration with MCMA 2003 and continuing in the Atmospheric Science Program field study, Megacity Aerosol Experiment-Mexico City, (MAX-Mex) during March of 2006 aimed at determining the variability of aerosol optical properties. A suite of instrumentation was deployed in MAX-Mex at site TO, located in the northern part of the Mexico City Metropolitan Area, (MCMA), for the characterization of the aerosol optical properties in the field. Measurements were made of the following aerosol properties: (1) aerosol absorption as a function of wavelength, measured at two minute intervals with a 7-wavelength Aethalometer (2) aerosol scattering as a function of wavelength, measured at one minute intervals with a 3-wavelength nephelometer; 3) aerosol scattering as a function of relative humidity (RH), measured at one minute intervals with 2 single-wavelength nephelometers operated under dry (10% RH) and wet (80% RH) conditions; and 4) collection of size-fractionated aerosol samples on quartz fiber filters at 12 hour intervals (day/night) for further laboratory characterization. Aerosol filter samples were also collected at site Tl (located north of MCMA) for comparison with those collected in the city center. Preliminary results from in situ measurements have indicated an enhanced UV absorption in the afternoon over that expected from black carbon (BC) aerosols alone. These results are directly applicable to both modeling of aerosol radiative forcing and satellite optical depth retrieval algorithms. Both of these applications assume that the aerosol absorption is due only to BC with a wavelength dependence of A, " whereas results obtained in MAX-Mex show that the aerosol wavelength exponent varies over Mexico City from-0.7 to-1.5. All of the data collected in the field from the measurement sets 1-3 have been made available to the ASP community via the MILAGRO data site housed at NCAR. The laboratory characterization of aerosol samples collected in the ASP MAX-Mex field study compared results from Mexico City to samples collected at other sites, including Chicago, Little Rock, and Mt. Bachelor, OR. The project focused on obtaining complete spectral characterization of aerosols-especially their absorption characteristics as they relate to basic chemical functional groups. Particular attention was given to organics and from biogenic derived organic compounds. This included determinations of the UV-Visible-NIR characteristics of the aerosol absorption as reported as Angstrom Absorption Exponents. Correlation of these results with IR band observations of carboxylic acid, and carboxylate groups were conducted, along with past correlations with carbon...
The atmospheric effects of soot aerosols include interference with radiative transfer, visibility impairment, and alteration of cloud formation and are highly sensitive to the manner by which soot is internally mixed with other aerosol constituents. We present experimental studies to show that soot particles acquire a large mass fraction of sulfuric acid during atmospheric aging, considerably altering their properties. Soot particles exposed to subsaturated sulfuric acid vapor exhibit a marked change in morphology, characterized by a decreased mobility-based diameter but an increased fractal dimension and effective density. These particles experience large hygroscopic size and mass growth at subsaturated conditions (<90% relative humidity) and act efficiently as cloud-condensation nuclei. Coating with sulfuric acid and subsequent hygroscopic growth enhance the optical properties of soot aerosols, increasing scattering by Ϸ10-fold and absorption by nearly 2-fold at 80% relative humidity relative to fresh particles. In addition, condensation of sulfuric acid is shown to occur at a similar rate on ambient aerosols of various types of a given mobility size, regardless of their chemical compositions and microphysical structures. Representing an important mechanism of atmospheric aging, internal mixing of soot with sulfuric acid has profound implications on visibility, human health, and direct and indirect climate forcing.climate ͉ clouds ͉ radiative properties ͉ human health ͉ anthropogenic pollution S oot aerosols produced from fossil-fuel combustion, automobile and aircraft emissions, and biomass burning are ubiquitous in the atmosphere, comprising Ϸ10-50% of the total tropospheric particulate matter (1-6). Once emitted into the atmosphere, soot particles are subjected to several aging processes, including adsorption or condensation of gaseous species (7-9), coagulation with other preexisting aerosols, and oxidation (10-12). Model calculations have shown that, when associated with other nonabsorbing aerosol constituents (e.g., sulfate), soot seems more absorptive and exerts a higher positive direct radiative forcing, and the warming effect by soot nearly balances the net cooling effect of other anthropogenic aerosols (5, 13). Also, on the basis of mesoscale model simulations, absorption of solar radiation by internally mixed soot aerosols causes warming in the middle atmosphere and reduction in cloudiness over the tropics (4). The mixing state and associated physical, optical, and geometrical properties of soot particles are of critical importance in evaluating the effects of light-absorbing aerosols and improving climate predictions by using global climate models (GCMs). Current knowledge on such an issue is very limited for developing an accurate representation of soot particles in GCMs, leading to underestimation of climatic forcing (14).Hygroscopic aerosols also act as cloud-condensation nuclei (CCN) that impact cloud formation and the lifetime and albedo of clouds (4, 6). Freshly generated soot particles exist...
Atmospheric aerosols often contain a substantial fraction of organic matter, but the role of organic compounds in new nanometer-sized particle formation is highly uncertain. Laboratory experiments show that nucleation of sulfuric acid is considerably enhanced in the presence of aromatic acids. Theoretical calculations identify the formation of an unusually stable aromatic acid-sulfuric acid complex, which likely leads to a reduced nucleation barrier. The results imply that the interaction between organic and sulfuric acids promotes efficient formation of organic and sulfate aerosols in the polluted atmosphere because of emissions from burning of fossil fuels, which strongly affect human health and global climate.
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