[1] The wavelength dependence of light absorption by aerosols collected on filters is investigated throughout the near-ultraviolet to near-infrared spectral region. Measurements were made using an optical transmission method. Aerosols produced by biomass combustion, including wood and savanna burning, and by motor vehicles, including diesel trucks, are included in the analysis. These aerosol types were distinguished by different wavelength (l) dependences in light absorption. Light absorption by the motor vehicle aerosols exhibited relatively weak wavelength dependence; absorption varied approximately as l À1 , indicating that black carbon (BC) was the dominant absorbing aerosol component. By contrast, the biomass smoke aerosols had much stronger wavelength dependence, approximately l À2 . The stronger spectral dependence was the result of enhanced light absorption at wavelengths shorter than 600 nm and was largely reduced when much of the sample organic carbon (OC) was extracted by dissolution in acetone. This indicates that OC in addition to BC in the biomass smoke aerosols contributed significantly to measured light absorption in the ultraviolet and visible spectral regions and that OC in biomass burning aerosols may appreciably absorb solar radiation. Estimated absorption efficiencies and imaginary refractive indices are presented for the OC extracted from biomass burning samples and the BC in motor vehicle-dominated aerosol samples. The uncertainty of these constants is discussed. Overall, results of this investigation show that low-temperature, incomplete combustion processes, including biomass burning, can produce light-absorbing aerosols that exhibit much stronger spectral dependence than high-temperature combustion processes, such as diesel combustion.
[1] We characterized the gas-and speciated aerosol-phase emissions from the open combustion of 33 different plant species during a series of 255 controlled laboratory burns during the Fire Laboratory at Missoula Experiments (FLAME). The plant species we tested were chosen to improve the existing database for U.S. domestic fuels: laboratory-based emission factors have not previously been reported for many commonly burned species that are frequently consumed by fires near populated regions and protected scenic areas. The plants we tested included the chaparral species chamise, manzanita, and ceanothus, and species common to the southeastern United States (common reed, hickory, kudzu, needlegrass rush, rhododendron, cord grass, sawgrass, titi, and wax myrtle). Fire-integrated emission factors for gas-phase CO 2 , CO, CH 4 , C 2 -4 hydrocarbons, NH 3 , SO 2 , NO, NO 2 , HNO 3 , and particle-phase organic carbon (OC), elemental carbon (EC), SO 4 2À , NO 3 À , Cl À , Na + , K + , and NH 4 + generally varied with both fuel type and with the fire-integrated modified combustion efficiency (MCE), a measure of the relative importance of flaming-and smoldering-phase combustion to the total emissions during the burn. Chaparral fuels tended to emit less particulate OC per unit mass of dry fuel than did other fuel types, whereas southeastern species had some of the largest observed emission factors for total fine particulate matter. Our measurements spanned a larger range of MCE than prior studies, and thus help to improve estimates of the variation of emissions with combustion conditions for individual fuels.
Air pollution affects billions of people worldwide, yet ambient pollution measurements are limited for much of the world. Urban air pollution concentrations vary sharply over short distances (≪1 km) owing to unevenly distributed emission sources, dilution, and physicochemical transformations. Accordingly, even where present, conventional fixed-site pollution monitoring methods lack the spatial resolution needed to characterize heterogeneous human exposures and localized pollution hotspots. Here, we demonstrate a measurement approach to reveal urban air pollution patterns at 4-5 orders of magnitude greater spatial precision than possible with current central-site ambient monitoring. We equipped Google Street View vehicles with a fast-response pollution measurement platform and repeatedly sampled every street in a 30-km area of Oakland, CA, developing the largest urban air quality data set of its type. Resulting maps of annual daytime NO, NO, and black carbon at 30 m-scale reveal stable, persistent pollution patterns with surprisingly sharp small-scale variability attributable to local sources, up to 5-8× within individual city blocks. Since local variation in air quality profoundly impacts public health and environmental equity, our results have important implications for how air pollution is measured and managed. If validated elsewhere, this readily scalable measurement approach could address major air quality data gaps worldwide.
[1] Airborne measurements of particles and gases from a 1000-ha savanna fire in South Africa are presented. These measurements represent the most extensive data set reported on the aging of biomass smoke. The measurements include total concentrations of particles (CN), particle sizes, particulate organic carbon and black carbon, light-scattering coefficients, downwelling UV fluxes, and mixing ratios for 42 trace gases and 7 particulate species. The ratios of excess nitrate, ozone, and gaseous acetic acid to excess CO increased significantly as the smoke aged over $40-45 min, indicating that these species were formed by photochemistry in the plume. For 17 other species, the excess mixing ratio normalized by the excess mixing ratio of CO decreased significantly with smoke age. The relative rates of decrease for a number of chemical species imply that the average OH concentration in the plume was $1.7 Â 10 7 molecules cm À3 . Excess CN, normalized by excess CO, decreased rapidly during the first $5 min of aging, probably due to coagulation, and then increased, probably due to gas-to-particle conversion. The CO-normalized concentrations of particles <1.5 mm in diameter decreased, and particles >1.5 mm diameter increased, with smoke age. The spectral depletion of solar radiation by the smoke is depicted. The downwelling UV flux near the vertical center of the plume was about two-thirds of that near the top of the plume.
[1] During the SAFARI 2000 field campaign, both smoke aerosols from savanna fires and haze aerosols in the boundary layer and in the free troposphere were collected from an aircraft in southern Africa. These aerosol samples were analyzed for their water-soluble chemical components, particularly the organic species. A novel technique, electrospray ionization-ion trap mass spectrometry, was used concurrently with an ion chromatography system to analyze for carbohydrate species. Seven carbohydrates, seven organic acids, five metallic elements, and three inorganic anions were identified and quantified. On the average, these 22 species comprised 36% and 27% of the total aerosol mass in haze and smoke aerosols, respectively. For the smoke aerosols, levoglucosan was the most abundant carbohydrate species, while gluconic acid was tentatively identified as the most abundant organic acid. The mass abundance and possible source of each class of identified species are discussed, along with their possible formation pathways. The combustion phase of a fire had an impact on the chemical composition of the emitted aerosols. Secondary formation of sulfate, nitrate, levoglucosan, and several organic acids occurred during the initial aging of smoke aerosols. It is likely that under certain conditions, some carbohydrate species in smoke aerosols, such as levoglucosan, were converted to organic acids during upward transport.
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