Publications (7)7.58 Total impact
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Article: Measured and modeled humidification factors of fresh smoke particles from biomass burning: role of inorganic constituents
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ABSTRACT: During the 2006 FLAME study (Fire Laboratory at Missoula Experiment), laboratory burns of biomass fuels were performed to investigate the physico-chemical, optical, and hygroscopic properties of fresh biomass smoke. As part of the experiment, two nephelometers simultaneously measured dry and humidified light scattering coefficients (bsp(dry) and bsp(RH), respectively) in order to explore the role of relative humidity (RH) on the optical properties of biomass smoke aerosols. Results from burns of several biomass fuels showed large variability in the humidification factor (f(RH)=bsp(RH)/bsp(dry)). Values of f(RH) at RH=85–90% ranged from 1.02 to 2.15 depending on fuel type. We incorporated measured chemical composition and size distribution data to model the smoke hygroscopic growth to investigate the role of inorganic and organic compounds on water uptake for these aerosols. By assuming only inorganic constituents were hygroscopic, we were able to model the water uptake within experimental uncertainty, suggesting that inorganic species were responsible for most of the hygroscopic growth. In addition, humidification factors at 85–90% RH increased for smoke with increasing inorganic salt to carbon ratios. Particle morphology as observed from scanning electron microscopy revealed that samples of hygroscopic particles contained soot chains either internally or externally mixed with inorganic potassium salts, while samples of weak to non-hygroscopic particles were dominated by soot and organic constituents. This study provides further understanding of the compounds responsible for water uptake by young biomass smoke, and is important for accurately assessing the role of smoke in climate change studies and visibility regulatory efforts.Atmospheric Chemistry and Physics Discussions. 01/2010; -
Article: Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer
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ABSTRACT: Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used were Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients revealed a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: (1) shielding of inner monomers after particle consolidation or collapse with water uptake; (2) the lower case contribution of mass transfer through evaporation and condensation at high relative humidity (RH) to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.Atmospheric Chemistry and Physics. 01/2009; -
Article: Optical measurements of aerosol size distributions in Great Smoky Mountains National Park: dry aerosol characterization.
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ABSTRACT: Aerosol size distributions were measured during the summertime 1995 Southeastern Aerosol and Visibility Study (SEAVS) in Great Smoky Mountains National Park using an Active Scattering Aerosol Spectrometer (ASASP-X) optical particle counter. We present an overview of the experimental method, our data inversion technique, timelines of the size distribution parameters, and calculations of dry accumulation mode aerosol density and refractive index. Aerosol size distributions were recorded during daylight hours for aerosol in the size range 0.1 < Dp < 2.5 microns. The particle refractive index used for the data inversion was calculated with the partial molar refractive index approach using 12-hr measured aerosol chemical composition. Aerosol accumulation mode volume concentrations ranging from 1 to 26 micron 3 cm-3 were observed, with an average of 7 +/- 5 micron 3 cm-3. The study average dry accumulation mode geometric volume median diameter was 0.27 +/- 0.03 micron, and the mean geometric standard deviation was 1.45 +/- 0.06. Using an internally mixed aerosol model, and assuming chemical homogeneity across the measured particle distribution, an average accumulation mode dry sulfate ion mass scattering efficiency of 3.8 +/- 0.6 m2 g-1 was calculated.Journal of the Air & Waste Management Association (1995) 06/2000; 50(5):665-76. · 1.52 Impact Factor -
Article: Light scattering characteristics of aerosols at ambient and as a function of relative humidity: Part II--A comparison of measured scattering and aerosol concentrations using statistical models.
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ABSTRACT: The eastern United States national parks experience some of the worst visibility conditions in the nation. To study these conditions, the Southeastern Aerosol and Visibility Study (SEAVS) was undertaken to characterize the size-dependent composition, thermodynamic properties, and optical characteristics of the ambient atmospheric particles. It is a cooperative three-year study that is sponsored by the National Park Service and the Electric Power Research Institute and its member utilities. The field portion of the study was carried out from July 15 to August 25, 1995. The study design, instrumental configuration, and estimation of aerosol types from particle measurements is presented in a companion paper. In the companion paper, we compare measurements of scattering at ambient conditions and as functions of relative humidity to theoretical predictions of scattering. In this paper, we make similar comparisons, but using statistical techniques. Statistically derived specific scattering associated with sulfates suggest that a reasonable estimate of sulfate scattering can be arrived at by assuming nominal dry specific scattering and treating the aerosols as an external mixture with ammoniation of sulfate accounted for and by the use of Tang's growth curves to predict water absorption. However, the regressions suggest that the sulfate scattering may be underestimated by about 10%. Regression coefficients on organics, to within the statistical uncertainty of the model, suggest that a reasonable estimate of organic scattering is about 4.0 m2/g. A new analysis technique is presented, which does not rely on comparing measured to model estimates of scattering to evoke an understanding of ambient aerosol growth properties, but rather relies on measurements of scattering as a function of relative humidity to develop actual estimates of f(RH) curves. The estimates of the study average f(RH) curve for sulfates compares favorably with the theoretical f(RH) curve for ammonium bisulfate, which is in turn consistent with the study average sulfate ammoniation corresponding to a molar ratio of NH4/SO4 of approximately one. The f(RH) curve for organics is not significantly different from one, suggesting that organics are weakly to nonhygroscopic.Journal of the Air & Waste Management Association (1995) 06/2000; 50(5):701-9. · 1.52 Impact Factor -
Article: Light scattering characteristics of aerosols as a function of relative humidity: Part I--A comparison of measured scattering and aerosol concentrations using the theoretical models.
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ABSTRACT: The Southeastern Aerosol and Visibility Study (SEAVS) was undertaken to characterize the size-dependent composition, thermodynamic properties, and optical characteristics of the ambient atmospheric particles in the southeastern United States. The field portion of the study was carried out from July 15 to August 25, 1995. As part of the study a relative humidity controlled inlet was built to raise or lower the relative humidity to predetermined levels before the aerosol was passed into an integrating nephelometer or particle-sizing device. Five other integrating nephelometers were operated in various configurations, two of which were fitted with a 2.5 microns inlet. Fine particle (< 2.5 microns) samplers were operated to measure concentrations of sulfate, nitrate, and ammonium ions, organic and elemental carbon, and fine soil. Mass size distributions were measured with an eight-stage, single orifice cascade impactor. Four different strategies for estimating scattering were used. First, an externally mixed model with constant specific scattering coefficients, sulfate ion mass interpreted as ammonium bisulfate, and ammonium bisulfate growth as a function of relative humidity, is assumed. Second, an externally mixed aerosol model, assuming constant dry specific scattering but with sulfate ammoniation and associated composition-dependent hygroscopicity explicitly accounted for, is used. Third, an externally mixed aerosol model, but with sulfate ammoniation, associated growth as a function of relative humidity, and sulfate size distributions, is applied. Fourth, an internally mixed aerosol model with measured sulfur size distributions and estimated size distributions for other species is used with the growth characteristics of the mixture being estimated using the Zdanovskii-Stokes-Robinson (ZSR) assumptions. Only ionic species were considered to be hygroscopic. The second, third, and fourth approaches yield similar results with reconstructed scattering comparing quite favorably with measured scattering. Accounting for sulfate ammoniation and associated water uptake was the most important detail in achieving closure between measurements and modeled scattering. In general, differences between estimated scattering, assuming internally or externally mixed models, was small. These same models were used to estimate wet to dry scattering ratios. The R2 for an ordinary least-squares regression between measured and predicted ratios was high (0.71-0.92), and in most cases the scattering ratio was insensitive to modeling assumptions. However, during some sample periods differences between predicted scattering ratios for the different modeling assumptions were as high as 30%.Journal of the Air & Waste Management Association (1995) 06/2000; 50(5):686-700. · 1.52 Impact Factor -
Article: Aerosol light scattering measurements as a function of relative humidity.
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ABSTRACT: The hygroscopic nature of atmospheric fine aerosol was investigated at a rural site in the Great Smoky Mountains National Park during July and August 1995. Passing the sample aerosol through an inlet, which housed an array of Perma Pure diffusion dryers, controlled the sample aerosol's relative humidity (RH). After conditioning the aerosol sample in the inlet, the light scattering coefficient and the aerosol size distribution were simultaneously measured. During this study, the conditioned aerosol's humidity ranged between 5% < RH < 95%. Aerosol response curves were produced using the ratio bspw/bspd; where bspw is the scattering coefficient measured at some RH greater than 20% and bspd is the scattering coefficient of the "dry" aerosol. For this work, any sample RH values below 15% were considered dry. Results of this investigation showed that the light scattering ratio increased continuously and smoothly over the entire range of relative humidity. The magnitude of the ratio at a particular RH value, however, varied considerably in time, particularly for RH values greater than approximately 60%. Curves of the scattering coefficient ratios as a function of RH were generated for each day and compared to the average 12-hour chemical composition of the aerosol. This comparison showed that for any particular RH value the ratio was highest during time periods of high sulfate concentrations and lowest during time periods of high soil or high organic carbon concentrations.Journal of the Air & Waste Management Association (1995) 06/2000; 50(5):710-6. · 1.52 Impact Factor -
Article: Estimates of particle hygroscopicity during the Southeastern Aerosol and Visibility Study.
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ABSTRACT: Aerosol water content was determined from relative humidity controlled optical particle counter (ASASP-X) size distribution measurements made during the Southeastern Aerosol and Visibility Study (SEAVS) in the Great Smoky Mountains National Park during summer 1995. Since the scattering response function of the ASASP-X is sensitive to particle refractive index, a technique for calibrating the ASASP-X for any real refractive index was developed. A new iterative process was employed to calculate water mass concentration and wet refractive index as functions of relative humidity. Experimental water mass concentrations were compared to theoretically predicted values assuming only ammonium sulfate compounds were hygroscopic. These comparisons agreed within experimental uncertainty. Estimates of particle hygroscopicity using a rural aerosol model of refractive index as a function of relative humidity demonstrated no significant differences from those made with daily varying refractive index estimates. Although aerosol size parameters were affected by the assumed chemical composition, forming ratios of these parameters nearly canceled these effects.Journal of the Air & Waste Management Association (1995) 06/2000; 50(5):677-85. · 1.52 Impact Factor
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2000–2009
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Colorado State University
- Department of Atmospheric Science
Fort Collins, CO, USA
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