Showing papers by "Robert J. Yokelson published in 2003"
TL;DR: In this article, trace gas and particle emissions were measured from 47 laboratory fires burning 16 regionally to globally significant fuel types, including coal, rice straw, methanol, and acetic acid.
Abstract: Trace gas and particle emissions were measured from 47 laboratory fires burning 16 regionally to globally significant fuel types. Instrumentation included the following: open-path Fourier transform infrared spectroscopy; proton transfer reaction mass spectrometry; filter sampling with subsequent analysis of particles with diameter <2.5 μm for organic and elemental carbon and other elements; and canister sampling with subsequent analysis by gas chromatography (GC)/flame ionization detector, GC/electron capture detector, and GC/mass spectrometry. The emissions of 26 compounds are reported by fuel type. The results include the first detailed measurements of the emissions from Indonesian fuels. Carbon dioxide, CO, CH 4 , NH 3 , HCN, methanol, and acetic acid were the seven most abundant emissions (in order) from burning Indonesian peat. Acetol (hydroxyacetone) was a major, previously unobserved emission from burning rice straw (21-34 g/kg). The emission factors for our simulated African fires are consistent with field data for African fires for compounds measured in both the laboratory and the field. However, the higher concentrations and more extensive instrumentation in this work allowed quantification of at least 10 species not previously quantified for African field fires (in order of abundance): acetaldehyde, phenol, acetol, glycolaldehyde, methylvinylether, furan, acetone, acetonitrile, propenenitrile, and propanenitrile. Most of these new compounds are oxygenated organic compounds, which further reinforces the importance of these reactive compounds as initial emissions from global biomass burning. A few high-combustion-efficiency fires emitted very high levels of elemental (black) carbon, suggesting that biomass burning may produce more elemental carbon than previously estimated.
404 citations
TL;DR: In this paper, a 1000-ha savanna fire in South Africa was investigated, and the results showed that the CO-normalized concentrations of particles 1.5 micron diameter increased with smoke age.
Abstract: Airborne measurements of particles and gases fiom 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 approximately 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 approximately 1.7 x l0(exp 7) molecules /cubic centimeter. Excess CN, normalized by excess CO, decreased rapidly during the first approximately 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 micron 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.
220 citations
Journal Article•
TL;DR: In this article, a 1000-ha savanna fire in South Africa was investigated, and the results showed that the CO-normalized concentrations of particles 1.5 μm diameter increased with smoke age.
Abstract: 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 x 10 7 molecules cm -3 . 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 μm 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.
194 citations
TL;DR: This paper measured stable and reactive trace gases with an airborne Fourier transform infrared spectrometer (AFTIR) on the University of Washington Convair-580 research aircraft in August/September 2000 during the SAFARI 2000 dry season campaign in Southern Africa.
Abstract: We measured stable and reactive trace gases with an airborne Fourier transform infrared spectrometer (AFTIR) on the University of Washington Convair-580 research aircraft in August/September 2000 during the SAFARI 2000 dry season campaign in Southern Africa. The measurements included vertical profiles of C02, CO, H20, and CH4 up to 5.5 km on six occasions above instrumented ground sites and below the TERRA satellite and ER-2 high-flying research aircraft. We also measured the trace gas emissions from 10 African savanna fires. Five of these fires featured extensive ground-based fuel characterization, and two were in the humid savanna ecosystem that accounts for most African biomass burning. The major constituents we detected in nascent CH3OOH, HCHO, CH30H, HCN, NH3, HCOOH, and C2H2. These are the first quantitative measurements of the initial emissions of oxygenated volatile organic compounds (OVOC), NH3, and HCN from African savanna fires. On average, we measured 5.3 g/kg of OVOC and 3.6 g/kg of hydrocarbons (including CH4) in the initial emissions from the fires. Thus, the OVOC will have profound, largely unexplored effects on tropical tropospheric chemistry. The HCN emission factor was only weakly dependent on fire type; the average value (0.53 g/kg) is about 20 times that of a previous recommendation. HCN may be useful as a tracer for savanna fires. Delta O3/Delta CO and Delta CH3COO/Delta CO increased to as much as 9% in <1 h of photochemical processing downwind of fires. Direct measurements showed that cloud processing of smoke greatly reduced CH30H, NH3, CH3COOH, SO2, and NO2 levels, but significantly increased HCHO and NO.
183 citations
TL;DR: Bertschi et al. as discussed by the authors adopted a working definition of residual smoldering combustion (RSC) as biomass combustion that produces emissions that are not lofted by strong fire-induced convection.
Abstract: [1] We adopt a working definition of residual smoldering combustion (RSC) as biomass combustion that produces emissions that are not lofted by strong fire-induced convection. RSC emissions can be produced for up to several weeks after the passage of a flame front and they are mostly unaffected by flames. Fuels prone to RSC include downed logs, duff, and organic soils. Limited observations in the tropics and the boreal forest suggest that RSC is a globally significant source of emissions to the troposphere. This source was previously uncharacterized. We measured the first emission factors (EF) for RSC in a series of laboratory fires and in a wooded savanna in Zambia, Africa. We report EFRSC for both particles with diameter <2.5 mm (PM2.5) and the major trace gases as measured by open-path Fourier transform infrared (OP-FTIR) spectroscopy. The major trace gases include carbon dioxide, carbon monoxide, methane, ethane, ethene, acetylene, propene, formaldehyde, methanol, acetic acid, formic acid, glycolaldehyde, phenol, furan, ammonia, and hydrogen cyanide. We show that a model used to predict trace gas EF for fires in a wide variety of aboveground fine fuels fails to predict EF for RSC. For many compounds, our EF for RSC-prone fuels from the boreal forest and wooded savanna are very different from the EF for the same compounds measured in fire convection columns above these ecosystems. We couple our newly measured EFRSC with estimates of fuel consumption by RSC to refine emission estimates for fires in the boreal forest and wooded savanna. We find some large changes in estimates of biomass fire emissions with the inclusion of RSC. For instance, the wooded savanna methane EF increases by a factor of 2.5 even when RSC accounts for only 10% of fuel consumption. This shows that many more measurements of fuel consumption and EF for RSC are needed to improve estimates of biomass burning emissions. INDEX TERMS: 0345 Atmospheric Composition and Structure: Pollution—urban and regional (0305); 0368 Atmospheric Composition and Structure: Troposphere—constituent transport and chemistry; 0394 Atmospheric Composition and Structure: Instruments and techniques; 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; KEYWORDS: biomass burning, smoldering combustion, oxygenated organic compounds, ammonia, methanol, smoke Citation: Bertschi, I., R. J. Yokelson, D. E. Ward, R. E. Babbitt, R. A. Susott, J. G. Goode, and W. M. Hao, Trace gas and particle emissions from fires in large diameter and belowground biomass fuels, J. Geophys. Res., 108(D13), 8472, doi:10.1029/2002JD002100, 2003.
171 citations
Journal Article•
TL;DR: In this article, the authors adopt a working definition of residual smoldering combustion (RSC) as biomass combustion that produces emissions that are not lofted by strong fire-induced convection.
Abstract: We adopt a working definition of residual smoldering combustion (RSC) as biomass combustion that produces emissions that are not lofted by strong fire-induced convection. RSC emissions can be produced for up to several weeks after the passage of a flame front and they are mostly unaffected by flames. Fuels prone to RSC include downed logs, duff, and organic soils. Limited observations in the tropics and the boreal forest suggest that RSC is a globally significant source of emissions to the troposphere. This source was previously uncharacterized. We measured the first emission factors (EF) for RSC in a series of laboratory fires and in a wooded savanna in Zambia, Africa. We report EF RSC for both particles with diameter <2.5 μm (PM2.5) and the major trace gases as measured by open-path Fourier transform infrared (OP-FTIR) spectroscopy. The major trace gases include carbon dioxide, carbon monoxide, methane, ethane, ethene, acetylene, propene, formaldehyde, methanol, acetic acid, formic acid, glycolaldehyde, phenol, furan, ammonia, and hydrogen cyanide. We show that a model used to predict trace gas EF for fires in a wide variety of aboveground fine fuels fails to predict EF for RSC. For many compounds, our EF for RSC-prone fuels from the boreal forest and wooded savanna are very different from the EF for the same compounds measured in fire convection columns above these ecosystems. We couple our newly measured EF RSC with estimates of fuel consumption by RSC to refine emission estimates for fires in the boreal forest and wooded savanna. We find some large changes in estimates of biomass fire emissions with the inclusion of RSC. For instance, the wooded savanna methane EF increases by a factor of 2.5 even when RSC accounts for only 10% of fuel consumption. This shows that many more measurements of fuel consumption and EF for RSC are needed to improve estimates of biomass burning emissions.
166 citations
TL;DR: In this paper, the authors measured the emissions of 50 gaseous and particulate species from 10 savanna fires in southern Africa, including carbon dioxide, carbon monoxide, sulfur dioxide, nitrogen oxides, methane, ammonia, dimethyl sulfide, methyl nitrate, five hydrocarbons, and particles with diameters from 0.1 to 3 microns.
Abstract: Airborne measurements made on initial smoke from 10 savanna fires in southern Africa provide quantitative data on emissions of 50 gaseous and particulate species, including carbon dioxide, carbon monoxide, sulfur dioxide, nitrogen oxides, methane, ammonia, dimethyl sulfide, nonmethane organic compounds, halocarbons, gaseous organic acids, aerosol ionic components, carbonaceous aerosols, and condensation nuclei (CN). Measurements of several of the gaseous species by gas chromatography and Fourier transform infrared spectroscopy are compared. Emission ratios and emission factors are given for eight species that have not been reported previously for biomass burning of savanna in southern Africa (namely, dimethyl sulfide, methyl nitrate, five hydrocarbons, and particles with diameters from 0.1 to 3 microns). The emission factor that we measured for ammonia is lower by a factor of 4, and the emission factors for formaldehyde, hydrogen cyanide, and CN are greater by factors of about 3, 20, and 3 - 15, respectively, than previously reported values. The new emission factors are used to estimate annual emissions of these species from savanna fires in Africa and worldwide.
165 citations
Journal Article•
TL;DR: In this article, the authors measured the emissions of 50 gaseous and particulate species from 10 savanna fires in southern Africa, including carbon dioxide, carbon monoxide, sulfur dioxide, nitrogen oxides, methane, ammonia, dimethyl sulfide, methyl nitrate, five hydrocarbons, and particles with diameters from 0. 1 to 3 μm.
Abstract: Airborne measurements made on initial smoke from 10 savanna fires in southern Africa provide quantitative data on emissions of 50 gaseous and particulate species, including carbon dioxide, carbon monoxide, sulfur dioxide, nitrogen oxides, methane, ammonia, dimethyl sulfide, nonmethane organic compounds, halocarbons, gaseous organic acids, aerosol ionic components, carbonaceous aerosols, and condensation nuclei (CN). Measurements of several of the gaseous species by gas chromatography and Fourier transform infrared spectroscopy are compared. Emission ratios and emission factors are given for eight species that have not been reported previously for biomass burning of savanna in southern Africa (namely, dimethyl sulfide, methyl nitrate, five hydrocarbons, and particles with diameters from 0. 1 to 3 μm). The emission factor that we measured for ammonia is lower by a factor of 4, and the emission factors for formaldehyde, hydrogen cyanide, and CN are greater by factors of about 3, 20, and 3-15, respectively, than previously reported values. The new emission factors are used to estimate annual emissions of these species from savanna fires in Africa and worldwide.
142 citations
TL;DR: In this article, measurements were made of the emissions of particles and gases from two diesel-powered ships in the southern Atlantic Ocean off the coast of Namibia, and the measurements were used to derive emission factors from ships of three species not reported previously, namely, black carbon, accumulation-mode particles, and cloud condensation nuclei (CCN), as well as for carbon dioxide, carbon monoxide (CO), methane (CH4), non-methane hydrocarbons, sulfur dioxide (SO2), nitrogen oxides (NOx).
134 citations
TL;DR: In this paper, the authors used open-path Fourier transform infrared (OP-FTIR) spectroscopy to quantify 18 of the most abundant trace gases emitted by wood and charcoal cooking fires and an earthen charcoal-making kiln in Zambia.
Abstract: [1] Domestic biomass fuels (biofuels) were recently estimated to be the second largest source of carbon emissions from global biomass burning. Wood and charcoal provide approximately 90% and 10% of domestic energy in tropical Africa. In September 2000, we used open-path Fourier transform infrared (OP-FTIR) spectroscopy to quantify 18 of the most abundant trace gases emitted by wood and charcoal cooking fires and an earthen charcoal-making kiln in Zambia. These are the first in situ measurements of an extensive suite of trace gases emitted by tropical biofuel burning. We report emission ratios (ER) and emission factors (EF) for (in order of abundance) carbon dioxide (CO2), carbon monoxide (CO), methane (CH4), acetic acid (CH3COOH), methanol (CH3OH), formaldehyde (HCHO), ethene (C2H4), ammonia (NH3), acetylene (C2H2), nitric oxide (NO), ethane (C2H6), phenol (C6H5OH), propene (C3H6), formic acid (HCOOH), nitrogen dioxide (NO2), hydroxyacetaldehyde (HOCH2CHO), and furan (C4H4O). Compared to previous work, our emissions of organic acids and NH3 are 3–6.5 times larger. Another significant finding is that reactive oxygenated organic compounds account for 70–80% of the total nonmethane organic compounds (NMOC). For most compounds, the combined emissions from charcoal production and charcoal burning are larger than the emissions from wood fires by factors of 3–10 per unit mass of fuel burned and ∼2 per unit energy released. We estimate that Zambian savanna fires produce more annual CO2, HCOOH, and NOx than Zambian biofuel use by factors of 2.5, 1.7, and 5, respectively. However, biofuels contribute larger annual emissions of CH4, CH3OH, C2H2, CH3COOH, HCHO, and NH3 by factors of 5.1, 3.9, 2.7, 2.4, 2.2, and 2.0, respectively. Annual CO and C2H4 emissions are approximately equal from both sources. Coupling our data with recent estimates of global biofuel consumption implies that global biomass burning emissions for several compounds are significantly larger than previously reported. Biofuel emissions are produced year-round, disperse differently than savanna fire emissions, and could strongly impact the tropical troposphere.
77 citations
Journal Article•
TL;DR: In this paper, the first in situ measurements of an extensive suite of trace gases emitted by tropical biofuel burning were reported. But the results were limited to the most abundant trace gases, such as carbon dioxide and carbon monoxide.
Abstract: Domestic biomass fuels (biofuels) were recently estimated to be the second largest source of carbon emissions from global biomass burning. Wood and charcoal provide approximately 90% and 10% of domestic energy in tropical Africa. In September 2000, we used open-path Fourier transform infrared (OP-FTIR) spectroscopy to quantify 18 of the most abundant trace gases emitted by wood and charcoal cooking fires and an earthen charcoal-making kiln in Zambia. These are the first in situ measurements of an extensive suite of trace gases emitted by tropical biofuel burning. We report emission ratios (ER) and emission factors (EF) for (in order of abundance) carbon dioxide (CO 2 ), carbon monoxide (CO), methane (CH 4 ), acetic acid (CH 3 COOH), methanol (CH 3 OH), formaldehyde (HCHO), ethene (C 2 H 4 ), ammonia (NH 3 ), acetylene (C 2 H 2 ), nitric oxide (NO), ethane (C 2 H 6 ), phenol (C 6 H 5 OH), propene (C 3 H 6 ), formic acid (HCOOH), nitrogen dioxide (NO 2 ), hydroxyacetaldehyde (HOCH 2 CHO), and furan (C 4 H 4 O). Compared to previous work, our emissions of organic acids and NH 3 are 3-6.5 times larger. Another significant finding is that reactive oxygenated organic compounds account for 70-80% of the total nonmethane organic compounds (NMOC). For most compounds, the combined emissions from charcoal production and charcoal burning are larger than the emissions from wood fires by factors of 3 - 10 per unit mass of fuel burned and ∼2 per unit energy released. We estimate that Zambian savanna fires produce more annual CO 2 , HCOOH, and NO x than Zambian biofuel use by factors of 2.5, 1.7, and 5, respectively. However, biofuels contribute larger annual emissions of CH 4 , CH 3 OH, C 2 H 2 , CH 3 COOH, HCHO, and NH 3 by factors of 5.1, 3.9, 2.7, 2.4, 2.2, and 2.0, respectively. Annual CO and C 2 H 4 emissions are approximately equal from both sources. Coupling our data with recent estimates of global biofuel consumption implies that global biomass burning emissions for several compounds are significantly larger than previously reported. Biofuel emissions are produced year-round, disperse differently than savanna fire emissions, and could strongly impact the tropical troposphere.
TL;DR: In this article, the authors examined how adsorption and desorption of gases from inlets and a cell could affect the accuracy of closed-cell FTIR measurements of carbon dioxide (CO2), carbon monoxide (CO), methane (CH4), nitric oxide (NO), nitrogen dioxide (NO2), methanol (CH3OH), acetic acid (CH 3COOH), and ammonia (NH3).
Abstract: [1] We examined how adsorption and desorption of gases from inlets and a cell could affect the accuracy of closed-cell FTIR measurements of carbon dioxide (CO2), carbon monoxide (CO), methane (CH4), nitric oxide (NO), nitrogen dioxide (NO2), methanol (CH3OH), acetic acid (CH3COOH), and ammonia (NH3). When standards were delivered to the cell through a stainless steel inlet, temporarily reduced transmission was observed for CH3OH and NH3. However, a halocarbon wax coated inlet (normally used on the system) had excellent transmission (comparable to room temperature Teflon) for both CH3OH and NH3, even at temperatures as low as 5°C. Thus the wax is valuable for coating sampling system components that cannot be fashioned from Teflon. The instrument had a delayed response (∼10–40 s) for NH3 only, which was attributed to passivation of the Pyrex multipass cell. To determine sampling artifacts that could arise from the complex sample matrix presented by smoke, the closed-cell FTIR system was intercompared with an open-path FTIR system (which is immune to sampling artifacts) in well-mixed smoke. A similar cell passivation delay for NH3 was the only artifact found in this test. Overall, the results suggest that ∼10 s is sufficient to detect >80% of an NH3/CO ratio sampled by our fast-flow, closed-cell system. Longer sampling times or consecutive samples return better results. In field campaigns the closed-cell system sampling times were normally 10 to >100 s so NH3 was probably underestimated by 5–15%.
TL;DR: In this paper, the first early dry season (early June-early August) emission factor measurements for carbon dioxide (CO2), carbon monoxide (CO), methane (Ca), nonmethane hydrocarbons (NMHC), and particulates with a diameter less than 2.5 microns (pM2.5) for southern African grassland and woodland fires were presented.
Abstract: In this paper we present the first early dry season (early June-early August) emission factor measurements for carbon dioxide (CO2), carbon monoxide (CO), methane (Ca), nonmethane hydrocarbons (NMHC), and particulates with a diameter less than 2.5 microns (pM2.5) for southern African grassland and woodland fires. Seasonal emission factors for grassland fires correlate linearly with the proportion of green grass, used as a surrogate for the fuel moisture content, and are higher for products of incomplete combustion in the early part of the dry season compared with later in the dry season. Models of emission factors for NMHC and PM(sub 2.5) versus modified combustion efficiency (MCE) are statistically different in grassland compared with woodland ecosystems. We compare predictions based on the integration of emissions factors from this study, from the southern African Fire-Atmosphere Research Initiative 1992 (SAFARI-92), and from SAFARI-2000 with those based on the smaller set of ecosystem-specific emission factors to estimate the effects of using regional-average rather than ecosystem-specific emission factors. We also test the validity of using the SAFARI-92 models for emission factors versus MCE to predict the early dry season emission factors measured in this study. The comparison indicates that the largest discrepancies occur at the low end (0.907) and high end (0.972) of MCE values measured in this study. Finally, we combine our models of MCE versus proportion of green grass for grassland fires with emission factors versus MCE for selected oxygenated volatile organic compounds measured in the SAFARI-2000 campaign to derive the first seasonal emission factors for these compounds. The results of this study demonstrate that seasonal variations in savanna fire emissions are important and should be considered in modeling emissions at regional to continental scales.
TL;DR: In this paper, the authors presented the vertical profiles in the lower troposphere of temperature, relative humidity, sulfur dioxide (SO2), ozone (O3), condensation nuclei (CN), and carbon monoxide (CO), and horizontal distributions of twenty gaseous and particulate species, for five regions of southern Africa during the dry biomass burning season of 2000.
Abstract: Vertical profiles in the lower troposphere of temperature, relative humidity, sulfur dioxide (SO2), ozone (O3), condensation nuclei (CN), and carbon monoxide (CO), and horizontal distributions of twenty gaseous and particulate species, are presented for five regions of southern Africa during the dry biomass burning season of 2000. The regions are the semiarid savannas of northeast South Africa and northern Botswana, the savanna-forest mosaic of coastal Mozambique, the humid savanna of southern Zambia, and the desert of western Namibia. The highest average concentrations of carbon dioxide (CO2), CO, methane (CH4), O3, black particulate carbon, and total particulate carbon were in the Botswana and Zambia sectors (388 and 392 ppmv, 369 and 453 ppbv, 1753 and 1758 ppbv, 79 and 88 ppbv, 2.6 and 5.5 micrograms /cubic meter and 13.2 and 14.3 micrograms/cubic meter). This was due to intense biomass burning in Zambia and surrounding regions. The South Africa sector had the highest average concentrations of SO2, sulfate particles, and CN (5.1 ppbv, 8.3 micrograms/cubic meter, and per 6400 cubic meter , respectively), which derived from biomass burning and electric generation plants and mining operations within this sector. Air quality in the Mozambique sector was similar to the neighboring South Africa sector. Over the arid Namibia sector there were polluted layers aloft, in which average SO2, O3, and CO mixing ratios (1.2 ppbv, 76 ppbv, and 3 10 ppbv, respectively) were similar to those measured over the other more polluted sectors. This was due to transport of biomass smoke from regions of widespread savanna burning in southern Angola. Average concentrations over all sectors of CO2 (386 +/- 8 ppmv), CO (261 +/- 81 ppbv), SO2 (2.5 +/- 1.6 ppbv), O3 (64 +/- 13 ppbv), black particulate carbon (2.3 +/- 1.9 microgram/cubic meter), organic particulate carbon (6.2 +/- 5.2 microgram/cubic meter), total particle mass (26.0 +/- 4.7 microgram/cubic meter), and potassium particles (0.4 +- 0.1 microgram/cubic meter) were comparable to those in polluted, urban air. Since the majority of the measurements in this study were obtained in locations well removed from industrial sources of pollution, the high average concentrations of pollutants reflect the effects of widespread biomass burning. On occasions, relatively thin (-0.5 km) layers of remarkably clean air were located at -3 km above mean sea level, sandwiched between heavily polluted air. The data presented here can be used for inputs to and validation of regional and global atmospheric chemical models.
TL;DR: In this paper, the authors presented the results of a flight on the NASA ER-2 on 7 September 2000 as part of the Southern African Regional Science Initiative (SAFARI 2000) dry season field campaign, where they retrieved tropospheric carbon monoxide (CO) column densities for more than 9000 spectra obtained by the UWis Scanning High-Resolution Interferometer Sounder (SHIS).
Abstract: Retrieved tropospheric carbon monoxide (CO) column densities are presented for more than 9000 spectra obtained by the University of Wisconsin-Madison (UWis) Scanning High-Resolution Interferometer Sounder (SHIS) during a flight on the NASA ER-2 on 7 September 2000 as part of the Southern African Regional Science Initiative (SAFARI 2000) dry season field campaign. Enhancements in tropospheric column CO were detected in the vicinity of a controlled biomass burn in the Timbavati Game Reserve in northeastern South Africa and over the edge of the river of smoke in south central Mozambique. Relatively clean air was observed over the far southern coast of Mozambique. Quantitative comparisons are presented with in situ measurements from five different instruments flying on two other aircraft: the University of Washington Convair-580 (CV) and the South African Aerocommander JRB in the vicinity of the Timbavati fire. Measured tropospheric CO columns (extrapolated from 337 to 100 mb) of 2.1 x 10(exp 18) per square centimeter in background air and up to 1.5 x 10(exp 19) per square centimeter in the smoke plume agree well with SHIS retrieved tropospheric CO columns of (2.3 plus or minus 0.25) x 10(exp 18) per square centimeter over background air near the fire and (1.5 plus or minus 0.35) x 10(exp 19) per square centimeter over the smoke plume. Qualitative comparisons are presented with three other in situ CO profiles obtained by the South African JRA aircraft over Mozambique and northern South Africa showing the influence of the river of smoke.
Journal Article•
TL;DR: This article measured stable and reactive trace gases with an airborne Fourier transform infrared spectrometer (AFTIR) on the University of Washington Convair-580 research aircraft in August/September 2000 during the SAFARI 2000 dry season campaign in Southern Africa.
Abstract: We measured stable and reactive trace gases with an airborne Fourier transform infrared spectrometer (AFTIR) on the University of Washington Convair-580 research aircraft in August/September 2000 during the SAFARI 2000 dry season campaign in Southern Africa. The measurements included vertical profiles of CO 2 , CO, H 2 O, and CH 4 up to 5.5 km on six occasions above instrumented ground sites and below the TERRA satellite and ER-2 high-flying research aircraft. We also measured the trace gas emissions from 10 African savanna fires. Five of these fires featured extensive ground-based fuel characterization, and two were in the humid savanna ecosystem that accounts for most African biomass burning. The major constituents that we detected in nascent smoke were (in order of excess molar abundance) H 2 O, CO 2 , CO, CH 4 , NO 2 , NO, C 2 H 4 , CH 3 COOH, HCHO, CH 3 OH, HCN, NH 3 , HCOOH, and C 2 H 2 . These are the first quantitative measurements of the initial emissions of oxygenated volatile organic compounds (OVOC), NH 3 , and HCN from African savanna fires. On average, we measured 5.3 g/kg of OVOC and 3.6 g/kg of hydrocarbons (including CH 4 ) in the initial emissions from the fires. Thus, the OVOC will have profound, largely unexplored effects on tropical tropospheric chemistry. The HCN emission factor was only weakly dependent on fire type; the average value (0.53 g/kg) is about 20 times that of a previous recommendation. HCN may be useful as a tracer for savanna fires. ΔO 3 /ΔCO and ΔCH 3 COOH/ΔCO increased to as much as 9% in <1 h of photochemical processing downwind of fires. Direct measurements showed that cloud processing of smoke greatly reduced CH 3 OH, NH 3 , CH 3 COOH, SO 2 , and NO 2 levels, but significantly increased HCHO and NO.