Abstract. We used an airborne Fourier transform infrared spectrometer (AFTIR), coupled to a flow-through, air-sampling cell, on a King Air B-90 to make in situ trace gas measurements in isolated smoke plumes from four, large, boreal zone wildfires in interior Alaska during June 1997. AFTIR spectra acquired near the source of the smoke plumes yielded excess mixing ratios for 13 of the most common trace gases: water, carbon dioxide, AFTIR spectra collected in downwind smoke that had aged 2.2 + 1 hours in the upper, early plume y?elded AO3/ACO ratios of 7.9 + 2.4% resulting from 03 production rates of -50 ppbv h-. The ANH3/ACO ratio in another plume decreased to 1/e of its initial value in --2.5 hours. A set of average emission ratios and emission factors for fires in Alaskan boreal forests is derived. We estimate that the 1997 Alaskan fires emitted 46 i 11 Tg of CO2.

Abstract. Biomass burning is an important source of many trace gases in the global troposphere. We have constructed an airborne trace gas measurement system consisting of a Fourier transform infrared spectrometer (F'FIR) coupled to a "flow-through" multipass cell (AFrlR) and installed it on a U.S. Department of Agriculture Forest Service King Air B-90. The first measurements with the new system were conducted in North Carolina during April 1997 on large, isolated biomass fire plumes. Simultaneous measurements included Global Positioning System (GPS); airborne sonde; particle light scattering, CO, and CO2; and integrated filter and canister samples. AFrlR spectra acquired within a few kilometers of the fires yielded excess mixing ratios for 10 of the most common trace gases in the smoke: water, carbon dioxide, carbon monoxide, methane, formaldehyde, acetic acid, formic acid, methanol, ethylene, and ammonia. Emission ratios to carbon monoxide for formaldehyde, acetic acid, and methanol were each 2.5 _+ 1%. This is in excellent agreement with (and confirms the relevance of) our results from laboratory fires. However, these ratios are significantly higher than the emission ratios reported for these compounds in some previous studies of "fresh" smoke. We present a simple photochemical model calculation that suggests that oxygenated organic compounds should be included in the assessment of ozone formation in smoke plumes. Our measured emission factors indicate that biomass fires could account for a significant portion of the oxygenated organic compounds and HOx present in the tropical troposphere during the dry season. Our fire measurements, along with recent measurements of oxygenated biogenic emissions and oxygenated organic compounds in the free troposphere, indicate that these rarely measured compounds play a major, but poorly understood, role in the HOx, NOx, and 03 chemistry of the troposphere.

[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 EF RSC 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 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.

Abstract. The trace gas emissions from six biomass fires, including three grass fires, were measured using a Fourier transform infrared (FTIR) spectrometer coupled to an open-path, multipass cell (OP-FTIR). The quantified emissions consisted of carbon dioxide, nitric oxide, water vapor, carbon monoxide, methane, ammonia, ethylene, acetylene, isobutene, methanol, acetic acid, formic acid, formaldehyde, and hydroxyacetaldehyde. By including grass fires in this study we have now measured smoke composition from fires in each major vegetation class. The emission ratios of the oxygenated compounds, formaldehyde, methanol, and acetic acid, were 1-2% of CO in the grass fires, similar to our other laboratory and field measurements but significantly higher than in some other studies. These oxygenated compounds are important, as they affect O.• and HOx chemistry in both biomass fire plumes and the free troposphere. The OP-FTIR data and the simultaneously collected canister data indicated that the dominant C4 emission was isobutene (C4H8) and not 1-butene. The rate constant for the reaction of isobutene with the OH radical is 60% larger than that of 1-butene. We estimate that 67 + 9% of the fuel nitrogen was volatilized with the major nitrogen emissions, ammonia, and nitric oxide, accounting for 22 + 8%.