S. K. Akagi

Bio: S. K. Akagi is an academic researcher from University of Montana. The author has contributed to research in topics: Aerosol & Particulates. The author has an hindex of 15, co-authored 23 publications receiving 3615 citations.

Emission factors for open and domestic biomass burning for use in atmospheric models

Abstract: . Biomass burning (BB) is the second largest source of trace gases and the largest source of primary fine carbonaceous particles in the global troposphere. Many recent BB studies have provided new emission factor (EF) measurements. This is especially true for non-methane organic compounds (NMOC), which influence secondary organic aerosol (SOA) and ozone formation. New EF should improve regional to global BB emissions estimates and therefore, the input for atmospheric models. In this work we present an up-to-date, comprehensive tabulation of EF for known pyrogenic species based on measurements made in smoke that has cooled to ambient temperature, but not yet undergone significant photochemical processing. All EFs are converted to one standard form (g compound emitted per kg dry biomass burned) using the carbon mass balance method and they are categorized into 14 fuel or vegetation types. Biomass burning terminology is defined to promote consistency. We compile a large number of measurements of biomass consumption per unit area for important fire types and summarize several recent estimates of global biomass consumption by the major types of biomass burning. Post emission processes are discussed to provide a context for the emission factor concept within overall atmospheric chemistry and also highlight the potential for rapid changes relative to the scale of some models or remote sensing products. Recent work shows that individual biomass fires emit significantly more gas-phase NMOC than previously thought and that including additional NMOC can improve photochemical model performance. A detailed global estimate suggests that BB emits at least 400 Tg yr−1 of gas-phase NMOC, which is almost 3 times larger than most previous estimates. Selected recent results (e.g. measurements of HONO and the BB tracers HCN and CH3CN) are highlighted and key areas requiring future research are briefly discussed.

The Fire INventory from NCAR (FINN): a high resolution global model to estimate the emissions from open burning

Abstract: . The Fire INventory from NCAR version 1.0 (FINNv1) provides daily, 1 km resolution, global estimates of the trace gas and particle emissions from open burning of biomass, which includes wildfire, agricultural fires, and prescribed burning and does not include biofuel use and trash burning. Emission factors used in the calculations have been updated with recent data, particularly for the non-methane organic compounds (NMOC). The resulting global annual NMOC emission estimates are as much as a factor of 5 greater than some prior estimates. Chemical speciation profiles, necessary to allocate the total NMOC emission estimates to lumped species for use by chemical transport models, are provided for three widely used chemical mechanisms: SAPRC99, GEOS-CHEM, and MOZART-4. Using these profiles, FINNv1 also provides global estimates of key organic compounds, including formaldehyde and methanol. Uncertainties in the emissions estimates arise from several of the method steps. The use of fire hot spots, assumed area burned, land cover maps, biomass consumption estimates, and emission factors all introduce error into the model estimates. The uncertainty in the FINNv1 emission estimates are about a factor of two; but, the global estimates agree reasonably well with other global inventories of biomass burning emissions for CO, CO2, and other species with less variable emission factors. FINNv1 emission estimates have been developed specifically for modeling atmospheric chemistry and air quality in a consistent framework at scales from local to global. The product is unique because of the high temporal and spatial resolution, global coverage, and the number of species estimated. FINNv1 can be used for both hindcast and forecast or near-real time model applications and the results are being critically evaluated with models and observations whenever possible.

Evolution of trace gases and particles emitted by a chaparral fire in California

Abstract: Biomass burning (BB) is a major global source of trace gases and particles. Accurately representing the pro- duction and evolution of these emissions is an important goal for atmospheric chemical transport models. We measured a suite of gases and aerosols emitted from an 81 hectare pre- scribed fire in chaparral fuels on the central coast of Cali- fornia, US on 17 November 2009. We also measured physi- cal and chemical changes that occurred in the isolated down- wind plume in the first 4 h after emission. The measure- ments were carried out onboard a Twin Otter aircraft outfit- ted with an airborne Fourier transform infrared spectrome- ter (AFTIR), aerosol mass spectrometer (AMS), single par- ticle soot photometer (SP2), nephelometer, LiCor CO2 an- alyzer, a chemiluminescence ozone instrument, and a wing- mounted meteorological probe. Our measurements included: CO2; CO; NOx; NH3; non-methane organic compounds; or- ganic aerosol (OA); inorganic aerosol (nitrate, ammonium, sulfate, and chloride); aerosol light scattering; refractory black carbon (rBC); and ambient temperature, relative hu- midity, barometric pressure, and three-dimensional wind ve- locity. The molar ratio of excess O3 to excess CO in the plume (1O3/1CO) increased from 5.13 (±1.13)◊ 10 3 to 10.2 (±2.16)◊ 10 2 in 4.5 h following smoke emis- sion. Excess acetic and formic acid (normalized to excess CO) increased by factors of 1.73± 0.43 and 7.34± 3.03 (re- spectively) over the same time since emission. Based on the rapid decay of C2H4 we infer an in-plume average OH concentration of 5.27 (±0.97)◊ 10 6 molec cm 3 , consistent with previous studies showing elevated OH concentrations in biomass burning plumes. Ammonium, nitrate, and sulfate all increased over the course of 4 h. The observed ammo- nium increase was a factor of 3.90± 2.93 in about 4 h, but accounted for just 36 % of the gaseous ammonia lost on a molar basis. Some of the gas phase NH3 loss may have been due to condensation on, or formation of, particles be- low the AMS detection range. NOx was converted to PAN and particle nitrate with PAN production being about two times greater than production of observable nitrate in the first 4 h following emission. The excess aerosol light scattering in the plume (normalized to excess CO2) increased by a fac- tor of 2.50± 0.74 over 4 h. The increase in light scattering was similar to that observed in an earlier study of a biomass burning plume in Mexico where significant secondary forma- tion of OA closely tracked the increase in scattering. In the California plume, however, 1OA/1CO2 decreased sharply for the first hour and then increased slowly with a net de- crease of 20 % over 4 h. The fraction of thickly coated rBC particles increased up to 85 % over the 4 h aging period. Decreasing OA accompanied by increased scattering/particle coating in initial aging may be due to a combination of par- ticle coagulation and evaporation processes. Recondensation of species initially evaporated from the particles may have contributed to the subsequent slow rise in OA. We compare our results to observations from other plume aging studies

Coupling field and laboratory measurements to estimate the emission factors of identified and unidentified trace gases for prescribed fires

Abstract: . An extensive program of experiments focused on biomass burning emissions began with a laboratory phase in which vegetative fuels commonly consumed in prescribed fires were collected in the southeastern and southwestern US and burned in a series of 71 fires at the US Forest Service Fire Sciences Laboratory in Missoula, Montana. The particulate matter (PM2.5) emissions were measured by gravimetric filter sampling with subsequent analysis for elemental carbon (EC), organic carbon (OC), and 38 elements. The trace gas emissions were measured by an open-path Fourier transform infrared (OP-FTIR) spectrometer, proton-transfer-reaction mass spectrometry (PTR-MS), proton-transfer ion-trap mass spectrometry (PIT-MS), negative-ion proton-transfer chemical-ionization mass spectrometry (NI-PT-CIMS), and gas chromatography with MS detection (GC-MS). 204 trace gas species (mostly non-methane organic compounds (NMOC)) were identified and quantified with the above instruments. Many of the 182 species quantified by the GC-MS have rarely, if ever, been measured in smoke before. An additional 153 significant peaks in the unit mass resolution mass spectra were quantified, but either could not be identified or most of the signal at that molecular mass was unaccounted for by identifiable species. In a second, "field" phase of this program, airborne and ground-based measurements were made of the emissions from prescribed fires that were mostly located in the same land management units where the fuels for the lab fires were collected. A broad variety, but smaller number of species (21 trace gas species and PM2.5) was measured on 14 fires in chaparral and oak savanna in the southwestern US, as well as pine forest understory in the southeastern US and Sierra Nevada mountains of California. The field measurements of emission factors (EF) are useful both for modeling and to examine the representativeness of our lab fire EF. The lab EF/field EF ratio for the pine understory fuels was not statistically different from one, on average. However, our lab EF for "smoldering compounds" emitted from the semiarid shrubland fuels should likely be increased by a factor of ~2.7 to better represent field fires. Based on the lab/field comparison, we present emission factors for 357 pyrogenic species (including unidentified species) for 4 broad fuel types: pine understory, semiarid shrublands, coniferous canopy, and organic soil. To our knowledge this is the most comprehensive measurement of biomass burning emissions to date and it should enable improved representation of smoke composition in atmospheric models. The results support a recent estimate of global NMOC emissions from biomass burning that is much higher than widely used estimates and they provide important insights into the nature of smoke. 31–72% of the mass of gas-phase NMOC species was attributed to species that we could not identify. These unidentified species are not represented in most models, but some provision should be made for the fact that they will react in the atmosphere. In addition, the total mass of gas-phase NMOC divided by the mass of co-emitted PM2.5 averaged about three (range ~2.0–8.7). About 35–64% of the NMOC were likely semivolatile or of intermediate volatility. Thus, the gas-phase NMOC represent a large reservoir of potential precursors for secondary formation of ozone and organic aerosol. For the single lab fire in organic soil about 28% of the emitted carbon was present as gas-phase NMOC and ~72% of the mass of these NMOC was unidentified, highlighting the need to learn more about the emissions from smoldering organic soils. The mass ratio of total NMOC to "NOx as NO" ranged from 11 to 267, indicating that NOx-limited O3 production would be common in evolving biomass burning plumes. The fuel consumption per unit area was 7.0 ± 2.3 Mg ha−1 and 7.7 ± 3.7 Mg ha−1 for pine-understory and semiarid shrubland prescribed fires, respectively.

Boreal forest fire emissions in fresh Canadian smoke plumes: C 1 -C 10 volatile organic compounds (VOCs), CO 2 , CO, NO 2 , NO, HCN and CH 3 CN

Abstract: . Boreal regions comprise about 17 % of the global land area, and they both affect and are influenced by climate change. To better understand boreal forest fire emissions and plume evolution, 947 whole air samples were collected aboard the NASA DC-8 research aircraft in summer 2008 as part of the ARCTAS-B field mission, and analyzed for 79 non-methane volatile organic compounds (NMVOCs) using gas chromatography. Together with simultaneous measurements of CO2, CO, CH4, CH2O, NO2, NO, HCN and CH3CN, these measurements represent the most comprehensive assessment of trace gas emissions from boreal forest fires to date. Based on 105 air samples collected in fresh Canadian smoke plumes, 57 of the 80 measured NMVOCs (including CH2O) were emitted from the fires, including 45 species that were quantified from boreal forest fires for the first time. After CO2, CO and CH4, the largest emission factors (EFs) for individual species were formaldehyde (2.1 ± 0.2 g kg−1), followed by methanol, NO2, HCN, ethene, α-pinene, β-pinene, ethane, benzene, propene, acetone and CH3CN. Globally, we estimate that boreal forest fires release 2.4 ± 0.6 Tg C yr−1 in the form of NMVOCs, with approximately 41 % of the carbon released as C1-C2 NMVOCs and 21 % as pinenes. These are the first reported field measurements of monoterpene emissions from boreal forest fires, and we speculate that the pinenes, which are relatively heavy molecules, were detected in the fire plumes as the result of distillation of stored terpenes as the vegetation is heated. Their inclusion in smoke chemistry models is expected to improve model predictions of secondary organic aerosol (SOA) formation. The fire-averaged EF of dichloromethane or CH2Cl2, (6.9 ± 8.6) × 10−4 g kg−1, was not significantly different from zero and supports recent findings that its global biomass burning source appears to have been overestimated. Similarly, we found no evidence for emissions of chloroform (CHCl3) or methyl chloroform (CH3CCl3) from boreal forest fires. The speciated hydrocarbon measurements presented here show the importance of carbon released by short-chain NMVOCs, the strong contribution of pinene emissions from boreal forest fires, and the wide range of compound classes in the most abundantly emitted NMVOCs, all of which can be used to improve biomass burning inventories in local/global models and reduce uncertainties in model estimates of trace gas emissions and their impact on the atmosphere.

Bounding the role of black carbon in the climate system: A scientific assessment

Abstract: Black carbon aerosol plays a unique and important role in Earth's climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. This assessment provides an evaluation of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice. These effects are calculated with climate models, but when possible, they are evaluated with both microphysical measurements and field observations. Predominant sources are combustion related, namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom-up inventory methods are 7500 Gg yr−1 in the year 2000 with an uncertainty range of 2000 to 29000. However, global atmospheric absorption attributable to black carbon is too low in many models and should be increased by a factor of almost 3. After this scaling, the best estimate for the industrial-era (1750 to 2005) direct radiative forcing of atmospheric black carbon is +0.71 W m−2 with 90% uncertainty bounds of (+0.08, +1.27) W m−2. Total direct forcing by all black carbon sources, without subtracting the preindustrial background, is estimated as +0.88 (+0.17, +1.48) W m−2. Direct radiative forcing alone does not capture important rapid adjustment mechanisms. A framework is described and used for quantifying climate forcings, including rapid adjustments. The best estimate of industrial-era climate forcing of black carbon through all forcing mechanisms, including clouds and cryosphere forcing, is +1.1 W m−2 with 90% uncertainty bounds of +0.17 to +2.1 W m−2. Thus, there is a very high probability that black carbon emissions, independent of co-emitted species, have a positive forcing and warm the climate. We estimate that black carbon, with a total climate forcing of +1.1 W m−2, is the second most important human emission in terms of its climate forcing in the present-day atmosphere; only carbon dioxide is estimated to have a greater forcing. Sources that emit black carbon also emit other short-lived species that may either cool or warm climate. Climate forcings from co-emitted species are estimated and used in the framework described herein. When the principal effects of short-lived co-emissions, including cooling agents such as sulfur dioxide, are included in net forcing, energy-related sources (fossil fuel and biofuel) have an industrial-era climate forcing of +0.22 (−0.50 to +1.08) W m−2 during the first year after emission. For a few of these sources, such as diesel engines and possibly residential biofuels, warming is strong enough that eliminating all short-lived emissions from these sources would reduce net climate forcing (i.e., produce cooling). When open burning emissions, which emit high levels of organic matter, are included in the total, the best estimate of net industrial-era climate forcing by all short-lived species from black-carbon-rich sources becomes slightly negative (−0.06 W m−2 with 90% uncertainty bounds of −1.45 to +1.29 W m−2). The uncertainties in net climate forcing from black-carbon-rich sources are substantial, largely due to lack of knowledge about cloud interactions with both black carbon and co-emitted organic carbon. In prioritizing potential black-carbon mitigation actions, non-science factors, such as technical feasibility, costs, policy design, and implementation feasibility play important roles. The major sources of black carbon are presently in different stages with regard to the feasibility for near-term mitigation. This assessment, by evaluating the large number and complexity of the associated physical and radiative processes in black-carbon climate forcing, sets a baseline from which to improve future climate forcing estimates.

Reducing food’s environmental impacts through producers and consumers

Abstract: Food’s environmental impacts are created by millions of diverse producers. To identify solutions that are effective under this heterogeneity, we consolidated data covering five environmental indicators; 38,700 farms; and 1600 processors, packaging types, and retailers. Impact can vary 50-fold among producers of the same product, creating substantial mitigation opportunities. However, mitigation is complicated by trade-offs, multiple ways for producers to achieve low impacts, and interactions throughout the supply chain. Producers have limits on how far they can reduce impacts. Most strikingly, impacts of the lowest-impact animal products typically exceed those of vegetable substitutes, providing new evidence for the importance of dietary change. Cumulatively, our findings support an approach where producers monitor their own impacts, flexibly meet environmental targets by choosing from multiple practices, and communicate their impacts to consumers.

The model of emissions of gases and aerosols from nature version 2.1 (MEGAN2.1): An extended and updated framework for modeling biogenic emissions

Abstract: . The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1) is a modeling framework for estimating fluxes of biogenic compounds between terrestrial ecosystems and the atmosphere using simple mechanistic algorithms to account for the major known processes controlling biogenic emissions. It is available as an offline code and has also been coupled into land surface and atmospheric chemistry models. MEGAN2.1 is an update from the previous versions including MEGAN2.0, which was described for isoprene emissions by Guenther et al. (2006) and MEGAN2.02, which was described for monoterpene and sesquiterpene emissions by Sakulyanontvittaya et al. (2008). Isoprene comprises about half of the total global biogenic volatile organic compound (BVOC) emission of 1 Pg (1000 Tg or 1015 g) estimated using MEGAN2.1. Methanol, ethanol, acetaldehyde, acetone, α-pinene, β-pinene, t-β-ocimene, limonene, ethene, and propene together contribute another 30% of the MEGAN2.1 estimated emission. An additional 20 compounds (mostly terpenoids) are associated with the MEGAN2.1 estimates of another 17% of the total emission with the remaining 3% distributed among >100 compounds. Emissions of 41 monoterpenes and 32 sesquiterpenes together comprise about 15% and 3%, respectively, of the estimated total global BVOC emission. Tropical trees cover about 18% of the global land surface and are estimated to be responsible for ~80% of terpenoid emissions and ~50% of other VOC emissions. Other trees cover about the same area but are estimated to contribute only about 10% of total emissions. The magnitude of the emissions estimated with MEGAN2.1 are within the range of estimates reported using other approaches and much of the differences between reported values can be attributed to land cover and meteorological driving variables. The offline version of MEGAN2.1 source code and driving variables is available from http://bai.acd.ucar.edu/MEGAN/ and the version integrated into the Community Land Model version 4 (CLM4) can be downloaded from http://www.cesm.ucar.edu/ .

The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions

Abstract: . The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1) is a modeling framework for estimating fluxes of biogenic compounds between terrestrial ecosystems and the atmosphere using simple mechanistic algorithms to account for the major known processes controlling biogenic emissions. It is available as an offline code and has also been coupled into land surface and atmospheric chemistry models. MEGAN2.1 is an update from the previous versions including MEGAN2.0, which was described for isoprene emissions by Guenther et al. (2006) and MEGAN2.02, which was described for monoterpene and sesquiterpene emissions by Sakulyanontvittaya et al. (2008). Isoprene comprises about half of the total global biogenic volatile organic compound (BVOC) emission of 1 Pg (1000 Tg or 1015 g) estimated using MEGAN2.1. Methanol, ethanol, acetaldehyde, acetone, α-pinene, β-pinene, t-β-ocimene, limonene, ethene, and propene together contribute another 30% of the MEGAN2.1 estimated emission. An additional 20 compounds (mostly terpenoids) are associated with the MEGAN2.1 estimates of another 17% of the total emission with the remaining 3% distributed among >100 compounds. Emissions of 41 monoterpenes and 32 sesquiterpenes together comprise about 15% and 3%, respectively, of the estimated total global BVOC emission. Tropical trees cover about 18% of the global land surface and are estimated to be responsible for ~80% of terpenoid emissions and ~50% of other VOC emissions. Other trees cover about the same area but are estimated to contribute only about 10% of total emissions. The magnitude of the emissions estimated with MEGAN2.1 are within the range of estimates reported using other approaches and much of the differences between reported values can be attributed to land cover and meteorological driving variables. The offline version of MEGAN2.1 source code and driving variables is available from http://bai.acd.ucar.edu/MEGAN/ and the version integrated into the Community Land Model version 4 (CLM4) can be downloaded from http://www.cesm.ucar.edu/ .

Carbon and Other Biogeochemical Cycles

Abstract: For base year 2010, anthropogenic activities created ~210 (190 to 230) TgN of reactive nitrogen Nr from N2. This human-caused creation of reactive nitrogen in 2010 is at least 2 times larger than the rate of natural terrestrial creation of ~58 TgN (50 to 100 TgN yr−1) (Table 6.9, Section 1a). Note that the estimate of natural terrestrial biological fixation (58 TgN yr−1) is lower than former estimates (100 TgN yr−1, Galloway et al., 2004), but the ranges overlap, 50 to 100 TgN yr−1 vs. 90 to 120 TgN yr−1, respectively). Of this created reactive nitrogen, NOx and NH3 emissions from anthropogenic sources are about fourfold greater than natural emissions (Table 6.9, Section 1b). A greater portion of the NH3 emissions is deposited to the continents rather than to the oceans, relative to the deposition of NOy, due to the longer atmospheric residence time of the latter. These deposition estimates are lower limits, as they do not include organic nitrogen species. New model and measurement information (Kanakidou et al., 2012) suggests that incomplete inclusion of emissions and atmospheric chemistry of reduced and oxidized organic nitrogen components in current models may lead to systematic underestimates of total global reactive nitrogen deposition by up to 35% (Table 6.9, Section 1c). Discharge of reactive nitrogen to the coastal oceans is ~45 TgN yr−1 (Table 6.9, Section 1d). Denitrification converts Nr back to atmospheric N2. The current estimate for the production of atmospheric N2 is 110 TgN yr−1 (Bouwman et al., 2013).