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At least 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Low diffusive methane emissions from the main channel of a large Amazonian run-of-the-river reservoir attributed to high methane oxidation

The global development of hydropower dams has rapidly expanded over the last several decades and has spread to historically non-impounded systems such as the Amazon River's main low land tributaries in Brazil. Despite the recognized significance of reservoirs to the global methane (CH4) emission, the processes controlling this emission remain poorly understood, especially in Tropical reservoirs. Here we evaluate CH4 dynamics in the main channel and downstream of the Santo Antônio hydroelectric reservoir, a large tropical run-of-the-river (ROR) reservoir in Amazonia. This study is intended to give a snapshot of the CH4 dynamics during the falling water season at the initial stage after the start of operations. Our results show substantial and higher CH4 production in reservoirs' littoral sediment than in the naturally flooded areas downstream of the dam. Despite the large production in the reservoir or naturally flooded areas, high CH4 oxidation in the main channel keep the concentration and fluxes of CH4 in the main channel low. Similar CH4 concentrations in the reservoir and downstream close to the dam suggest negligible degassing at the dam, but stable isotopic evidence indicates the presence of a less oxidized pool of CH4 after the dam. ROR reservoirs are designed to disturb the natural river flow dynamics less than traditional reservoirs. If enough mixing and oxygenation remain throughout the reservoir's water column, naturally high CH4 oxidation rates can also remain and limit the diffusive CH4 emissions from the main channel. Nevertheless, it is important to highlight that our results focused on emissions in the deep and oxygenated main channel. High emissions, mainly through ebullition, may occur in the vast and shallow areas represented by bays and tributaries. However, detailed assessments are still required to understand the impacts of this reservoir on the annual emissions of CH4.

Amazon, aquatic, biogeochemistry, carbon cycling, ↗
NASA NTRS1986

Atmospheric methane sources - Alaskan tundra bogs, an alpine fen, and a subarctic boreal marsh

Methane (CH4) flux measurements from Alaska tundra bogs, an alpine fen, and a subarctic boreal marsh were obtained at field sites ranging from Prudhoe Bay on the coast of the Arctic Ocean to the Alaskan Range south of Fairbanks during August 1984. In the tundra, average CH4 emission rates varied from 4.9 mg CH4 per sq m per day (moist tundra) to 119 mg CH4 per sq m per day (waterlogged tundra). Fluxes averaged 40 mg CH4 per sq m per day from wet tussock meadows in the Brooks Range and 289 mg Ch4 per sq m per day from an alpine fen in the Alaskan Range. The boreal marsh had an average CH4 emission rate of 106 mg CH4 per sq m per day. Significant emissions were detected in tundra areas where peat temperatures were as low as 4 C, and permafrost was only 25 cm below the ground surface. Emission rates from the 17 sites sampled were found to be logarithmically related to water levels at the sites. Extrapolation of the data to an estimate of the total annual CH4 emission from all arctic and boreal wetlands suggests that these ecosystems are a major source of atmospheric CH4 and could account for up to 23 percent of global CH4 emissions from wetlands.

Sebacher, D. I.↗
NASA NTRS2000

Methanogenesis, Mesospheric Clouds, and Global Habitability

Hyperthermophilic methanogens can exist in a deep hot biosphere up to 110 C, or 10 km deep. Methane (CH4) itself is thermodynamically stable to depths of 300 km. Geologic (microbial plus abiogenic thermal) methane is transported upward, attested to by its association with helium, to form petroleum pools. Near or at the surface, geologic CH4 mixes with other natural and with anthropogenic CH4 yielding annual emissions into the atmosphere of 500 Tg, of which 200 Tg are natural and 300 Tg are man-made. The atmospheric lifetime of CH4, a greenhouse gas 20 times more effective than CO2 in raising global temperatures, is approximately 10 years. It is removed from the atmosphere mainly by reactions with hydroxyl radical (OH) to form CO2, but also by dry soil and by conversion to H2O in the stratosphere and middle atmosphere. A sudden rise in atmospheric temperatures by 9-12 C some 55 million years ago has been explained by the release in a few thousand years of three trillion tons of CH4 out of 15 trillion tons that had formed beneath the sea floor. What prevented this CH4-induced greenhouse effect from running away? An analog to the CH4-burp of 55 million years ago is the CH4-doubling over the past century which resulted in a increase in upper level H2O from 4.3 ppmv to 6 ppmv. This 30% increase in H2O vapor yielded a tenfold increase in brightness of polar mesospheric clouds because of a strong dependence of the ice particle nucleation rate on the water saturation ratios. Models show that at a given temperature the optical depth of mesospheric clouds scales as [H2O]beta with beta varying between 4 and 8. Radiative transfer tools applied to mesospheric particles suggest that an optical depth of approximately one, or 1000 times the current mesospheric cloud optical depth, would result in tropospheric cooling of about 10 K. Assuming beta=6, a thousandfold increase in optical thickness would require a three-fold increase of H2O, or a 20-fold increase of CH4. At the current rate of anthropogenic emissions this is expected to occur within the next 1000 years. This timescale is also commensurate with what has been assumed for the CH4- burp 55 million years ago.

Pueschel, Rudolf F.↗
NASA NTRS2015

Investigation of Benthic Foraminiferal Non-Traditional Stable Isotopes to Reconstruct Methane Fluxes in Sedimentary Environments

Methane (CH4) is an important greenhouse gas, with a global warming potential much higher than carbon dioxide (CO2) on a short time scale. Even if the residence time of CH4 in the atmosphere is relatively short (tens of years), one of the products of CH4 oxidation is CO2, a greenhouse gas with a much longer residence time in the atmosphere (tens to hundreds of years). CH4 has been proposed as one of the trigger mechanisms for rapid global climate change today and in the geological past. With regards to the geological past, numerous studies proposed the benthic foraminiferal carbon isotope ratio (Delta13C) as a tool to reconstruct the impact of marine CH4 on rapid climate changes; however, the investigation of modern benthic foraminiferal Delta13C have produced inconclusive results. CH4 has a distinctive hydrogen isotope (Delta(D)) and Delta13C signature compared to seawater, and sulfate reduction, often coupled to CH4 anaerobic oxidation in sediments, changes the sulfur isotope signature (Delta34S) of the remaining sulfate in porewater. Therefore, we hypothesize that the Delta(D) and Delta34S signature of infaunal benthic foraminiferal species can provide a complementary approach to Delta13C to study CH4 dynamics in sedimentary environments. Here, we present the preliminary results obtained analyzing Uvigerina peregrina Delta(D) and Delta34S from three different locations at Hydrate Ridge, offshore Oregon. Unfortunately, the lack of chemical data related to the moment of foraminiferal calcification makes difficult to build a robust relationship among the U. peregrina stable isotopes and the CH4 fluxes at the sampling sites. However, our results look very promising, as each site is characterized by a different Delta(D) and Delta34S signature. We emphasize that this study represents the first step in the development of new proxies (Delta(D)) and Delta34S), which may complement the more traditional benthic foraminiferal Delta13C values, to reconstruct marine CH4 fluxes in the geological past.

Borrelli, C.↗
DOE OSTI2020

A synthesis of methane dynamics in thermokarst lake environments

Greenhouse gas emissions from physical permafrost thaw disturbance and subsidence, including the formation and expansion of thermokarst (thaw) lakes, may double the magnitude of the permafrost carbon feedback this century. These processes are not accounted for in current global climate models. Thermokarst lakes, in particular, have been shown to be hotspots for emissions of methane (CH4), a potent greenhouse gas with 32 times more global warming potential than carbon dioxide (CO2) over a 100-year timescale. Here, we synthesize several studies examining CH4 dynamics in a representative first-generation thermokarst lake (Vault Lake, informal name) to show that CH4 production and oxidation potentials vary with depth in thawed sediments beneath the lake. This variation leads to depth-dependent differences in both in situ dissolved CO2:CH4 ratios and net CH4 production responses to additional warming. Comparing CH4 production, oxidation, and flux values from studies at Vault Lake suggests up to 99% of produced CH4 is oxidized and/or periodically entrapped before entering the atmosphere. We summarize these findings in the context of CH4 literature from thermokarst lakes and identify future research directions for incorporating thermokarst lake CH4 dynamics into estimates of the permafrost carbon feedback.

58 GEOSCIENCES↗
NASA NTRS1994

Clouds, hazes, and the stratospheric methane abundance in Neptune

Analysis of high-spatial-resolution (approximately 0.8 arcsec) methane band and continuum imagery of Neptune's relatively homogeneous Equatorial Region yields significant constraints on (1) the stratospheric gaseous methane mixing ratio (f(sub CH4, S)), (2) the column abundances and optical properties of stratospheric and tropospheric hydrocarbon hazes, and (3) the wavelength-dependent single-scattering albedo of the 3-bar opaque cloud. From the center-to-limb behavior of the 7270-A and 8900-A CH4 bands, the stratospheric methane mixing ratios is limited to f(sub CH4, S) less than 1.7 x 10(exp -3), with a nominal value of f(sub CH4, S) = 3.5 x 10(exp -4), one to two orders of magnitude less than pre-Voyager estimates, but in agreement with a number of recent ultraviolet and thermal infrared measurements, and largely in agreement with the tropopause mixing ratio implied by Voyager temperature measurements. Upper limits to the stratospheric haze mass column abundance and 6190-A and 8900-A haze opacities are 0.61 micrograms/sq cm and 0.075 and 0.042, respectively, with nominal values of 0.20 micrograms/sq cm and 0.025 and 0.014 for the 0.2 micrometers radius particles preferred by the recent Voyager PPS analysis of Pryor et al. (1992). The tropospheric CH4 haze opacities are comparable to that found in the stratosphere, i.e., upper limits of 0.104 and 0.065 at 6190 A and 8900 A, respectively, with nominal values of 0.085 and 0.058. This indicates a column abundance less than 11.0 micrograms/sq cm, corresponding to the methane gas content within a well-mixed 3% methane tropospheric layer only 0.1 cm thick near the 1.5-bar CH4 condensation level. Conservative scattering is ruled out for the opaque cloud near 3 bars marking the bottom of the visible atmosphere. Specifically, we find cloud single-scattering albedos of 0.915 +/- 0.006 at 6340 A, 0.775 +/- 0.012 at 7490 A, and 0.803 +/- 0.010 at 8260 A. Global models utilizing a complete global spectrum confirm the red-absorbing character of the 3-bar cloud. The global-mean model has approximately 7.7 times greater stratospheric aerosol content than the Equatorial Region. An analysis of stratospheric haze precipitation rates indicates a steady-state haze production rate of 0.185-1.5 x 10(exp -14) g/sq cm/s, in agreement with recent theoretical photochemical estimates. Finally, reanalysis of the Voyager PPS 7500-A phase angle data utilizing the f(sub CH4, S) value derived here confirms the Pryor et al. result of a tropospheric CH4 haze opacity of a few tenths in the 22-30 degs S latitude region, several times that of the Equatorial Region or of the globe. The factor-of-10 reduction in f(sub CH4, S) below that assumed by Pryor et al. implies decreased gas absorption and consequently a decrease in the forward-scattering component of tropospheric aerosols.

Baines, Kevin H.↗
NASA NTRS2017

Global Wetland Contribution to 2000-2012 Atmospheric Methane Growth Rate Dynamics

Increasing atmospheric methane (CH4) concentrations have contributed to approximately 20% of anthropogenic climate change. Despite the importance of CH4 as a greenhouse gas, its atmospheric growth rate and dynamics over the past two decades, which include a stabilization period (1999-2006), followed by renewed growth starting in 2007, remain poorly understood. We provide an updated estimate of CH4 emissions from wetlands, the largest natural global CH4 source, for 2000-2012 using an ensemble of biogeochemical models constrained with remote sensing surface inundation and inventory-based wetland area data. Between 2000-2012, boreal wetland CH4 emissions increased by 1.2 Tg yr(sup -1) (-0.2-3.5 Tg yr(sup -1), tropical emissions decreased by 0.9 Tg yr(sup -1) (-3.2-1.1 Tg yr(sup -1), yet globally, emissions remained unchanged at 184 +/- 22 Tg yr(sup -1). Changing air temperature was responsible for increasing high-latitude emissions whereas declines in low-latitude wetland area decreased tropical emissions; both dynamics are consistent with features of predicted centennial-scale climate change impacts on wetland CH4 emissions. Despite uncertainties in wetland area mapping, our study shows that global wetland CH4 emissions have not contributed significantly to the period of renewed atmospheric CH4 growth, and is consistent with findings from studies that indicate some combination of increasing fossil fuel and agriculture-related CH4 emissions, and a decrease in the atmospheric oxidative sink.

Poulter, Benjamin↗
NASA NTRS2013

Analyzing Carbon Dioxide and Methane Emissions in California Using Airborne Measurements and Model Simulations

Greenhouse gas (GHG) concentrations have increased over the past decades and are linked to global temperature increases and climate change. These changes in climate have been suggested to have varying effects, and uncertain consequences, on agriculture, water supply, weather, sea-level rise, the economy, and energy. To counteract the trend of increasing atmospheric concentrations of GHGs, the state of California has passed the California Global Warming Act of 2006 (AB-32). This requires that by the year 2020, GHG (e.g., carbon dioxide (CO2) and methane (CH4)) emissions will be reduced to 1990 levels. To quantify GHG fluxes, emission inventories are routinely compiled for the State of California (e.g., CH4 emissions from the California Greenhouse Gas Emissions Measurement (CALGEM) Project). The major sources of CO2 and CH4 in the state of California are: transportation, electricity production, oil and gas extraction, cement plants, agriculture, landfills/waste, livestock, and wetlands. However, uncertainties remain in these emission inventories because many factors contributing to these processes are poorly quantified. To alleviate these uncertainties, a synergistic approach of applying air-borne measurements and chemical transport modeling (CTM) efforts to provide a method of quantifying local and regional GHG emissions will be performed during this study. Additionally, in order to further understand the temporal and spatial distributions of GHG fluxes in California and the impact these species have on regional climate, CTM simulations of daily variations and seasonality of total column CO2 and CH4 will be analyzed. To assess the magnitude and spatial variation of GHG emissions and to identify local “hot spots”, airborne measurements of CH4 and CO2 were made by the Alpha Jet Atmospheric eXperiment (AJAX) over the San Francisco Bay Area (SFBA) and San Joaquin Valley (SJV) in January and February 2013 during the Discover-AQ-CA study. High mixing ratios of GHGs were observed in-flight with a high degree of spatial variability. To provide an additional method to quantify GHG emissions, and analyze AJAX measurement data, the GEOS-Chem CTM is used to simulate SFBA/SJV GHG measurements. A nested-grid version of GEOS-Chem will be applied and utilizes varying emission inventories and model parameterizations to simulate GHG fluxes/emissions. The model considers CO2 fluxes from fossil fuel use, biomass/biofuel burning, terrestrial and oceanic biosphere exchanges, shipping and aviation, and production from the oxidation of carbon monoxide, CH4, and non-methane volatile organic carbons. The major sources of CH4 simulated in GEOS-Chem are domesticated animals, rice fields, natural gas leakage, natural gas venting/flaring (oil production), coal mining, wetlands, and biomass burning. Preliminary results from the comparison between available observations (e.g., AJAX and CALGEM CH4 emission maps) and GEOS-Chem results will be presented, along with a discussion of CO2 and CH4 source apportionment and the use of the GEOS-Chem-adjoint to perform inverse GHG modeling.

Johnson, Matthew S.↗
NASA NTRSDate not supplied

TPSAS-NF1676L-32105-DND

NASA Langley Research Center is developing the High-Altitude Lidar Observatory (HALO) system to address the observational needs of NASA’s weather, climate, carbon cycle, and atmospheric composition focus areas. HALO is a multi-function airborne lidar being developed to measure atmospheric H2O and CH4 mixing ratios and aerosol/cloud/ocean optical properties using the Differential Absorption Lidar (DIAL) and High Spectral Resolution Lidar (HSRL) techniques, respectively. To respond to a wide range of airborne process studies, HALO can be rapidly reconfigured to provide either CH4 DIAL+HSRL, H2O DIAL+HSRL, or CH4 DIAL+H2O DIAL measurements using three different laser transmitters. During spring 2018 NASA Langley demonstrated the world’s first combined airborne CH4 DIAL and HSRL measurements from the Langley King Air aircraft during four test flights. The HALO methane configuration also participated in the Long Island Sound Tropospheric Ozone Study (LISTOS) air quality field campaign on the NASA B200 aircraft. The flown instrument configuration employed the DIAL technique at 1645 nm for column and multi-layer range resolved measurements of CH4 concentrations, and the HSRL technique at 532 nm to make independent, unambiguous retrievals of aerosol extinction and backscatter. It also employed the standard backscatter technique at 1064 nm and is polarization-sensitive at the 1064/532 nm wavelengths. The addition of the HSRL channels provides context to the airborne CH4 DIAL measurements such as source attribution, transport, and vertical mixing through mixed layer height retrievals, as well as providing the critical capability to validate aerosol induced biases from passive space-borne measurements of column CH4. In this presentation we focus on the instrument capabilities, initial CH4 measurements over oil and gas production sites in coordination with the ACT-America campaign, CH4 signatures over the Long Island Sound domain during the LISTOS campaign, and prospects for future airborne campaigns with cohosted payloads consisting of active and passive sensors.

Rory Barton-Grimley↗
NASA NTRS2021

Anthropogenic Emissions are the Main Contribution to the Rise of Atmospheric Methane (1993-2017)

Atmospheric methane (CH4) concentrations have shown a puzzling resumption of growth since 2007 following a period of stabilization from 2000 to 2006. Multiple hypotheses have been proposed to explain the temporal variations in CH4 growth, which attributes the rise of atmospheric CH4 either to increases in emissions from fossil fuel activities, agriculture, and natural wetlands or to a decrease in the atmospheric chemical sink. Here, we use a comprehensive ensemble of CH4 source estimates and isotopic δ13C-CH4 source signature data to show that the resumption of CH4 growth is most likely due to increased anthropogenic emissions. Our emission scenarios that have the fewest biases with respect to isotopic composition suggest that the agriculture, landfill, and waste sectors were responsible for 53 ± 13% of the renewed growth over the period 2007–2017 compared to 2000–2006; industrial fossil fuel sources explained an additional 34 ± 24%, and wetland sources contributed the least at 13 ± 9%. The hypothesis that a large increase in emissions from natural wetlands drove the decrease in atmospheric δ13C-CH4 values cannot be reconciled with current process-based wetland CH4 models. This finding suggests the need for increased wetland measurements to better constrain the contemporary and future role of wetlands in the rise of atmospheric methane and climate feedbacks. Our findings highlight the predominant role of anthropogenic activities in driving the growth of atmospheric CH4 concentrations.

Zhen Zhang↗
NASA NTRSDate not supplied

Generating a 4D Global CH(4) Product by Assimilating TROPOMI column CH(4) in NASA’s GEOS GCM

Examination of temporal and spatial CH4 variability is crucial for better understanding the human and natural processes driving climate change and ultimately designing mitigation strategies. Here we present an analysis framework that uses NASA’s GEOS General Circulation Model (GCM) to construct a high-resolution, time varying picture of atmospheric CH4 consistent with measurements from a variety of platforms, both in situ and remotely sensed. The resulting time varying atmospheric CH4 product can (i) support interpretation of high-resolution point source detection approaches, (ii) provide reanalysis fields for CH4 and other greenhouse gases, and (iii) supply boundary conditions for regional models. Our approach starts with a set of CH4 emissions from various inventories that have been adjusted to match the global annual growth rate over recent decades. These emissions are transported by the GEOS GCM, which in turn is constrained by meteorology from NASA’s Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) product. The simulated atmospheric field is compared with CH4 measurements, such as those from the TROPOspheric Monitoring Instrument (TROPOMI), and adjustments calculated following a Bayesian protocol. The accuracy of the resultant optimal atmospheric CH4 field can be demonstrated by its improved agreement (compared to a direct simulation of the CH4 inventories) with a host of independent CH4 measurements, such as those from the Total Carbon Column Observation Network (TCCON) and in situ observations from surface and airborne platforms.

Nikolay V. Balashov↗
DOE OSTI2023

SPRUCE Anaerobic oxidation of methane mitigates net methane production and responds to long-term experimental warming in a northern bog: Supporting data

This data set contains measurements of anaerobic oxidation of methane (AOM), net methane (CH4) production, carbon dioxide (CO2) production, and gross CH4 production measurements from the SPRUCE experiment (Hanson et al. 2017). CH4 is greenhouse gas with 45 times the sustained global warming potential of CO2 over 100 years, which may have significant implications on global climate change. The process of AOM plays a large role in the extent of CH4 emissions from wetland environments like those at the SPRUCE experiment site. This study conducted two on different dates. In experiment 1, net CH4 and CO2 production were measured with a gas chromatograph through the peat profile at in situ temperatures of the SPRUCE plots four times from May to October, 2016 (2016-05 to 2016-10). Two treatments were examined, a Porewater Treatment that was a 1:1 volumetric peat:porewater slurry and a No Porewater Treatment that was field-moist peat with no porewater added. Additionally, net CH4 production were measured at frequent intervals (from 4 hr to 9 d) in peat from selected SPRUCE plots from soil collected on October 16, 2016 (2016-10-16). Samples were collected from the SPRUCE plots, immediately made anaerobic, and transported to the University of Oregon for rate measurements within several days of collection. In experiment 2, AOM, net CH4 production, CO2 production, and gross CH4 production were measured through the peat profile at in situ field temperatures once from samples collected in July, 2021 (2021-07). The same two porewater treatments were examined. AOM was measured with a 13CH4 tracer method using a Picarro G2201-i analyzer for isotopic CO2/CH4 quantification with a small stable isotope module attached. This data set contains three data files in comma separate (*.csv) format. This data set is associated with the following publication: Barney, M, AM Hopple, LL Gregory, JK Keller, and SD Bridgham. 2024. Anaerobic oxidation of methane mitigates net methane production and responds to long-term experimental warming in a northern bog. Soil Biology and Biochemistry, 190, 109316. https://doi.org/10.1016/j.soilbio.2024.109316.

SPRUCE Experiment, Marcell Experimental Forest, Me↗
NASA NTRS1981

Pluto's atmospheric bulk near perihelion

The detection of CH4 frost on Pluto's surface implies a significant atmosphere for Pluto. Although Pluto's mass is small, about 7% of Triton's mass, the rapid escape ('blowoff') of gaseous CH4 can be prevented by the presence of a heavy gas mixed with the CH4. The resulting slow escape ('Jeans escape') of CH4 can be accommodated by sublimation of the surface CH4 frost so that an atmosphere exists in the steady state. A heavier gas must exist, otherwise the CH4 frost would have sublimated away long ago because of solar heat and rapid blowoff of gaseous CH4. Pluto is currently near perihelion where the CH4 component of the atmosphere may be 500 times denser than at apehelion. Significant seasonal changes in the atmospheric bulk are therefore possible.

Trafton, L.↗
NASA NTRS1994

Airborne boundary layer flux measurements of trace species over Canadian boreal forest and northern wetland regions

Airborne heat, moisture, O3, CO, and CH4 flux measurements were obtained over the Hudson Bay lowlands (HBL) and northern boreal forest regions of Canada during July - August 1990. The airborne flux measurements were an integral part of the NASA/Arctic Boundary Layer Expedition (ABLE) 3B field experiment executed in collaboration with the Canadian Northern Wetlands Study (NOWES). Airborne CH4 flux measurements were taken over a large portion of the HBL. The surface level flux of CH4 was obtained from downward extrapolations of multiple-level CH4 flux measurements. Methane source strengths ranged from -1 to 31 mg m(exp -2)/d, with the higher values occurring in relatively small, isolated areas. Similar measurements of the CH4 source strength in the boreal forest region of Schefferville, Quebec, ranged from 6 to 27 mg m(exp -2)/d and exhibited a diurnal dependence. The CH4 source strengths found during the ABLE 3B expedition were much lower than the seasonally averaged source strength of 51 mg m(exp -2)/d found for the Yukon-Kuskokwim delta region of Alaska during the previous ABLE 3A study. Large positive CO fluxes (0.31 to 0.53 parts per billion by volume (ppbv) m/s) were observed over the inland, forested regions of the HBL study area, although the mechanism for the generation of these fluxes was not identified. Repetitive measurements along the same ground track at various times of day near the Schefferville site also suggested a diurnal dependence for CO emissions. Measurements of surface resistance to the uptake of O3 (1.91 to 0.80 s/cm) for the HBL areas investigated were comparable to those observed near the Schefferville site (3.40 to 1.10 s/cm). Surface resistance values for the ABLE 3B study area were somewhat less than those observed over the Yukon-Kuskokwim delta during the previous ABLE 3A study. The budgets for heat, moisture, O3, CO, and CH4 were evaluated. The residuals from these budget studies indicated, for the cases selected, a moderate net photochemical production of O3 present in the boundary layer over the HBL that coincided with an in situ destruction of CO, although the mechanism responsible for the destruction of CO was not identified. Results from the O3 budget analysis indicate the importance of in situ photochemical production and its possible dominance over surface deposition to the local O3 budget at the Schefferville site. Measurements of the in situ production of O3 indicated a direct relationship between the presence of biomass burning or large-scale pollution effects. Residuals from budget calculations for conserved quantities (heat, moisture, and CH4) were compared with their respective surface fluxes to provide a measure of the internal self-consistency of the flux measurements.

Ritter, John A.↗
NASA NTRS2012

On the Sources of Methane to the Los Angeles Atmosphere

We use historical and new atmospheric trace gas observations to refine the estimated source of methane (CH4) emitted into California's South Coast Air Basin (the larger Los Angeles metropolitan region). Referenced to the California Air Resources Board (CARB) CO emissions inventory, total CH4 emissions are 0.44 +/- 0.15 Tg each year. To investigate the possible contribution of fossil fuel emissions, we use ambient air observations of methane (CH4), ethane (C2H6), and carbon monoxide (CO), together with measured C2H6 to CH4 enhancement ratios in the Los Angeles natural gas supply. The observed atmospheric C2H6 to CH4 ratio during the ARCTAS (2008) and CalNex (2010) aircraft campaigns is similar to the ratio of these gases in the natural gas supplied to the basin during both these campaigns. Thus, at the upper limit (assuming that the only major source of atmospheric C2H6 is fugitive emissions from the natural gas infrastructure) these data are consistent with the attribution of most (0.39 +/- 0.15 Tg yr-1) of the excess CH4 in the basin to uncombusted losses from the natural gas system (approximately 2.5-6% of natural gas delivered to basin customers). However, there are other sources of C2H6 in the region. In particular, emissions of C2H6 (and CH4) from natural gas seeps as well as those associated with petroleum production, both of which are poorly known, will reduce the inferred contribution of the natural gas infrastructure to the total CH4 emissions, potentially significantly. This study highlights both the value and challenges associated with the use of ethane as a tracer for fugitive emissions from the natural gas production and distribution system.

Wennberg, Paul O.↗
NASA NTRS2014

Analyzing Source Apportioned Methane in Northern California During DISCOVER-AQ-CA Using Airborne Measurements and Model Simulations

This study analyzes source apportioned methane (CH4) emissions and atmospheric concentrations in northern California during the Discover-AQ-CA field campaign using airborne measurement data and model simulations. Source apportioned CH4 emissions from the Emissions Database for Global Atmospheric Research (EDGAR) version 4.2 were applied in the 3-D chemical transport model GEOS-Chem and analyzed using airborne measurements taken as part of the Alpha Jet Atmospheric eXperiment over the San Francisco Bay Area (SFBA) and northern San Joaquin Valley (SJV). During the time period of the Discover-AQ-CA field campaign EDGAR inventory CH4 emissions were 5.30 Gg/day (Gg 1.0 109 grams) (equating to 1.9 103 Gg/yr) for all of California. According to EDGAR, the SFBA and northern SJV region contributes 30 of total emissions from California. Source apportionment analysis during this study shows that CH4 concentrations over this area of northern California are largely influenced by global emissions from wetlands and local/global emissions from gas and oil production and distribution, waste treatment processes, and livestock management. Model simulations, using EDGAR emissions, suggest that the model under-estimates CH4 concentrations in northern California (average normalized mean bias (NMB) -5 and linear regression slope 0.25). The largest negative biases in the model were calculated on days when hot spots of local emission sources were measured and atmospheric CH4 concentrations reached values 3.0 parts per million (model NMB -10). Sensitivity emission studies conducted during this research suggest that local emissions of CH4 from livestock management processes are likely the primary source of the negative model bias. These results indicate that a variety, and larger quantity, of measurement data needs to be obtained and additional research is necessary to better quantify source apportioned CH4 emissions in California and further the understanding of the physical processes controlling them.

Methane↗
NASA NTRS2012

The Influence of Ozone Precursor Emissions from Four World Regions on Tropospheric Composition and Radiative Climate Forcing

Ozone (O3) precursor emissions influence regional and global climate and air quality through changes in tropospheric O3 and oxidants, which also influence methane (CH4) and sulfate aerosols (SO4 (sup 2-)). We examine changes in the tropospheric composition of O3, CH4, SO4 (sup 2-) and global net radiative forcing (RF) for 20% reductions in global CH4 burden and in anthropogenic O3 precursor emissions (NOx, NMVOC, and CO) from four regions (East Asia, Europe and Northern Africa, North America, and South Asia) using the Task Force on Hemispheric Transport of Air Pollution Source-Receptor global chemical transport model (CTM) simulations, assessing uncertainty (mean plus or minus 1 standard deviation) across multiple CTMs. We evaluate steady state O3 responses, including long-term feedbacks via CH4. With a radiative transfer model that includes greenhouse gases and the aerosol direct effect, we find that regional NOx reductions produce global, annually averaged positive net RFs (0.2 plus or minus 0.6 to 1.7 2 mWm(sup -2)/Tg N yr(sup -1), with some variation among models. Negative net RFs result from reductions in global CH4 (-162.6 plus or minus 2 mWm(sup -2) for a change from 1760 to 1408 ppbv CH4) and regional NMVOC (-0.4 plus or minus 0.2 to 0.7 plus or minus 0.2 mWm(sup -2)/Tg C yr(sup -1) and CO emissions (-0.13 plus or minus 0.02 to -0.15 plus or minus 0.02 mWm(sup-2)/Tg CO yr(sup-1). Including the effect of O3 on CO2 uptake by vegetation likely makes these net RFs more negative by -1.9 to- 5.2 mWm(sup -2)/Tg N yr(sup -1), -0.2 to -0.7 mWm(sup -2)/Tg C yr(sup -1), and -0.02 to -0.05 mWm(sup -2)/ Tg CO yr(sup -1). Net RF impacts reflect the distribution of concentration changes, where RF is affected locally by changes in SO4 (sup -2), regionally to hemispherically by O3, and globally by CH4. Global annual average SO4 2 responses to oxidant changes range from 0.4 plus or minus 2.6 to -1.9 plus or minus 1.3 Gg for NOx reductions, 0.1 plus or minus 1.2 to -0.9 plus or minus 0.8 Gg for NMVOC reductions, and -0.09 plus or minus 0.5 to -0.9 plus or minus 0.8 Gg for CO reductions, suggesting additional research is needed. The 100-year global warming potentials (GWP(sub 100)) are calculated for the global CH4 reduction (20.9 plus or minus 3.7 without stratospheric O3 or water vapor, 24.2 plus or minus 4.2 including those components), and for the regional NOx, NMVOC, and CO reductions (18.7 plus or minus 25.9 to 1.9 plus or minus 8.7 for NOx, 4.8 plus or minus 1.7 to 8.3 plus or minus 1.9 for NMVOC, and 1.5 plus or minus 0.4 to 1.7 plus or minus 0.5 for CO). Variation in GWP(sub 100) for NOx, NMVOC, and CO suggests that regionally specific GWPs may be necessary and could support the inclusion of O3 precursors in future policies that address air quality and climate change simultaneously. Both global net RF and GWP100 are more sensitive to NOx and NMVOC reductions from South Asia than the other three regions.

ozone↗
NASA NTRS2015

Infrared Spectra and Optical Constants of Elusive Amorphous Methane

New and accurate laboratory results are reported for amorphous methane (CH4) ice near 10 K for the study of the interstellar medium (ISM) and the outer Solar System. Near- and mid-infrared (IR) data, including spectra, band strengths, absorption coefficients, and optical constants, are presented for the first time for this seldom-studied amorphous solid. The apparent IR band strength near 1300 cm(exp −1) (7.69 micrometer) for amorphous CH4 is found to be about 33% higher than the value long used by IR astronomers to convert spectral observations of interstellar CH4 into CH4 abundances. Although CH4 is most likely to be found in an amorphous phase in the ISM, a comparison of results from various laboratory groups shows that the earlier CH4 band strength at 1300 cm(exp −1) (7.69 micrometer) was derived from IR spectra of ices that were either partially or entirely crystalline CH4 Applications of the new amorphous-CH4 results are discussed, and all optical constants are made available in electronic form.

ISM: abundances↗