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Network design for quantifying urban CO<sub>2</sub> emissions: assessing trade-offs between precision and network density

The majority of anthropogenic CO 2 emissions are attributable to urban areas. While the emissions from urban electricity generation often occur in locations remote from consumption, many of the other emissions occur within the city limits. Evaluating the effectiveness of strategies for controlling these emissions depends on our ability to observe urban CO 2 emissions and attribute them to specific activities. Cost-effective strategies for doing so have yet to be described. Here we characterize the ability of a prototype measurement network, modeled after the Berkeley Atmospheric CO 2 Observation Network (BEACO 2 N) in California's Bay Area, in combination with an inverse model based on the coupled Weather Research and Forecasting/Stochastic Time-Inverted Lagrangian Transport (WRF-STILT) to improve our understanding of urban emissions. The pseudo-measurement network includes 34 sites at roughly 2 km spacing covering an area of roughly 400 km 2 . The model uses an hourly 1 × 1 km 2 emission inventory and 1 × 1 km 2 meteorological calculations. We perform an ensemble of Bayesian atmospheric inversions to sample the combined effects of uncertainties of the pseudo-measurements and the model. We vary the estimates of the combined uncertainty of the pseudo-observations and model over a range of 20 to 0.005 ppm and vary the number of sites from 1 to 34. We use these inversions to develop statistical models that estimate the efficacy of the combined model–observing system in reducing uncertainty in CO 2 emissions. We examine uncertainty in estimated CO 2 fluxes on the urban scale, as well as for sources embedded within the city such as a line source (e.g., a highway) or a point source (e.g., emissions from the stacks of small industrial facilities). Using our inversion framework, we find that a dense network with moderate precision is the preferred setup for estimating area, line, and point sources from a combined uncertainty and cost perspective. The dense network considered here (modeled after the BEACO 2 N network with an assumed mismatch error of 1 ppm at an hourly temporal resolution) could estimate weekly CO 2 emissions from an urban region with less than 5 % error, given our characterization of the combined observation and model uncertainty.

54 ENVIRONMENTAL SCIENCES↗

MIX: a mosaic Asian anthropogenic emission inventory under the international collaboration framework of the MICS-Asia and HTAP

Here, the MIX inventory is developed for the years 2008 and 2010 to support the Model Inter-Comparison Study for Asia (MICS-Asia) and the Task Force on Hemispheric Transport of Air Pollution (TF HTAP) by a mosaic of up-to-date regional emission inventories. Emissions are estimated for all major anthropogenic sources in 29 countries and regions in Asia. We conducted detailed comparisons of different regional emission inventories and incorporated the best available ones for each region into the mosaic inventory at a uniform spatial and temporal resolution. Emissions are aggregated to five anthropogenic sectors: power, industry, residential, transportation, and agriculture. We estimate the total Asian emissions of 10 species in 2010 as follows: 51.3 Tg SO 2 , 52.1 Tg NO x , 336.6 Tg CO, 67.0 Tg NMVOC (non-methane volatile organic compounds), 28.8 Tg NH 3 , 31.7 Tg PM 10 , 22.7 Tg PM 2.5 , 3.5 Tg BC, 8.3 Tg OC, and 17.3 Pg CO 2 . Emissions from China and India dominate the emissions of Asia for most of the species. We also estimated Asian emissions in 2006 using the same methodology of MIX. The relative change rates of Asian emissions for the period of 2006–2010 are estimated as follows: –8.1 % for SO 2 , +19.2 % for NO x , +3.9 % for CO, +15.5 % for NMVOC, +1.7 % for NH 3 , –3.4 % for PM 10 , –1.6 % for PM 2.5 , +5.5 % for BC, +1.8 % for OC, and +19.9 % for CO 2 . Model-ready speciated NMVOC emissions for SAPRC-99 and CB05 mechanisms were developed following a profile-assignment approach.

54 ENVIRONMENTAL SCIENCES↗

MIXv2: a long-term mosaic emission inventory for Asia (2010–2017)

The MIXv2 Asian emission inventory is developed under the framework of the Model Inter-Comparison Study for Asia (MICS-Asia) Phase IV and produced from a mosaic of up-to-date regional emission inventories. We estimated the emissions for anthropogenic and biomass burning sources covering 23 countries and regions in East, Southeast and South Asia and aggregated emissions to a uniform spatial and temporal resolution for seven sectors: power, industry, residential, transportation, agriculture, open biomass burning and shipping. Compared to MIXv1, we extended the dataset to 2010–2017, included emissions of open biomass burning and shipping, and provided model-ready emissions of SAPRC99, SAPRC07, and CB05. A series of unit-based point source information was incorporated covering power plants in China and India. A consistent speciation framework for non-methane volatile organic compounds (NMVOCs) was applied to develop emissions by three chemical mechanisms. The total Asian emissions for anthropogenic/open biomass sectors in 2017 are estimated as follows: 41.6/1.1 Tg NO x , 33.2/0.1 Tg SO 2 , 258.2/20.6 Tg CO, 61.8/8.2 Tg NMVOC, 28.3/0.3 Tg NH 3 , 24.0/2.6 Tg PM 10 , 16.7/2.0 Tg PM 2.5 , 2.7/0.1 Tg BC (black carbon), 5.3/0.9 Tg OC (organic carbon), and 18.0/0.4 Pg CO 2 . The contributions of India and Southeast Asia were emerging in Asia during 2010–2017, especially for SO 2 , NH 3 and particulate matter. Gridded emissions at a spatial resolution of 0.1° with monthly variations are now publicly available. This updated long-term emission mosaic inventory is ready to facilitate air quality and climate model simulations, as well as policymaking and associated analyses.

54 ENVIRONMENTAL SCIENCES↗

Is there warming in the pipeline? A multi-model analysis of the Zero Emissions Commitment from CO 2

Abstract. The Zero Emissions Commitment (ZEC) is the change in global mean temperature expected to occur following the cessation of net CO 2 emissions and as such is a critical parameter for calculating the remaining carbon budget. The Zero Emissions Commitment Model Intercomparison Project (ZECMIP) was established to gain a better understanding of the potential magnitude and sign of ZEC, in addition to the processes that underlie this metric. A total of 18 Earth system models of both full and intermediate complexity participated in ZECMIP. All models conducted an experiment where atmospheric CO 2 concentration increases exponentially until 1000 PgC has been emitted. Thereafter emissions are set to zero and models are configured to allow free evolution of atmospheric CO 2 concentration. Many models conducted additional second-priority simulations with different cumulative emission totals and an alternative idealized emissions pathway with a gradual transition to zero emissions. The inter-model range of ZEC 50 years after emissions cease for the 1000 PgC experiment is -0.36 to 0.29°C, with a model ensemble mean of -0.07 °C, median of -0.05°C, and standard deviation of 0.19°C. Models exhibit a wide variety of behaviours after emissions cease, with some models continuing to warm for decades to millennia and others cooling substantially. Analysis shows that both the carbon uptake by the ocean and the terrestrial biosphere are important for counteracting the warming effect from the reduction in ocean heat uptake in the decades after emissions cease. This warming effect is difficult to constrain due to high uncertainty in the efficacy of ocean heat uptake. Overall, the most likely value of ZEC on multi-decadal timescales is close to zero, consistent with previous model experiments and simple theory.

MacDougall, Andrew H.↗

Electrostatic emissions between electron gyroharmonics in the outer magnetosphere

Electrostatic emissions are often observed by spacecraft in the outer magnetosphere at frequencies between low electron gyroharmonics. The emissions include the well-known odd half-harmonic emissions as well as weaker emissions which occur near the electron plasma frequency. A scheme is constructed for classifying the emissions, and it is shown that a theoretical model which has been previously used to explain '3/2' emissions can be extended to the other classes of emissions. All of the emissions therefore appear to be generated by the same basic mechanism: an unstable electron plasma distribution consisting of cold electrons (below 100 eV) and hot loss cone electrons (about 1 keV). Each emission class is associated with a particular range of model parameters; the wide-band electric field data can thus be used to infer the density and temperature of the cold plasma component. The model predicts that gyroharmonic emissions near the plasma frequency require large cold plasma densities.

Hubbard, R. F.↗

Dynamics and X-ray emission of a galactic superwind interacting with disk and halo gas

There is a general agreement that the conspicuous extranuclear X-ray, optical-line, and radio-contiuum emission of starbursts is associated with powerful galactic superwinds blowing from their centers. However, despite the significant advances in observational studies of superwinds, there is no consensus on the nature of the emitting material and even on the emission mechanisms themselves. This is to a great extent a consequence of a poor understanding of dynamical processes in the starburst superwind regions. To address this issue, we have conducted two-dimensional hydrodynamical simulations of galactic superwinds. While previous similar studies have used a single (disk) component to represent the ISM of the starburst galaxy, we analyze the interaction of the wind with a two-component disk-halo ambient interstellar medium and argue that this two-component representation is crucial for adequate modeling of starbursts. The emphasis of this study is on the geometry and structure of the wind region and the X-ray emission arising in the wind material and the shocked gas in the disk and the halo of the galaxy. The simulation results have shown that a clear-cut bipolar wind can easily develop under a range of very different conditions. On the other hand, a complex 'filamentary' structure associated with the entrained dense disk material is found to arise within the hot bubble blown out by the wind. The flow pattern within the bubble is dominated equally by the central biconic outflow and a system of whirling motions r elated to the origin and development of the 'filaments'. The filament parameters make them a good candidate for optical-emission-line filamentary gas observed in starburst halos. We find that the history of mass and energy deposition in the starburst region of the galaxy is crucial for wind dynamics. A 'mild' early wind, which arises as a result of the cumulative effect of stellar winds from massive stars, produces a bipolar vertical cavity in the disk and halo gas without strongly affecting the gaseous disk, thus creating conditions for virtually free vertical escape of the hot gas at the later, much more violent supernova-dominated phases of the starburst. We calculate the luminosity, mass, and effective temperature of the X-ray emitting gas in the 'soft' (0.1 to 0.7 keV, 0.7 to 2.2 keV, and 0.1 to 2.2 keV) and 'hard' (1.6 to 8.3 keV) energy bands and estimate the contribution of different gaseous components to the X-ray flux in these bands. Analysis of these parameters enables us to make conclusions regarding the nature of the X-ray-emitting material. We have inferred that the bulk of the soft thermal X-ray emission from starbursts arises in the wind-shocked material of the disk and halo gas rather than in the wind material itself. This enables us to predict that the integrated soft X-ray spectra of starbursts need not show an overabundance of heavy elements which are believed to be produced copiously in the centers of starbursts. Unlike soft X-ray emission, the hard component of thermal X-ray emission is found to originate in the wind material ejected from the starburst region. However, the derived ratio of hard-to-soft X-ray luminosities is too small compared to that observed in starbursts. We conclude therefore that the observed hard X-ray emission of starbursts is probably not associated with the thermal emission of hot wind or ambient shocked gas. Typical temperatures of the bulk of the soft X-ray-emitting material in our very different models have been found to agree well with the ones estimated on the basis of the ROSAT data for the soft component of X-ray emission of nearby starbursts. We predict that temperatures of the extranuclear soft X-ray-emitting gas in starburst galaxies with heavy element abundances near solar should be close to T(sub Xs = 2 to 5 x 10(exp 6)K.

Suchkov, Anatoly A.↗

Analyses of Scenarios for Past and Possible Future Aircraft Emissions

This project contains several components to work with the NASA AEAP program in better definition of scenarios for aircraft emissions and in determining the sensitivity of the atmosphere to such emissions. Under this project, Don Wuebbles continues as chair of the Operations and Emissions Scenarios Committee for AEAP. We are also coordinating with the International Civil Aviation Organization (ICAO) to ensure the highest quality possible in the emissions scenarios promoted by the Emissions Scenarios committee. We continue to help coordination of NASA AEAP with international activities. This includes work with ICAO towards international analysis of aircraft emissions inventories; performing analyses to compare and evaluate databases of aircraft emissions developed for NASA and by various international groups and from these analyses, develop guidelines for future emissions scenarios development. Special sensitivity analyses, using our two-dimensional chemical-transport model of the global troposphere and stratosphere, have been used to determine potential sensitivity of further enhancements that could be made to emissions scenarios development. The latter studies are to be used in prioritizing further emissions scenario development.

Wuebbles, Donald J.↗

First Year Wilkinson Microwave Anisotropy Probe (WMAP) Observations: Foreground Emission

The WMAP mission has mapped the full sky to determine the geometry, content, and evolution of the universe. Full sky maps are made in five microwave frequency bands to separate the temperature anisotropy of the cosmic microwave background (CMB) from foreground emission, including diffuse Galactic emission and Galactic and extragalactic point sources. We define masks that excise regions of high foreground emission, so CMB analyses can became out with minimal foreground contamination. We also present maps and spectra of the individual emission components, leading to an improved understanding of Galactic astrophysical processes. The effectiveness of template fits to remove foreground emission from the WMAP data is also examined. These efforts result in a CMB map with minimal contamination and a demonstration that the WMAP CMB power spectrum is insensitive to residual foreground emission. We use a Maximum Entropy Method to construct a model of the Galactic emission components. The observed total Galactic emission matches the model to less than 1% and the individual model components are accurate to a few percent. We find that the Milky Way resembles other normal spiral galaxies between 408 MHz and 23 GHz, with a synchrotron spectral index that is flattest (beta(sub s) approx. -2.5) near star-forming regions, especially in the plane, and steepest (beta(sub s) approx. -3) in the halo. This is consistent with a picture of relativistic cosmic ray electron generation in star-forming regions and diffusion and convection within the plane. The significant synchrotron index steepening out of the plane suggests a diffusion process in which the halo electrons are trapped in the Galactic potential long enough to suffer synchrotron and inverse Compton energy losses and hence a spectral steepening. The synchrotron index is steeper in the WMAP bands than in lower frequency radio surveys, with a spectral break near 20 GHz to beta(sub s) less than -3. The modeled thermal dust spectral index is also steep in the WMAP bands, with beta(sub d) approx. = 2.2. Our model is driven to these conclusions by the low level of total foreground contamination at approx. 60 GHz. Microwave and Ha measurements of the ionized gas agree well with one another at about the expected levels. Spinning dust emission is limited to less than 5% of the Ka-band foreground emission. A catalog of 208 point sources is presented. The reliability of the catalog is 98%, i.e., we expect five of the 208 sources to be statistically spurious. The mean spectral index of the point sources is alpha approx. 0(beta approx. -2). Derived source counts suggest a contribution to the anisotropy power from unresolved sources of (15.0 +/- 1.4) x 10(exp -3)micro sq K sr at Q-band and negligible levels at V-band and W-band. The Sunyaev-Zeldovich effect is shown to be a negligible "contamination" to the maps.

Bennett, C. L.↗

Mapping Isoprene Emissions over North America using Formaldehyde Column Observations from Space

I] We present a methodology for deriving emissions of volatile organic compounds (VOC) using space-based column observations of formaldehyde (HCHO) and apply it to data from the Global Ozone Monitoring Experiment (GOME) satellite instrument over North America during July 1996. The HCHO column is related to local VOC emissions, with a spatial smearing that increases with the VOC lifetime. lsoprene is the dominant HCHO precursor over North America in summer, and its lifetime (approx. = 1 hour) is sufficiently short that the smearing can be neglected. We use the Goddard Earth Observing System global 3-D model of tropospheric chemistry (GEOS-CHEM) to derive the relationship between isoprene emissions and HCHO columns over North America and use these relationships to convert the GOME HCHO columns to isoprene emissions. We also use the GEOS-CHEM model as an intermediary to validate the GOME HCHO column measurements by comparison with in situ observations. The GEOS-CHEM model including the Global Emissions Inventory Activity (GEIA) isoprene emission inventory provides a good simulation of both the GOME data (r(sup 2) = 0.69, n = 756, bias = +l1 %) and the in situ summertime HCHO measurements over North America (r(sup 2) = 0.47, n = 10, bias = -3%). The GOME observations show high values over regions of known high isoprene emissions and a day-to-day variability that is consistent with the temperature dependence of isoprene emission. Isoprene emissions inferred from the GOME data are 20% less than GEIA on average over North America and twice those from the U S . EPA Biogenic Emissions Inventory System (BEIS2) inventory. The GOME isoprene inventory when implemented in the GEOS-CHEM model provides a better simulation of the HCHO in situ measurements thaneitherGEIAorBEIS2 (r(sup 2) = 0.71,n= 10, bias = -10 %).

Palmer, Paul I.↗

Removing Spectral Diagnostics of Galactic and Stellar X-Ray Emission from Charged Exchange Recombination

Our research uses the electron beam ion trap (EBIT) at the Lawrence Livermore National Laboratory to study X-ray emission from the charge exchange (CX) of highly charged ions with neutral gases. The resulting data help to fill a void in existing experimental and theoretical understanding of this atomic physics process, and are needed to explain all or part of the observed X-ray emission from the soft X-ray background, stellar winds, the Galactic Center and Galactic Ridge, supernova ejecta, and photoionized nebulae. Appreciation of the astrophysical relevance of our work continues to grow with the publication of roughly a dozen papers in the past four years describing Chandra and XMM observations of geocoronal and heliospheric CX emission, the temporal variation of such emission and correlation with X-ray emission enhancements observed by ROSAT, the theoretical spatial distribution of that emission, and CX emission around other stars. A similar number of papers were also published during that time describing CX emission from planets and comets. We expect that the launch of ASTRSE2, with its second-generation XRS microcalo- (with 6-eV resolution), will reveal even more clearly the contributions of CX to astrophysical emission. In our EBIT work we collected CX spectra from such ions as H-like and He-like Ne, Ar, and Fe. Our early measurements were made with a high-purity Ge detector, but during the second year we began operation of the first-generation XRS microcalorimeter (a twin of the XRS on ASTRO-E) and greatly improved the resolution of our measurements from roughly 150 eV (FWHM) with the Ge detectors to 10 eV with the XRS. We found that saturation of the XRS counting apparatus, which we described in our proposal as a potential concern, is not a problem for studying CX. During the course of our research, we expanded the number of injection gases permitted by the LLNL safety team, purchased and eventually operated an atomic H source, and clearly demonstrated the feasibility of our longer-range plan. For example, we successfully injected He into EBIT (not a small feat because of the difficulty of maintaining a good vacuum with He and avoiding electrical breakdown) to collect a H-like oxygen CX spectrum. The highest energy CX spectrum recorded with the XRS to date is that of the Ar K-shell emission. These measurements provided the first observation of the relative intensity ratios of resolved He-like singlet and triplet n=2->1 lines. We also carried out measurements of He-like Ne as a function of collision energy (i.e., ion temperature). Significant differences in the resulting x-ray spectra were noted. In all cases, the intensity of high-n H-like Lyman lines is significantly higher than current theoretical CX models predict.

Wargelin, Brad↗

Land Surface Microwave Emissivities Derived from AMSR-E and MODIS Measurements with Advanced Quality Control

A microwave emissivity database has been developed with data from the Advanced Microwave Scanning Radiometer-EOS (AMSR-E) and with ancillary land surface temperature (LST) data from the Moderate Resolution Imaging Spectroradiometer (MODIS) on the same Aqua spacecraft. The primary intended application of the database is to provide surface emissivity constraints in atmospheric and surface property retrieval or assimilation. An additional application is to serve as a dynamic indicator of land surface properties relevant to climate change monitoring. The precision of the emissivity data is estimated to be significantly better than in prior databases from other sensors due to the precise collocation with high-quality MODIS LST data and due to the quality control features of our data analysis system. The accuracy of the emissivities in deserts and semi-arid regions is enhanced by applying, in those regions, a version of the emissivity retrieval algorithm that accounts for the penetration of microwave radiation through dry soil with diurnally varying vertical temperature gradients. These results suggest that this penetration effect is more widespread and more significant to interpretation of passive microwave measurements than had been previously established. Emissivity coverage in areas where persistent cloudiness interferes with the availability of MODIS LST data is achieved using a classification-based method to spread emissivity data from less-cloudy areas that have similar microwave surface properties. Evaluations and analyses of the emissivity products over homogeneous snow-free areas are presented, including application to retrieval of soil temperature profiles. Spatial inhomogeneities are the largest in the vicinity of large water bodies due to the large water/land emissivity contrast and give rise to large apparent temporal variability in the retrieved emissivities when satellite footprint locations vary over time. This issue will be dealt with in the future by including a water fraction correction. Also note that current reliance on the MODIS day-night algorithm as a source of LST limits the coverage of the database in the Polar Regions. We will consider relaxing the current restriction as part of future development.

Moncet, Jean-Luc↗

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.↗

Quantification of CO2 and CH4 emissions over Sacramento, California, based on divergence theorem using aircraft measurements

Emission estimates of carbon dioxide (CO2) and methane (CH4) and the meteorological factors affecting them are investigated over Sacramento, California, using an aircraft equipped with a cavity ring-down greenhouse gas sensor as part of the Alpha Jet Atmospheric eXperiment (AJAX) project. To better constrain the emission fluxes, we designed flights in a cylindrical pattern and computed the emission fluxes from two flights using a kriging method and Gauss’s divergence theorem. Differences in wind treatment and assumptions about background concentrations affect the emission estimates by a factor of 1.5 to 7. The uncertainty is also impacted by meteorological conditions and distance from the emission sources. The vertical layer averaging affects the flux estimate, but the choice of raw wind or mass-balanced wind is more important than the thickness of the vertical averaging for massbalanced wind for both urban and local scales. The importance of vertical mass transfer for flux estimates is examined, and the difference in the total emission estimate with and without vertical mass transfer is found to be small, especially at the local scale. The total flux estimates accounting for the entire circumference are larger than those based solely on measurements made in the downwind region. This indicates that a closed-shape flight profile can better contain total emissions relative to a one-sided curtain flight because most cities have more than one point source and wind direction can change with time and altitude. To reduce the uncertainty of the emission estimate, it is important that the sampling strategy account not only for known source locations but also possible unidentified sources around the city. Our results highlight that aircraft-based measurements using a closed-shape flight pattern are an efficient and useful strategy for identifying emission sources and estimating local- and city-scale greenhouse gas emission fluxes.

Ju-Mee Ryoo↗

Wetland Emission and Atmospheric Sink Changes Explain Methane Growth in 2020

Atmospheric methane growth reached an exceptionally high rate of 15.1 ± 0.4 parts per billion per year in 2020 despite a probable decrease in anthropogenic methane emissions during COVID-19 lockdowns(1). Here we quantify changes in methane sources and in its atmospheric sink in 2020 compared with 2019. We find that, globally, total anthropogenic emissions decreased by 1.2 ± 0.1 teragrams of methane per year (Tg CH4 yr−1), fire emissions decreased by 6.5 ± 0.1 Tg CH4 yr−1 and wetland emissions increased by 6.0 ± 2.3 Tg CH4 yr−1. Tropospheric OH concentration decreased by 1.6 ± 0.2 per cent relative to 2019, mainly as a result of lower anthropogenic nitrogen oxide (NOx) emissions and associated lower free tropospheric ozone during pandemic lockdowns(2). From atmospheric inversions, we also infer that global net emissions increased by 6.9 ± 2.1 Tg CH4 yr−1 in 2020 relative to 2019, and global methane removal from reaction with OH decreased by 7.5 ± 0.8 Tg CH4 yr−1. Therefore, we attribute the methane growth rate anomaly in 2020 relative to 2019 to lower OH sink (53 ± 10 per cent) and higher natural emissions (47 ± 16 per cent), mostly from wetlands. In line with previous findings(3,4,) our results imply that wetland methane emissions are sensitive to a warmer and wetter climate and could act as a positive feedback mechanism in the future. Our study also suggests that nitrogen oxide emission trends need to be taken into account when implementing the global anthropogenic methane emissions reduction pledge(5).

Shushi Peng↗

Version 2 of the global catalogue of large anthropogenic and volcanic SO 2 sources and emissions derived from satellite measurements

Sulfur dioxide (SO 2 ) measurements from the Ozone Monitoring Instrument (OMI), Ozone Mapping and Profiler Suite (OMPS), and TROPOspheric Monitoring Instrument (TROPOMI) satellite spectrometers were used to update and extend the previously developed global catalogue of large SO 2 emission sources. This version 2 of the global catalogue covers the period of 2005–2021 and includes a total of 759 continuously emitting point sources releasing from about 10 kt yr −1 to more than 4000 kt yr −1 of SO 2 , that have been identified and grouped by country and primary source origin: volcanoes (106 sources); power plants (477); smelters (74); and sources related to the oil and gas industry (102). There are several major improvements compared to the original catalogue: it combines emissions estimates from three satellite instruments instead of just OMI, uses a new version 2 of the OMI and OMPS SO 2 dataset, and updated consistent site-specific air mass factors (AMFs) are used to calculate SO 2 vertical column densities (VCDs). The newest TROPOMI SO 2 data processed with the Covariance-Based Retrieval Algorithm (COBRA), used in the catalogue, can detect sources with emissions as low as 8 kt yr −1 (in 2018–2021) compared to the 30 kt yr −1 limit for OMI. In general, there is an overall agreement within ±12 % in total emissions estimated from the three satellite instruments for large regions. For individual emission sources, the spread is larger: the annual emissions estimated from OMI and TROPOMI agree within ±13 % in 50 % of cases and within ±28 % in 90 % of cases. The version 2 catalogue emissions were calculated as a weighted average of emission estimates from the three satellite instruments using an inverse-variance weighting method. OMI, OMPS, and TROPOMI data contribute 7 %, 5 %, and 88 % to the average, respectively, for small (<30 kt yr −1 ) sources and 33 %, 20 %, and 47 %, respectively, for large (>300 kt yr −1 ) sources. The catalogue data show an approximate 50 % decline in global SO 2 emissions between 2005 and 2021, although emissions were relatively stable during the last 3 years. The version 2 of the global catalogue has been posted at the NASA global SO 2 monitoring website (https://doi.org/10.5067/MEASURES/SO2/DATA406, Fioletov et al., 2022).

volcanic↗

The Search for High Energy Extended Emission by Fermi-LAT from Swift-Localized Gamma-Ray Bursts

The brighter Fermi-LAT bursts have exhibited emission at energies >0.1 GeV that persists as late as {approx}2 ks after the prompt phase has nominally ended. This so-called 'extended emission' could arise from continued activity of the prompt burst mechanism or it could be the start of a high energy afterglow component. The high energy extended emission seen by the LAT has typically followed a t{sup -}{gamma} power-law temporal decay where {gamma} {approx} 1.2-1.7 and has shown no strong indication of spectral evolution. In contrast, the prompt burst emission generally displays strong spectral variability and more complex temporal changes in the LAT band. This differing behavior suggests that the extended emission likely corresponds to an early afterglow phase produced by an external shock. In this study, we look for evidence of high energy extended emission from 145 Swift-localized GRBs that have occurred since the launch of Fermi. A majority of these bursts were either outside of the LAT field-of-view or were otherwise not detected by the LAT during the prompt phase. However, because of the scanning operation of the Fermi satellite, the long-lived extended emission of these bursts may be detectable in the LAT data on the {approx}few ks time scale. We will look for emission from individual bursts and will perform a stacking analysis in order to set bounds on this emission for the sample as a whole. The detection of such emission would have implications for afterglow models and for the overall energy budget of GRBs.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Criteria Air Pollutants and Greenhouse Gas Emissions from Hydrogen Production in U.S. Steam Methane Reforming Facilities

The global and U.S. domestic effort to develop a clean energy economy and curb environmental pollution incentivizes the use of hydrogen as a transportation fuel, owing to its zero tailpipe pollutant emissions and high fuel efficiency in fuel cell electric vehicles (FCEVs). However, the hydrogen production process is not emissions free. Conventional hydrogen production via steam methane reforming (SMR) is energy intensive, coproduces carbon dioxide, and emits air pollutants. Therefore, it is necessary to quantify the environmental impacts of SMR hydrogen production alongside the use-phase of FCEVs. This study fills the information gap, analyzing the greenhouse gas (GHG) and criteria air pollutant (CAP) emissions associated with hydrogen production in U.S. SMR facilities by compiling and matching the facility-reported GHG and CAP emissions data with facilities’ hydrogen production data. The actual amounts of hydrogen produced at U.S. SMR facilities are often confidential. Thus, we have developed four approaches to estimate the hydrogen production amounts. The resultant GHG and CAP emissions per MJ of hydrogen produced in individual facilities were aggregated to develop emission values for both a national median and a California state median. Lastly, this study also investigates the breakdown of facility emissions into combustion emissions and noncombustion emissions.

54 ENVIRONMENTAL SCIENCES↗

Three-dimensional spectrum mapping of bright emission centers: Investigating the brightness-limiting process in Eu-doped GaN red light emitting diodes

A pulse-driven emission-spectroscopy mapping technique is used to investigate the bright emission centers in Eu-doped GaN (GaN:Eu) red light emitting diodes (LED). The LEDs are operated in pulse-driven mode, and the emission spectra are acquired for a range of pulse frequencies. This ensemble of emission spectral data yields a three-dimensional mapping that allows the origin of emission lines to be identified by visual inspection. The identification was achieved even for a weak {sup 5}D{sub 0} → {sup 7}F{sub 3} transition in conventional photoluminescence measurements. A peculiar split is observed in the {sup 5}D{sub 0} → {sup 7}F{sub 3} transition for the bright emission center referred to as OMVPE 8. Despite the unique transition at this emission center, the emission efficiencies for the {sup 5}D{sub 0} → {sup 7}F{sub 3} and {sup 5}D{sub 0} → {sup 7}F{sub 2} transitions were identical. This finding indicates that the excitation of the emission centers, rather than the radiative transitions, is the limiting process that determines the GaN:Eu red LED brightness.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗