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DOE OSTI2015

Optimal carbon capture and storage contracts using historical CO 2 emissions levels

In an effort to reduce carbon dioxide (CO 2 ) emissions to the atmosphere, carbon capture and storage (CCS) technology has been developed to collect CO 2 from emissions generators and store it underground. Recent proposed legislation would limit the volume of emissions generated from power sources, effectively requiring some sources to participate in CCS. Both emissions sources and storage operators require incentives to enter into contracts to capture excess emissions at the source, and transport and store the CO 2 underground. As the level of emissions from power plants is stochastic and carryover into future time periods is expensive, we develop a newsvendor model to determine the optimal price and volume of these contracts to maximize the expected profit of the storage operator and encourage the participation of multiple emissions sources. Because the storage operator has a limit on the amount of CO 2 that can be injected each month, this limit affects the allocation of the optimal contract amounts between the emitters. Furthermore, the distribution of emissions and relative costs of transportation also influence the optimal policy. In addition to analytical solutions, we present data-driven methods for using correlated emissions data to determine the optimal price and volume of these contracts.

42 ENGINEERING↗

DOE OSTI2011

Comparison of methodologies estimating emissions of aircraft pollutants, environmental impact assessment around airports

Air transportation growth has increased continuously over the years. The rise in air transport activity has been accompanied by an increase in the amount of energy used to provide air transportation services. It is also assumed to increase environmental impacts, in particular pollutant emissions. Traditionally, the environmental impacts of atmospheric emissions from aircraft have been addressed in two separate ways; aircraft pollutant emissions occurring during the landing and take-off (LTO) phase (local pollutant emissions) which is the focus of this study, and the non-LTO phase (global/regional pollutant emissions). Aircraft pollutant emissions are an important source of pollution and directly or indirectly harmfully affect human health, ecosystems and cultural heritage. There are many methods to asses pollutant emissions used by various countries. However, using different and separate methodology will cause a variation in results, some lack of information and the use of certain methods will require justification and reliability that must be demonstrated and proven. In relation to this issue, this paper presents identification, comparison and reviews of some of the methodologies of aircraft pollutant assessment from the past, present and future expectations of some studies and projects focusing on emissions factors, fuel consumption, and uncertainty. This paper also provides reliable information on the impacts of aircraft pollutant emissions in short term and long term predictions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2013

Developing an indicator for the chronic health impact of traffic-related pollutant emissions

The goal of this study is to develop an emission based indicator for the health impact of the air pollution caused by traffic. This indicator must make it possible to compare different situations, for example different Urban Travel Plans, or technical innovations. Our work is based on a literature survey of methods for evaluating health impacts and, more particularly, those which relate to the atmospheric pollution caused by transport. We then define a health impact indicator based on the traffic emissions, named IISCEP for Chronic health impact indicator of pollutant emission. Here health is understood in a restricted meaning, excluding well-being. Only primary pollutants can be considered, as the inputs are emission data and an indicator must be simple. The indicator is calculated as the sum of each pollutant emission multiplied by a dispersion and exposition factor and a substance specific toxicity factor taking account of the severity. Last, two examples are shown using the IISCEP: comparison between petrol and diesel vehicles, and Nantes urban district in 2008 vs 2002. Even if it could still be improved, IISCEP is a straightforward indicator which can be used to gauge the chronic effects of inhaling primary pollutants. It can only be used in comparisons, between different scenarios or different technologies. The quality of the emissions data and the choice of the pollutants that are considered are the two essential factors that determine its validity and reliability. - Highlights: Black-Right-Pointing-Pointer The goal of the study is to develop an emission based indicator for the health impact of the air pollution caused by traffic. Black-Right-Pointing-Pointer It is based on a literature survey of methods for evaluating health impacts related to the atmospheric pollution. Black-Right-Pointing-Pointer We define a composite indicator based on the traffic emissions and on local data as dispersion conditions and population. Black-Right-Pointing-Pointer The indicator is a combination of pollutant emission, dispersion, exposition factor, and substance specific toxicity factor. Black-Right-Pointing-Pointer Applications are global (e.g. comparison of vehicle technologies) or local (e.g. comparison of populations or areas).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2016

New research assessing the effect of engine operating conditions on regulated emissions of a 4-stroke motorcycle by test bench measurements

In the latest years the effect of powered two-wheelers on air polluting emissions is generally noteworthy all over the world, notwithstanding advances in internal combustion engines allowed to reduce considerably both fuel consumption and exhaust emissions of SI engines. Nowadays, in fact, these vehicles represent common means of quotidian moving, serving to meet daily urban transport necessities with a significant environmental impact on air quality. Besides, the emissive behavior of the two-wheelers measured under fixed legislative driving standards (and not on the local driving conditions) might not be sufficiently representative of real world motorcycle riding. The purpose of this investigation is a deeper research on emissive levels of in-use motorcycles equipped with last generation SI engines under real world driving behavior. In order to analyze the effect of vehicle instantaneous speed and acceleration on emissive behavior, instantaneous emissions of CO, HC and NO{sub X} were measured in the exhaust of a four-stroke motorcycle, equipped with a three-way catalyst and belonging to the Euro-3 legislative category. Experimental tests were executed on a chassis dynamometer bench in the laboratories of the National Research Council (Italy), during the Type Approval test cycle, at constant speed and under real-world driving cycles. This analytical-experimental investigation was executed with a methodology that improves vehicles emission assessment in comparison with the modeling approaches that are based on fixed legislative driving standards. The statistical processing results so obtained are very useful also in order to improve the database of emission models commonly used for estimating emissions from road transport sector, then they can be used to evaluate the environmental impact of last generation medium-size motorcycles under real driving behaviors.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Soil carbon inventory to quantify the impact of land use change to mitigate greenhouse gas emissions and ecosystem services

We report that currently the land use and land use change (LULUC) emits 1.3 ± 0.5 Pg carbon (C) year -1 , equivalent to 8% of the global annual emissions. The objectives of this study were to quantify (1) the impact of LULUC on greenhouse gas (GHG) emissions in a subtropical region and (2) the role of conservation agriculture to mitigate GHG emissions promoting ecosystem services. We developed a detailed IPCC Tier 2 GHG inventory for the Campos Gerais region of southern Brazil that has large cropland area under long-term conservation agriculture with high crop yields. The inventory accounted for historical and current emissions from fossil fuel combustion, LULUC and other minor sources. We used Century model to simulate the adoption of conservation best management practices, to all croplands in the region from 2017 to 2117. Our results showed historical (1930 – 2017) GHG emissions of 412 Tg C, in which LULUC contributes 91% (376±130 Tg C), the uncertainties ranged between 13 and 36%. Between 1930 and 1985 LULUC was a major source of GHG emission, however from 1985 to 2015 fossil fuel combustion became the primary source of GHG emission. Forestry sequestered 52 ± 24 Tg C in 0.6 Mha in a period of 47 years (1.8 Tg C Mha -1 year -1 ) and no-till sequestered 30.4 ± 24 Tg C in 2 Mha in a period of 32 years (0.5 Tg C Mha -1 year -1 ) being the principal GHG mitigating activities in the study area. Lastly, the model predictions showed that best management practices have the potential to mitigate 13 years of regional emissions (330 Tg C in 100 years) or 105 years of agriculture, forestry and livestock emissions (40 Tg C in 100 years) making the agriculture sector a net carbon (C) sink and promoting ecosystem services.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2012

Impacts of ethanol fuel level on emissions of regulated and unregulated pollutants from a fleet of gasoline light-duty vehicles

The study investigated the impact of ethanol blends on criteria emissions (THC, NMHC, CO, NOx), greenhouse gas (CO2), and a suite of unregulated pollutants in a fleet of gasoline-powered light-duty vehicles. The vehicles ranged in model year from 1984 to 2007 and included one Flexible Fuel Vehicle (FFV). Emission and fuel consumption measurements were performed in duplicate or triplicate over the Federal Test Procedure (FTP) driving cycle using a chassis dynamometer for four fuels in each of seven vehicles. The test fuels included a CARB phase 2 certification fuel with 11% MTBE content, a CARB phase 3 certification fuel with a 5.7% ethanol content, and E10, E20, E50, and E85 fuels. In most cases, THC and NMHC emissions were lower with the ethanol blends, while the use of E85 resulted in increases of THC and NMHC for the FFV. CO emissions were lower with ethanol blends for all vehicles and significantly decreased for earlier model vehicles. Results for NOx emissions were mixed, with some older vehicles showing increases with increasing ethanol level, while other vehicles showed either no impact or a slight, but not statistically significant, decrease. CO2 emissions did not show any significant trends. Fuel economy showed decreasing trends with increasing ethanol content in later model vehicles. There was also a consistent trend of increasing acetaldehyde emissions with increasing ethanol level, but other carbonyls did not show strong trends. The use of E85 resulted in significantly higher formaldehyde and acetaldehyde emissions than the specification fuels or other ethanol blends. BTEX and 1,3-butadiene emissions were lower with ethanol blends compared to the CARB 2 fuel, and were almost undetectable from the E85 fuel. The largest contribution to total carbonyls and other toxics was during the cold-start phase of FTP.

02 PETROLEUM↗

DOE OSTI2013

Tunable upconversion emission in Ba{sub 2}YF{sub 7}:Yb{sup 3+}/Er{sup 3+} nanocrystals with different Yb{sup 3+} concentration

Graphical abstract: The emission intensity at 520 nm and 540 nm can be tuned by Yb{sup 3+} concentration. - Highlights: • High concentration of Yb{sup 3+} can be doped into Ba{sub 2}YF{sub 7} without a phase change. • The emission intensity at 520 nm and 540 nm can be tuned by Yb{sup 3+} concentration. • The long lifetime of {sup 4}F{sub 9/2} level makes its populating effective. - Abstract: Ba{sub 2}YF{sub 7}:xYb{sup 3+},0.02Er{sup 3+} nanocrystals with different Yb{sup 3+} concentration (x = 0.2, 0.4, 0.6, 0.8, 0.98) were synthesized via a solvothermal method. Their X-ray diffraction patterns reveal that all the samples are cubic phase without phase change at arbitrary Yb{sup 3+} concentration. Upon excitation of 980 nm laser, these nanocrystals display upconversion emission in the green and red spectral regions. The relative emission intensity at these two regions can be tuned by Yb{sup 3+} concentration. To investigate the effect of Yb{sup 3+} ion, the decay times of 650 nm emission were measured and analyzed. Ba{sub 2}YF{sub 7}:0.6Yb{sup 3+},0.02Er{sup 3+} nanocrystals have the longest lifetime and highest emission intensity among all the samples. We concluded the lifetime of {sup 4}F{sub 9/2} level has an effect on its own population and intensity ratio of red and green emission. Our results show Yb{sup 3+} ion can tune the upconversion emission and improve upconverison emission intensity.

36 MATERIALS SCIENCE↗

DOE OSTI2025

How demand for and trade of construction materials affects greenhouse gas emissions

Construction materials generate nearly one-third of global carbon emissions, yet conventional accounting captures only a fraction of this impact. Using EXIOBASE data spanning 25 years, we tracked emissions across construction supply chains for cement, steel, metals, and plastics. While global construction demand nearly tripled, regional patterns diverged significantly. The EU reduced emissions despite increased demand through renewable energy adoption and emissions trading, while China's construction boom—driving most global growth—significantly increased domestic emissions. Manufacturing contributes most to embodied emissions compared to resource extraction and waste treatment. Increased reliance on offshore production undermines domestic emission control strategies, highlighting the need for expanded carbon border adjustment mechanisms. Without policies addressing full supply chain emissions, even aggressive climate initiatives will be compromised by carbon leakage, creating an emissions trajectory incompatible with global climate targets.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2013

Emissions from US waste collection vehicles

Highlights: ► Life-cycle emissions for alternative fuel technologies. ► Fuel consumption of alternative fuels for waste collection vehicles. ► Actual driving cycle of waste collection vehicles. ► Diesel-fueled waste collection vehicle emissions. - Abstract: This research is an in-depth environmental analysis of potential alternative fuel technologies for waste collection vehicles. Life-cycle emissions, cost, fuel and energy consumption were evaluated for a wide range of fossil and bio-fuel technologies. Emission factors were calculated for a typical waste collection driving cycle as well as constant speed. In brief, natural gas waste collection vehicles (compressed and liquid) fueled with North-American natural gas had 6–10% higher well-to-wheel (WTW) greenhouse gas (GHG) emissions relative to diesel-fueled vehicles; however the pump-to-wheel (PTW) GHG emissions of natural gas waste collection vehicles averaged 6% less than diesel-fueled vehicles. Landfill gas had about 80% lower WTW GHG emissions relative to diesel. Biodiesel waste collection vehicles had between 12% and 75% lower WTW GHG emissions relative to diesel depending on the fuel source and the blend. In 2011, natural gas waste collection vehicles had the lowest fuel cost per collection vehicle kilometer travel. Finally, the actual driving cycle of waste collection vehicles consists of repetitive stops and starts during waste collection; this generates more emissions than constant speed driving.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2014

Greenhouse gas emissions from landfill leachate treatment plants: A comparison of young and aged landfill

Highlights: • Young and aged leachate works accounted for 89.1% and 10.9% of 33.35 Gg CO{sub 2} yr{sup −1}. • Fresh leachate owned extremely low ORP and high organic matter content. • Strong CH{sub 4} emissions occurred in the fresh leachate ponds, but small in the aged. • N{sub 2}O emissions became dominant in the treatment units of both systems. • 8.45–11.9% of nitrogen was removed as the form of N{sub 2}O under steady-state. - Abstract: With limited assessment, leachate treatment of a specified landfill is considered to be a significant source of greenhouse gas (GHG) emissions. In our study, the cumulative GHG emitted from the storage ponds and process configurations that manage fresh or aged landfill leachate were investigated. Our results showed that strong CH{sub 4} emissions were observed from the fresh leachate storage pond, with the fluxes values (2219–26,489 mg C m{sup −2} h{sup −1}) extremely higher than those of N{sub 2}O (0.028–0.41 mg N m{sup −2} h{sup −1}). In contrast, the emission values for both CH{sub 4} and N{sub 2}O were low for the aged leachate tank. N{sub 2}O emissions became dominant once the leachate entered the treatment plants of both systems, accounting for 8–12% of the removal of N-species gases. Per capita, the N{sub 2}O emission based on both leachate treatment systems was estimated to be 7.99 g N{sub 2}O–N capita{sup −1} yr{sup −1}. An increase of 80% in N{sub 2}O emissions was observed when the bioreactor pH decreased by approximately 1 pH unit. The vast majority of carbon was removed in the form of CO{sub 2}, with a small portion as CH{sub 4} (<0.3%) during both treatment processes. The cumulative GHG emissions for fresh leachate storage ponds, fresh leachate treatment system and aged leachate treatment system were 19.10, 10.62 and 3.63 Gg CO{sub 2} eq yr{sup −1}, respectively, for a total that could be transformed to 9.09 kg CO{sub 2} eq capita{sup −1} yr{sup −1}.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2012

Effects of Gasoline Direct Injection Engine Operating Parameters on Particle Number Emissions

A single-cylinder, wall-guided, spark ignition direct injection engine was used to study the impact of engine operating parameters on engine-out particle number (PN) emissions. Experiments were conducted with certification gasoline and a splash blend of 20% fuel grade ethanol in gasoline (E20), at four steady-state engine operating conditions. Independent engine control parameter sweeps were conducted including start of injection, injection pressure, spark timing, exhaust cam phasing, intake cam phasing, and air-fuel ratio. The results show that fuel injection timing is the dominant factor impacting PN emissions from this wall-guided gasoline direct injection engine. The major factor causing high PN emissions is fuel liquid impingement on the piston bowl. By avoiding fuel impingement, more than an order of magnitude reduction in PN emission was observed. Increasing fuel injection pressure reduces PN emissions because of smaller fuel droplet size and faster fuel-air mixing. PN emissions are insensitive to cam phasing and spark timing, especially at high engine load. Cold engine conditions produce higher PN emissions than hot engine conditions due to slower fuel vaporization and thus less fuel-air homogeneity during the combustion process. E20 produces lower PN emissions at low and medium loads if fuel liquid impingement on piston bowl is avoided. At high load or if there is fuel liquid impingement on piston bowl and/or cylinder wall, E20 tends to produce higher PN emissions. This is probably a function of the higher heat of vaporization of ethanol, which slows the vaporization of other fuel components from surfaces and may create local fuel-rich combustion or even pool-fires.

02 PETROLEUM↗

DOE OSTI2021

Experimental Soil Warming and Permafrost Thaw Increase CH 4 Emissions in an Upland Tundra Ecosystem

Rapid Arctic warming is causing permafrost to thaw and exposing large quantities of soil organic carbon (C) to potential decomposition. In dry upland tundra systems, subsidence from thawing permafrost can increase surface soil moisture resulting in higher methane (CH 4 ) emissions from newly waterlogged soils. The proportion of C released as carbon dioxide (CO 2 ) and CH 4 remains uncertain as previously dry landscapes transition to a thawed state, resulting in both wetter and drier microsites. To address how thaw and moisture interact to affect total C emissions, here we measured CH 4 and CO 2 emissions from paired chambers across thaw and moisture gradients created by nine years of experimental soil warming in interior Alaska. Cumulative growing season (May–September) CH 4 emissions were elevated at both wetter (216.1–1,099.4 mg CH 4 -C m –2 ) and drier (129.7–392.3 mg CH 4 -C m –2 ) deeply thawed microsites relative to shallow thaw (55.6–215.7 mg CH 4 -C m –2 ) and increased with higher deep soil temperatures and permafrost thaw depth. Interannual variability in CH4 emissions was driven by wet conditions in graminoid-dominated plots that generated >70% of emissions in a wet year. Shoulder season emissions were equivalent to growing season CH 4 emissions rates in the deeply thawed, warmed soils, highlighting the importance of non-growing season CH 4 emissions. Net C sink potential was reduced in deeply thawed wet plots by 4%–42%, and by 3.5%–8% in deeply thawed drier plots due to anaerobic respiration, suggesting that some dry upland tundra landscapes may transition into stronger CH 4 sources in a warming Arctic.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Projection of Future Fire Emissions Over the Contiguous US Using Explainable Artificial Intelligence and CMIP6 Models

Abstract Increasing temperature and water cycle changes due to warming climate may increase the frequency and intensity of wildfires. Fire emission projections are useful for informing strategies for adaptation and mitigation of fire impacts on societies and ecosystems. Here, we construct a neural network (NN) model explained by the Shapley Additive explanation to predict fire PM 2.5 emissions change and understand their drivers over the contiguous US (CONUS) in the mid‐21st century under a high greenhouse gas emissions scenario (SSP5‐8.5). Using future meteorology and leaf area index (LAI) simulated by eight global climate models from the Coupled Model Intercomparison Project Phase 6, future population density, and present‐day land use and land cover (LULC) as input to the NN model, the total fire PM 2.5 emissions over CONUS are projected to increase by 4%–75% (model spread). Among different regions, fire emissions in the western US are projected to increase more significantly in June‐July‐August than in other seasons and regions, with the median ratios of future to present‐day fire emissions ranging from 1.67 to 2.86. The increases in fire emissions are mainly driven by increasing normalized temperature (23%–29%) and decreasing soil moisture (2%–10%) in the future. When future LULC change is considered, the projected fire emissions further increase by 58%–83% over the western US compared to projections without LULC change because of future increases in vegetation fraction. The results highlight the important role of warmer temperature, decreasing soil moisture, and LULC change in increasing fire emissions in the future.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2014

Planck 2013 results. XIV. Zodiacal emission

The Planck satellite provides a set of all-sky maps at nine frequencies from 30GHz to 857GHz. Planets, minor bodies, and diffuse interplanetary dust emission (IPD) are all observed. The IPD can be separated from Galactic and other emissions because Planck views a given point on the celestial sphere multiple times, through different columns of IPD. We use the Planck data to investigate the behaviour of zodiacal emission over the whole sky at sub-millimetre and millimetre wavelengths. We fit the Planck data to find the emissivities of the various components of the COBE zodiacal model-a diffuse cloud, three asteroidal dust bands, a circumsolar ring, and an Earth-trailing feature. The emissivity of the diffuse cloud decreases with increasing wavelength, as expected from earlier analyses. The emissivities of the dust bands, however, decrease less rapidly, indicating that the properties of the grains in the bands are different from those in the diffuse cloud. We fit the small amount of Galactic emission seen through the telescope's far sidelobes, and place limits on possible contamination of the cosmic microwave background (CMB) results from both zodiacal and far-sidelobe emission. When necessary, the results are used in the Planck pipeline to make maps with zodiacal emission and far sidelobes removed. We show that the zodiacal correction to the CMB maps is small compared to the Planck CMB temperature power spectrum and give a list of flux densities for small solar system bodies.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Hunting for gamma-ray emission from fast radio bursts

Context. Fast radio bursts (FRBs) are a recently discovered class of GHz-band, ms-duration, Jansky-level-flux astrophysical transients. Although hundreds of models have been proposed so far for FRB progenitors (the most popular ones involve magnetars), their physical origin and emission mechanism are still a mystery, making them one of the most compelling problems in astrophysics. Aims. FRBs are caused by astrophysical processes that are not yet understood. Exploring their high-energy counterpart is crucial for constraining their origin and emission mechanism. Methods. Thanks to more than 13 years of gamma-ray data collected by the Large Area Telescope on board the Fermi Gamma-ray Space Telescope, and to more than 1000 FRB events (from 561 non-repeating and 22 repeating sources), one of the largest samples created thus far, we performed the largest and deepest search for high-energy emission from FRB sources to date (between 100 MeV and 1 TeV). In addition to the analysis involving individual FRB events on different timescales (from a few seconds up to several years), we performed, for the first time, a stacking analysis on the full sample of FRB events as well as a search for triplet photons in coincidence with the radio event. Results. We do not detect significant emission, reporting the most stringent constraints, on short timescales, for the FRB-like emission from SGR 1935+2154 with E γ <10 41 erg, corresponding to a factor η < 10 7 with respect to the emitted radio energy. Similarly, for the stacked signal of steady emission from all repeaters, the obtained upper limit (UL) on the FRBs luminosity (L γ < 1.6 × 10 43 erg s -1 is more than two orders of magnitude lower than those derived from the individual sources. Finally, no individual or triplet photons have been significantly associated with FRB events. We derived the LAT ms-sensitivity to be ~0.3 ph cm -2 s -1 and constrained the gamma-ray energy E γ,δT = 1 ms ≲ 10 47 (D L /150 Mpc) 2 erg, ruling out a gamma-ray-to-radio energy ratio greater than 10 9 on ms timescales. Conclusions. The results reported here represent the most stringent UL reported so far on the high-energy emission from FRBs on short and long time scales, as well as on cumulative emission and individual photon searches. While the origin of FRBs is still unclear, our work provides important constraints for FRB modelling, which might shed light on their emission mechanism.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2014

Intervalence charge transfer luminescence: Interplay between anomalous and 5d − 4f emissions in Yb-doped fluorite-type crystals

In this paper, we report the existence of intervalence charge transfer (IVCT) luminescence in Yb-doped fluorite-type crystals associated with Yb{sup 2+}–Yb{sup 3+} mixed valence pairs. By means of embedded cluster, wave function theory ab initio calculations, we show that the widely studied, very broad band, anomalous emission of Yb{sup 2+}-doped CaF{sub 2} and SrF{sub 2}, usually associated with impurity-trapped excitons, is, rather, an IVCT luminescence associated with Yb{sup 2+}–Yb{sup 3+} mixed valence pairs. The IVCT luminescence is very efficiently excited by a two-photon upconversion mechanism where each photon provokes the same strong 4f{sup 14}–1A{sub 1g}→ 4f{sup 13}({sup 2}F{sub 7/2})5de{sub g}–1T{sub 1u} absorption in the Yb{sup 2+} part of the pair: the first one, from the pair ground state; the second one, from an excited state of the pair whose Yb{sup 3+} moiety is in the higher 4f{sup 13}({sup 2}F{sub 5/2}) multiplet. The Yb{sup 2+}–Yb{sup 3+} → Yb{sup 3+}–Yb{sup 2+} IVCT emission consists of an Yb{sup 2+} 5de{sub g} → Yb{sup 3+} 4f{sub 7/2} charge transfer accompanied by a 4f{sub 7/2} → 4f{sub 5/2} deexcitation within the Yb{sup 2+} 4f{sup 13} subshell: [{sup 2}F{sub 5/2}5de{sub g},{sup 2}F{sub 7/2}] → [{sup 2}F{sub 7/2},4f{sup 14}]. The IVCT vertical transition leaves the oxidized and reduced moieties of the pair after electron transfer very far from their equilibrium structures; this explains the unexpectedly large band width of the emission band and its low peak energy, because the large reorganization energies are subtracted from the normal emission. The IVCT energy diagrams resulting from the quantum mechanical calculations explain the different luminescent properties of Yb-doped CaF{sub 2}, SrF{sub 2}, BaF{sub 2}, and SrCl{sub 2}: the presence of IVCT luminescence in Yb-doped CaF{sub 2} and SrF{sub 2}; its coexistence with regular 5d-4f emission in SrF{sub 2}; its absence in BaF{sub 2} and SrCl{sub 2}; the quenching of all emissions in BaF{sub 2}; and the presence of additional 5d–4f emissions in SrCl{sub 2} which are absent in SrF{sub 2}. They also allow to interpret and reproduce recent experiments on transient photoluminescence enhancement in Yb{sup 2+}-doped CaF{sub 2} and SrF{sub 2}, the appearance of Yb{sup 2+} 4f–5d absorption bands in the excitation spectra of the IR Yb{sup 3+} emission in partly reduced CaF{sub 2}:Yb{sup 3+} samples, and to identify the broadband observed in the excitation spectrum of the so far called anomalous emission of SrF{sub 2}:Yb{sup 2+} as an IVCT absorption, which corresponds to an Yb{sup 2+} 4f{sub 5/2} → Yb{sup 3+} 4f{sub 7/2} electron transfer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2011

A DEEP CHANDRA ACIS STUDY OF NGC 4151. III. THE LINE EMISSION AND SPECTRAL ANALYSIS OF THE IONIZATION CONE

This paper is the third in a series in which we present deep Chandra ACIS-S imaging spectroscopy of the Seyfert 1 galaxy NGC 4151, devoted to study its complex circumnuclear X-ray emission. Emission features in the soft X-ray spectrum of the bright extended emission (L{sub 0.3-2{sub keV}} {approx} 10{sup 40} erg s{sup -1}) at r > 130 pc (2'') are consistent with blended brighter O VII, O VIII, and Ne IX lines seen in the Chandra HETGS and XMM-Newton RGS spectra below 2 keV. We construct emission line images of these features and find good morphological correlations with the narrow-line region clouds mapped in [O III] {lambda}5007. Self-consistent photoionization models provide good descriptions of the spectra of the large-scale emission, as well as resolved structures, supporting the dominant role of nuclear photoionization, although displacement of optical and X-ray features implies a more complex medium. Collisionally ionized emission is estimated to be {approx}<12% of the extended emission. Presence of both low- and high-ionization spectral components and extended emission in the X-ray image perpendicular to the bicone indicates leakage of nuclear ionization, likely filtered through warm absorbers, instead of being blocked by a continuous obscuring torus. The ratios of [O III]/soft X-ray flux are approximately constant ({approx}15) for the 1.5 kpc radius spanned by these measurements, indicating similar relative contributions from the low- and high-ionization gas phases at different radial distances from the nucleus. If the [O III] and X-ray emission arise from a single photoionized medium, this further implies an outflow with a wind-like density profile. Using spatially resolved X-ray features, we estimate that the mass outflow rate in NGC 4151 is {approx}2 M{sub Sun} yr{sup -1} at 130 pc and the kinematic power of the ionized outflow is 1.7 Multiplication-Sign 10{sup 41} erg s{sup -1}, approximately 0.3% of the bolometric luminosity of the active nucleus in NGC 4151.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Tomographic optical emission spectroscopy of an atmospheric pressure plasma jet and surface ionization waves on planar and structured surfaces

Here in this paper, an approach for 3D plasma structure diagnostics using tomographic optical emission spectroscopy (Tomo-OES) of a nanosecond pulsed atmospheric pressure plasma jet (APPJ) is presented. In contrast to the well-known Abel inversion, Tomo-OES does not require cylindrical symmetry to recover 3D distributions of plasma light emission. Instead, many 2D angular projections are measured with intensified cameras and the multiplicative algebraic reconstruction technique is used to recover the 3D distribution of light emission. This approach solves the line-of-sight integration problem inherent to optical diagnostics, allowing recovery of localized OES information within the plasma that can be used to better infer plasma parameters within complex plasma structures. Here, Tomo-OES was applied to investigate an APPJ operated with helium in ambient air and impinging on planar and structured dielectric surfaces. Surface charging caused the guided streamer from the APPJ to transition to a surface ionization wave (SIW) that propagated along the surface. The SIW experienced variable geometrical and electrical material properties as it propagated, leading to 3D configurations that were non-symmetric and spatially complex. Light emission from He, N$_2^+$, and N2 were imaged at ten angular projections and the respective time-resolved 3D emission distributions in the plasma were then reconstructed. The spatial resolution of each tomographic reconstruction was 7.4 µm and the temporal resolution was 5 ns, sufficient to observe the guided streamer and the effects of the structured surface on the SIW. Emission from He showed the core of the jet and emission from N$_2^+$ and N2 indicated effects of entrainment of ambient air. Penning ionization of N2 created a ring or outer layer of N$_2^+$ that spatially converged to form the 'plasma bullet' or spatially diverged across a surface as part of a SIW. The SIW entered trenches of size 150 µm, leading to decreases in plasma light emission in regions above the trenches. The plasma light emission was higher in some regions with trenches, possibly due to effects of field enhancement.

plasma interactions with complex surfaces↗