Results for “fundamental parameters” — Page 70

NASA NTRS1991

Herman-Wallis factors in the C2H2nu5 infrared fundamental near 14 microns

The presence of acetylene has been confirmed for some time in the atmospheres of the outer planets Jupiter, Saturn, Neptune, and Saturn's satellite Titan. For these atmospheres, the determination of C2H2 abundances using its strong nu5 fundamental requires laboratory line position and intensity measurements. The 1-m Fourier transform spectrometer at McMath solar telescope of Kitt Peak National Observatory was used to measure C2H2 at an unapodized spectral resolution of 0.0025/cm. Synthetic spectra are generated by convolving a Voigt line shape with an instrument function and varying intensity parameters by means of a nonlinear least squares technique. Intensities of 37 nu5 lines spanning P18 through R20 were measured using 0.123 torr of gas in a 1-cm cell. A Herman-Wallis intensity correction parameter of 1.3(4) x 10 to the -3rd has been derived using a least squares linear fit.

Maguire, William C.↗

NASA NTRS2000

What Controls the Arctic Lower Stratosphere Temperature?

The temperature of the Arctic lower stratosphere is critical for understanding polar ozone levels. As temperatures drop below about 195 K, polar stratospheric clouds form, which then convert HCl and ClONO2 into reactive forms that are catalysts for ozone loss reactions. Hence, the lower stratospheric temperature during the March period is a key parameter for understanding polar ozone losses. The temperature is basically understood to be a result of planetary waves which drive the polar temperature away from a cold "radiative equilibrium" state. This is demonstrated using NCEP/NCAR reanalysis calculations of the heat flux and the mean polar temperature. The temperature during the March period is fundamentally driven by the integrated impact of large scale waves moving from the troposphere to the stratosphere during the January through February period.

Newman, Paul A.↗

NASA NTRS2001

What Controls the Arctic Lower Stratosphere Temperature?

The temperature of the Arctic lower stratosphere is critical for understanding polar ozone levels. As temperatures drop below about 195 K, polar stratospheric clouds form, which then convert HCl and ClONO2 into reactive forms that are catalysts for ozone loss reactions. Hence, the lower stratospheric temperature during the March period is a key parameter for understanding polar ozone losses. The temperature is basically understood to be a result of planetary waves which drive the polar temperature away from a cold "radiative equilibrium" state. This is demonstrated using NCEP/NCAR reanalysis calculations of the heat flux and the mean polar temperature. The temperature during the March period is fundamentally driven by the integrated impact of large scale waves moving from the troposphere to the stratosphere during the January through February period. We will further show that the recent cold years in the northern polar vortex are a result of this weakened wave driving of the stratosphere.

Newman, Paul A.↗

NASA NTRS1992

Status of the Validation of High-Angle-Of-Attack Nose-Down Pitch Control Margin Design Guidelines

This paper presents a summary of results obtained to date in an ongoing cooperative research program between NASA and the U.S. Navy to develop design criteria for high-angle-of-attack nose- down pitch control for combat aircraft. A fundamental design consideration for aircraft incorporating relaxed static stability in pitch is the level of stability which achieves a proper balance between high- speed performance considerations and low-speed requirements for maneuvering at high angles of attack. A comprehensive data base of piloted simulation results was generated for parametric variations of critical parameters affecting nose-down control capability. The results showed a strong correlation of pilot rating to the short-term pitch response for nose-down commands applied at high- angle-of-attack conditions. Using these data, candidate design guidelines and flight demonstration requirements were defined. Full- scale flight testing to validate the research methodology and proposed guidelines is in progress, some preliminary results of which are reviewed.

Ogburn, Marilyn E.↗

NASA NTRS2010

The Smallest Lunar Grains: Analytical TEM Characterization of the Sub-micron Size Fraction of a Mare Soil

The chemical composition, mineralogical type, and morphology of lunar regolith grains changes considerably with decreasing size, and below the approx.25 m size range the correlation between these parameters and remotely-sensed lunar surface properties connected to space weathering increases significantly. Although trends for these parameters across grain size intervals greater than 20 m are now well established, the 0 to 20 m size interval remains relatively un-subdivided with respect to variations in grain modal composition, chemistry and microstructure. Of particular interest in this size range are grains in the approximate < 1 m diameter class, whose fundamental properties are now the focus of lunar research pertaining to electrostatic grain transport, dusty plasmas, and lunar dust effects on crew health and exploration systems. In this study we have used analytical transmission electron microscopy (TEM) to characterize the mineralogy, microstructure and major element composition of grains below the 1 m size threshold in lunar soil 10084.

Thompson, M.↗

NASA NTRS2011

The Effects of Ambient Conditions on Helicopter Rotor Source Noise Modeling

A new physics-based method called Fundamental Rotorcraft Acoustic Modeling from Experiments (FRAME) is used to demonstrate the change in rotor harmonic noise of a helicopter operating at different ambient conditions. FRAME is based upon a non-dimensional representation of the governing acoustic and performance equations of a single rotor helicopter. Measured external noise is used together with parameter identification techniques to develop a model of helicopter external noise that is a hybrid between theory and experiment. The FRAME method is used to evaluate the main rotor harmonic noise of a Bell 206B3 helicopter operating at different altitudes. The variation with altitude of Blade-Vortex Interaction (BVI) noise, known to be a strong function of the helicopter s advance ratio, is dependent upon which definition of airspeed is flown by the pilot. If normal flight procedures are followed and indicated airspeed (IAS) is held constant, the true airspeed (TAS) of the helicopter increases with altitude. This causes an increase in advance ratio and a decrease in the speed of sound which results in large changes to BVI noise levels. Results also show that thickness noise on this helicopter becomes more intense at high altitudes where advancing tip Mach number increases because the speed of sound is decreasing and advance ratio increasing for the same indicated airspeed. These results suggest that existing measurement-based empirically derived helicopter rotor noise source models may give incorrect noise estimates when they are used at conditions where data were not measured and may need to be corrected for mission land-use planning purposes.

Schmitz, Frederic H.↗

DOE OSTI2024

An Integrated Electrochemical Approach to the Precision Synthesis of Sustainable Catalyst Materials

There is a pressing need to replace critical materials such as platinum group elements (PGE) in applications related to energy. This work responds to the need for fundamental principles of materials design to replace these metals by addressing a gap in the understanding of how to precisely control the surface structure of nanoscale materials. Electrochemical nanomaterials synthesis, such as techniques developed in the PI’s research group, expands the toolbox of available synthetic handles to include both electrochemical and chemical parameters, providing access to control over synthetic conditions in ways that are not possible in purely chemical nanoparticle growth. However, electrochemical materials synthesis (electrodeposition) is inherently serial, limiting throughput and preventing widespread implementation. Initial efforts in the short period of this award resulted in an innovative, high throughput, parallel approach to synthetic discovery for the electrodeposition of shaped metal nanoparticles that overcomes this limitation. Looking ahead, this work establishes an important capability that will enable researchers to push boundaries in the shape control of nanoparticles composed of non-PGE such as copper, iron, nickel, or cobalt.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Stable Thermotropic 3D and 2D Double Gyroid Nanostructures with Sub-2-nm Feature Size from Scalable Sugar–Polyolefin Conjugates

In this study, ultra-low molecular weight disaccharide–polyolefin conjugates with cellobiose, lactose and maltose head groups and atactic polypropene tails, such as 1, undergo a series of irreversible thermotropic order–order transitions with increasing temperature to provide nanostructured phases in the sequence: lamellar (L), hexagonal perforated lamellar (HPL), double gyroid (DG) and hexagonal cylindrical (C). The DG phase displays exceptional stability at ambient temperature and features two interpenetrating sugar domain networks having a sub-2-nm strut width and a lattice parameter, a DG , of 13.1 nm. The unique stability of this DG phase extends further within ultrathin films all the way down to the two-dimensional limit of 15 nm in which film thickness, l, is now less than the surface-oriented unit cell height, h DG . In addition to raising the fundamental question of what minimally constitutes a Schoen triply periodic minimal surface and DG lattice, these results serve to establish the class of sugar–polyolefin conjugates as a new material platform for nanoscience and nanotechnology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Non-standard neutrino interactions mediated by a light scalar at DUNE

Abstract We investigate the effect on neutrino oscillations generated by beyond-the-standard-model interactions between neutrinos and matter. Specifically, we focus on scalar-mediated non-standard interactions (NSI) whose impact fundamentally differs from that of vector-mediated NSI. Scalar NSI contribute as corrections to the neutrino mass matrix rather than the matter potential and thereby predict distinct phenomenology from the vector-mediated ones. Similar to vector-type NSI, the presence of scalar-mediated neutrino NSI can influence measurements of oscillation parameters in long-baseline neutrino oscillation experiments, with a notable impact on CP measurement in the case of DUNE. Our study focuses on the effect of scalar NSI on neutrino oscillations, using DUNE as an example. We introduce a model-independent parameterization procedure that enables the examination of the impact of all non-zero scalar NSI parameters simultaneously. Subsequently, we convert DUNE’s sensitivity to the NSI parameters into projected sensitivity concerning the parameters of a light scalar model. We compare these results with existing non-oscillation probes. Our findings reveal that the region of the light scalar parameter space sensitive to DUNE is predominantly excluded by non-oscillation probes, especially when considering all nonzero parameters simultaneously for DUNE.

Physics↗

DOE OSTI2022

Dynamical Study of Adsorbate-Induced Restructuring Kinetics in Bimetallic Catalysts Using the PdAu(111) Model System

The dynamic restructuring of bimetallic catalysts plays a crucial role in their catalytic activity and selectivity. In particular, catalyst pretreatment with species such as carbon monoxide and oxygen has been shown to be an effective strategy for tuning the surface composition and morphology. Mechanistic and kinetic understanding of such restructuring are fundamental to the chemistry and engineering of surface active sites but have remained challenging due to the large structural, chemical, and temporal degrees of freedom. Here, we combine time-resolved temperature-programmed infrared reflection absorption spectroscopy, ab initio thermodynamics, and machine-learning molecular dynamics to uncover previously unidentified timescale and kinetic parameters of in situ restructuring in Pd/Au(111), a highly relevant model system for dilute Pd-in-Au nanoparticle catalysts. The key innovation lies in utilizing CO not only as a chemically sensitive probe of surface Pd, but also as an agent that induces restructuring of the surface. Upon annealing in vacuum, as-deposited Pd islands became encapsulated by Au and partially dissolved into the subsurface, leaving behind isolated Pd monomers on the surface. Subsequent exposure to 0.1 mbar CO enabled Pd monomers to repopulate the surface up to 373 K, above which complete Pd dissolution occurred by 473 K, with apparent activation energies of 0.14 and 0.48 eV, respectively. Furthermore, these restructuring processes occurred over the span of ~1000 s at a given temperature. Such a minute-timescale dynamics not only elucidates the fluxional nature of alloy catalysts but also presents an opportunity to fine-tune the surface at moderate temperature and pressure conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Controlling product selectivity in hybrid gas/liquid reactors using gas conditions, voltage, and temperature

For the conversion of CO 2 into fuels and chemical feedstocks, hybrid gas/liquid-fed electrochemical flow reactors provide advantages in selectivity and production rates over traditional liquid phase reactors. However, fundamental questions remain about how to optimize conditions to produce desired products. Here, using an alkaline electrolyte to suppress hydrogen formation and a gas diffusion electrode catalyst composed of copper nanoparticles on carbon nanospikes, we investigate how hydrocarbon product selectivity in the CO 2 reduction reaction in hybrid reactors depends on three experimentally controllable parameters: (1) supply of dry or humidified CO 2 gas, (2) applied potential, and (3) electrolyte temperature. Changing from dry to humidified CO 2 dramatically alters product selectivity from C 2 products ethanol and acetic acid to ethylene and C 1 products formic acid and methane. Water vapor evidently influences product selectivity of reactions that occur on the gas-facing side of the catalyst by adding a source of protons that alters reaction pathways and intermediates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Plasma diagnostics and modeling of lithium-containing plasmas

Thin-film deposition from chemically reactive multi-component plasmas is complex, and the lack of electron collision cross-sections for even the most common metalorganic precursors and their fragments complicates their modeling based on fundamental plasma physics. This study focuses on understanding the plasma physics and chemistry in argon (Ar) plasmas containing lithium bis (trimethylsilyl) amide used to deposit Li x Si y thin films. These films are emerging as potential solid electrolytes for lithium-ion batteries, and the Li-to-Si ratio is a crucial parameter to enhance their ionic conductivity. We deposited Li x Si y films in an axial flow-through plasma reactor and studied the factors that determine the variation of the Li-to-Si ratio in films deposited at various points on a substrate spanning the entire reactor axis. While the Li-to-Si ratio is 1:2 in the precursor, the Li-to-Si ratio is as high as 3:1 in films deposited near the plasma entrance and decreases to 1:1 for films deposited downstream. Optical emission from the plasma is dominated by Li emission near the entrance, but Li emission disappears downstream, which we attribute to the complete consumption of the precursor. We hypothesized that the axially decreasing precursor concentration affects the electron energy distribution function in a way that causes different dissociation efficiencies for the production of Li and Si. We used Li line intensities to estimate the local precursor concentration and Ar line ratios to estimate the local reduced electric field to test this hypothesis. This analysis suggests that the mean electron energy increases along the reactor axis with decreasing precursor concentration. As a result, the decreasing Li-to-Si ratio with axially decreasing precursor concentration may be explained by Li release from the precursor having lower threshold energy than Si release.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Understanding detachment of the W7-X island divertor

The fundamental behavior of the W7-X island divertor under detached conditions, which has been theoretically predicted with the EMC3-Eirene code, is re-examined here under the experimental conditions achieved so far and compared with the first experimental results. Both simulations and experiments cover a range of divertor configurations and plasma parameters, and show the following common trends: (1) with rising impurity radiation, the target heat load decreases 'uniformly' over the entire target surface in the sense that both the peak and average heat loads can drop by an order of magnitude. Impurity radiation (mainly from intrinsic carbon) occurs primarily at the plasma edge and the resulting negative impact on the stored energy is less than 10%. (2) When the total radiation exceeds a critical level, the target particle flux (the recycling flux Γrecy) begins to fall and can drop by a factor of 3–5 at high radiation levels without an obvious indication of significant volume recombination. (3) While Γ recy decreases, the divertor neutral pressure continues to build up and reaches a maximum, at which point Γ recy has declined significantly. (4) During detachment, the electron temperature at the last closed flux surface falls in a way that is not quantitatively understandable from parallel classical heat conduction processes. This paper presents a physical explanation of the numerical/experimental results described above. Furthermore, using the EMC3-Eirene code as a diagnostic tool, we are able, apparently for the first time, to provide a full quantitative analysis of each transport channel in the island divertor, aiming to clarify how the island divertor plasma self-regulates to maintain particle, energy, and momentum balance under detached conditions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS1988

Laser action in chromium-activated forsterite for near infrared excitation

This paper reports on laser action in chromium-doped forsterite (Cr:Mg2SiO4) for 1064-nm excitation of the crystal's double-hump absorption band spanning the 850-1200-nm wavelength range. The cavity arrangement used for obtaining laser action in Cr:Mg2SiO2 was similar to that described by Petricevic et al. (1988). The fundamental and second harmonic emissions from a Q-switched Nd:YAG laser operating at a 10-Hz repetition rate were used for excitation of the NIR and visible bands, respectively. Pulsed laser action was readily observed for both the 1064-nm and 532-nm pumping at or above the respective thresholds. The laser parameters of the 532-nm and 1064-nm excitations were similar, indicating that the IR band is responsible for laser action for both excitations.

Petricevic, V.↗

NASA NTRS1993

A photostationary state analysis of the NO2-NO system based on airborne observations from the subtropical/tropical North and South Atlantic

The Chemical Instrumentation Test and Evaluation 3 (CITE 3) NO-NO2 database has provided a unique opportunity to examine important aspects of tropospheric photochemistry as related to the rapid cycling between NO and NO2. Our results suggest that when quantitative testing of this photochemical system is based on airborne field data, extra precautions may need to be taken in the analysis. This was particularly true in the CITE 3 data analysis where different regional environments produced quite different results when evaluating the photochemical test ratio (NO2)(sub expt)/(NO2)(sub calc), designated here as R(sub E)/R(sub C). The quantity (NO2)(sub Calc) was evaluated using the following photostationary state expression: (NO2)(sub Calc) = k(sub 1)(O3) + k(sub 4)(HO2) + k(sub 5)(CH3O2) + k(sub 6)(RO2))(NO)(sub Expt)/J(sub 2). The four most prominent regional environmental data sets identified in this analysis were those labeled here as free-tropospheric northern hemisphere (FTNH), free-tropospheric tropical northern hemisphere (FTTNH), free-tropospheric southern hemisphere (FTSH), and tropical-marine boundary layer (plume) (TMBL(P)). The respective R(sub E)/R(sub C) mean and median values for these four data subsets were 1.74, 1.69; 3.00, 2.79; 1.01, 0.97; and 0.99, 0.94. Of the four data subsets listed, the two that were statistically the most robust were FTNH and FTSH; for these the respective R(sub E)/R(sub C) mean and standard deviation of the mean values were 1.74 +/- 0.07 and 1.01 +/- 0.04. The FTSH observations were in good agreement with theory, whereas those from the FTNH data set were in significant disagreement. An examination of the critical photochemical parameters O3, UV(zenith), NO, NO2, and non-methane hydrocarbons (NMHCs) for these two databases indicated that the most likely source of the R(sub E)/R(sub C) bias in the FTNH results was the presence of a systematic error in the observational data rather than a shortening in our understanding of fundamental photochemical processes. Although neither a chemical nor meteorological analyses of these data identified this error with complete certainty, they did point to the three most likely possibilities: (1) an NO2 interference from a yet unidentified NO(y) species: (2) the presence of unmeasured hydrocarbons, the integrated reactivity of which would be equivalent to approximately 2.7 parts per billion by volume (ppbv) of toluene; or (3) some combination of points (1) and (2). Details concerning hypotheses (1) and (2) as well as possible ways to minimize these problems in future airborne missions are discussed.

Davis, D. D.↗

DOE OSTI2021

Advanced Fuels Campaign Execution Plan

The Advanced Fuels Campaign (AFC) Execution Plan outlines the strategy, mission, scope, near-term and long-term goals, structure, and organization associated with nuclear fuels and materials research, development, and demonstration activities within the Department of Energy’s (DOE) Nuclear Fuel Cycle and Supply Chain (NFCSC) program. NFCSC has been given responsibility to identify and mature advanced fuel technologies for the DOE using a science-based approach, focused on developing a fundamental understanding of nuclear fuels and materials to drive development of integrated nuclear fuel and materials technology. This science-based approach combines theory, experiments, and multiscale modeling and simulation to achieve a predictive understanding of relevant behaviors ranging from fuel fabrication processes (and their resulting fuel microstructures) through fuel/cladding performance under irradiation (in contrast to more empirical, observation-based approaches frequently used in fuel performance modeling and fuel qualification). The traditional scope of AFC includes the evaluation and development of multiple fuel forms to support two fuel cycle options: once-through and full recycle. The word “fuel” is used generically to include conventional fuels, transmutation targets, and any associated cladding or duct materials. The once-through fuel cycle addresses advanced light water reactor fuels with enhanced performance, extended burnup, and reduced waste generation. In fiscal year (FY) 2012, AFC’s scope expanded to include research, development, and demonstration (RD&D) for light water reactor (LWR) fuels with enhanced accident tolerance. Fuel fabrication activities include the development of innovative methods to enhance process efficiencies, reduce waste, and improve control over as-fabricated fuel microstructural properties to achieve desired in-reactor performance. Using modern modeling and simulation approaches, the objective is to predict fresh fuel properties given the feedstock characteristics and fabrication process parameters. The performance-related activities include small-scale, in-reactor, and out-of-reactor phenomenological testing (distinct from, but synergistic with, integral prototypic testing) and extensive, quantitative characterization (focusing on characterization of fuel and cladding materials at the scale of microstructure) both before and after testing. Larger-scale, prototypic experiments are conducted in concert with phenomenological testing to drive a Fuel Development and Qualification program, incorporating a fundamental understanding of fuel behavior performance characteristics. Then, using the tools developed under the productive science-based approach, fuels will be optimized to meet specific performance requirements, thereby minimizing the need to repeatedly perform large-scale, integral experiments over a wide parametric range as a means of experimental exploration. Two significant initiatives are underway within AFC. First, a gap analysis completed in early FY 2019 identified critical irradiation testing needs that are lacking within the national light water reactor (LWR) fuels testbed since the shutdown of the Halden Reactor in 2018. The identified gaps are for instrumented, prototypic testing of LWR fuels, especially under boiling water reactor conditions, ramp conditions, and conditions leading to fuel failure; these needs exist for supporting current LWR fuels and their possible extension to higher burnups, but are especially urgent relative to near-term development and qualification of accident-tolerant fuels. Recommendations that resulted from the Halden Gap Analysis focused on enhancements at Advanced Test Reactor (ATR) and Transient Reactor Test Facility (TREAT) to fill gaps in testing capabilities relative to these needs. Second, a concerted effort to develop and demonstrate a systematic approach to accelerating the development, testing, and qualification of new fuel systems has been initiated. This is highlighted by a test strategy that combines the considerable advances in multiscale, mechanistic fuel modeling of recent years with a MiniFuel separate effects test program in the High Flux Isotope Reactor (HFIR) and a Fission Accelerated Steady-state Testing (FAST) semi-integral accelerated test program in ATR. This approach is being tested/demonstrated using the metallic fuel system, but if successful it is expected to be extensible to multiple fuel types and diverse applications. This document includes an overview of the NFCSC program, a definition of science-based development of nuclear fuels, near-term goals for Advanced LWR fuels (ALFs), and longer-term goals for Advanced Reactor Fuels (ARFs) RD&D. This includes the activities that will be conducted to achieve success toward the grand challenge, as well as the goals and milestones to be achieved over the next few decades of research and development. Long-term goals are based on the DOE Office of Nuclear Energ

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Advanced Fuels Campaign Execution Plan

The Advanced Fuels Campaign (AFC) Execution Plan outlines the strategy, mission, scope, near-term and long-term goals, structure, and organization associated with nuclear fuels and materials research, development, and demonstration activities within the Department of Energy’s (DOE) Nuclear Fuel Cycle and Supply Chain (NFCSC) program. NFCSC has been given responsibility to identify and mature advanced fuel technologies for the DOE using a science-based approach, focused on developing a fundamental understanding of nuclear fuels and materials to drive development of integrated nuclear fuel and materials technology. This science-based approach combines theory, experiments, and multiscale modeling and simulation to achieve a predictive understanding of relevant behaviors ranging from fuel fabrication processes (and their resulting fuel microstructures) through fuel/cladding performance under irradiation (in contrast to more empirical, observation-based approaches frequently used in fuel performance modeling and fuel qualification). The traditional scope of AFC includes the evaluation and development of multiple fuel forms to support two fuel cycle options: once-through and full recycle. The word “fuel” is used generically to include conventional fuels, transmutation targets, and any associated cladding or duct materials. The once-through fuel cycle addresses advanced light water reactor fuels with enhanced performance, extended burnup, and reduced waste generation. In fiscal year (FY) 2012, AFC’s scope expanded to include research, development, and demonstration (RD&D) for light water reactor (LWR) fuels with enhanced accident tolerance. Fuel fabrication activities include the development of innovative methods to enhance process efficiencies, reduce waste, and improve control over as-fabricated fuel microstructural properties to achieve desired in-reactor performance. Using modern modeling and simulation approaches, the objective is to predict fresh fuel properties given the feedstock characteristics and fabrication process parameters. The performance-related activities include small-scale, in-reactor, and out-of-reactor phenomenological testing (distinct from, but synergistic with, integral prototypic testing) and extensive, quantitative characterization (focusing on characterization of fuel and cladding materials at the scale of microstructure) both before and after testing. Larger-scale, prototypic experiments are conducted in concert with phenomenological testing to drive a Fuel Development and Qualification program, incorporating a fundamental understanding of fuel behavior performance characteristics. Then, using the tools developed under the productive science-based approach, fuels will be optimized to meet specific performance requirements, thereby minimizing the need to repeatedly perform large-scale, integral experiments over a wide parametric range as a means of experimental exploration. Two significant initiatives are underway within AFC. First, a gap analysis completed in early FY 2019 identified critical irradiation testing needs that are lacking within the national light water reactor (LWR) fuels testbed since the shutdown of the Halden Reactor in 2018. The identified gaps are for instrumented, prototypic testing of LWR fuels, especially under boiling water reactor conditions, ramp conditions, and conditions leading to fuel failure; these needs exist for supporting current LWR fuels and their possible extension to higher burnups, but are especially urgent relative to near-term development and qualification of accident-tolerant fuels. Recommendations that resulted from the Halden Gap Analysis focused on enhancements at Advanced Test Reactor (ATR) and Transient Reactor Test Facility (TREAT) to fill gaps in testing capabilities relative to these needs. Second, a concerted effort to develop and demonstrate a systematic approach to accelerating the development, testing, and qualification of new fuel systems has been initiated. This is highlighted by a test strategy that combines the considerable advances in multiscale, mechanistic fuel modeling of recent years with a MiniFuel separate effects test program in the High Flux Isotope Reactor (HFIR) and a Fission Accelerated Steady-state Testing (FAST) semi-integral accelerated test program in ATR. This approach is being tested/demonstrated using the metallic fuel system, but if successful it is expected to be extensible to multiple fuel types and diverse applications. This document includes an overview of the NFCSC program, a definition of science-based development of nuclear fuels, near-term goals for Advanced LWR fuels (ALFs), and longer-term goals for Advanced Reactor Fuels (ARFs) RD&D. This includes the activities that will be conducted to achieve success toward the grand challenge, as well as the goals and milestones to be achieved over the next few decades of research and development. Long-term goals are based on the DOE Office of Nuclear Energ

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRS2001

Fitting Vibrational Energy Parameters to Falloff Experiments: CH3 + CH3 + He (0.6-2 Torr 200-298 K)

There are many reported experiments and theoretical calculations for the combination of methyl free radicals diluted in a non-reactive 'deactivator. At high pressure the ethane (C2H6) combination product is the sole product; with decreasing pressure the chemically activated C2H6 will decompose. The falloff in the observed rate coefficient is the result of the competition between collisional stabilization of the chemically activated CA and unimolecular decomposition. The dependence of the rate coefficient on pressure, temperature and collision properties is complex and can not be calculated from first principles. The understanding of this system is not only of fundamental importance but is relevant to the recent detection of methyl free radicals in the atmospheres of Saturn - and Neptune. The temperatures of these outer planet atmospheres are in the 140-200 K region with total pressures (predominately H2 and He) less than 0.2 Torr. Experimentally determined rate coefficients have been reported for this reaction at T = 296-906 K and T = 200-408 K mostly with argon as the deactivator. At T = 200 K only the high pressure rate coefficient has been determined. Complete falloff curves over a wide temperature range (200-1600 K) with a variety of weak collider models used to simulate argon as the deactivator have also been reported by Klippenstein and Harding (KH). More recently we have reported the experimental rate coefficients in the falloff region with helium as the deactivator at 200 and 298 K. In this paper we have used the calculated falloff curves reported by KH for argon to determine the average energy transferred per collision for helium in our recently reported experiments. Collision rates were converted using Lennard Jones parameters; the temperature dependence of this conversion factor is noted. The helium experiments were consistent with a down of approximately 100 cm (exp-1); the temperature dependence was slight. The magnitude of down and its temperature dependence will be compared to other systems with similar substrate complexity and reaction energetics.

Tardy, Dwight C.↗