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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 397 records · Page 22
All sourcesNASA NTRSDOE OSTI
NASA NTRS2014

Highly Accurate Potential Energy Surface, Dipole Moment Surface, Rovibrational Energy Levels, and Infrared Line List for (32)S(16)O2 up to 8000 cm(exp -1)

A purely ab initio potential energy surface (PES) was refined with selected (32)S(16)O2 HITRAN data. Compared to HITRAN, the root-mean-squares error (RMS) error for all J=0-80 rovibrational energy levels computed on the refined PES (denoted Ames-1) is 0.013 cm(exp -1). Combined with a CCSD(T)/aug-cc-pV(Q+d)Z dipole moment surface (DMS), an infrared (IR) line list (denoted Ames-296K) has been computed at 296K and covers up to 8,000 cm(exp -1). Compared to the HITRAN and CDMS databases, the intensity agreement for most vibrational bands is better than 85-90%. Our predictions for (34)S(16)O2 band origins, higher energy (32)S(16)O2 band origins and missing (32)S(16)O2 IR bands have been verified by most recent experiments and available HITRAN data. We conclude that the Ames-1 PES is able to predict (32/34)S(16)O2 band origins below 5500 cm(exp -1) with 0.01-0.03 cm(exp -1) uncertainties, and the Ames-296K line list provides continuous, reliable and accurate IR simulations. The Ka-dependence of both line position and line intensity errors is discussed. The line list will greatly facilitate SO2 IR spectral experimental analysis, as well as elimination of SO2 lines in high-resolution astronomical observations.

Sulfur Dioxide (SO2)↗
DOE OSTI2021

Resonances of A = 4T = 1 isospin triplet states within the ab initio no-core Gamow shell model

Here, the A = 4 nuclei, i.e., 4 H, 4 He, and 4 Li , establish an interesting isospin T = 1 isobaric system. 4 H and 4 Li are unbound broad resonances, whereas 4 He is deeply bound in its ground state but unbound in all its excited states. The present situation is that experiments so far have not given consistent data on the resonances. Few-body calculations have well studied the scatterings of the 4N systems. In the present work, we provide many-body calculations of the broad resonance structures, in an ab initio framework with modern realistic interactions. It occurs that, indeed, 4 H, 4 Li, and excited 4 He are broad resonances, which is in accordance with experimental observations. The calculations also show that the first 1 - excited state almost degenerates with the 2 - ground state in the pair of mirror isobars of 4 H and 4 Li, which may suggest that the experimental data on energy and width are the mixture of the ground state and the first excited state. The T = 1 isospin triplet formed with an excited state of 4 He and ground states of 4 H and 4 Li is studied, focusing on the effect of isospin symmetry breaking.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Advancements in Validation of TSLs through Inelastic Neutron Scattering and Transmission Measurements [Abstract]

Historically, the free gas approximation has been used to treat the thermal scattering of neutrons with energies below a few electron-volts (eV) in unevaluated materials. However, this method inadequately reproduces neutron scattering at these energies. Until recently, only a limited number of materials had available thermal scattering law (TSL) files/libraries in the ENDF nuclear data libraries in this energy range. With advancements in atomistic modeling techniques, such as molecular dynamics, ab-initio molecular dynamics, and density functional theory, TSL libraries have become available for many more materials. This is particularly relevant due to the rising interest in several advanced reactor systems that require novel moderator and reflector materials. While quasi-integral and integral benchmarks have been designed to validate historically important moderator materials (such as light water and polyethylene), there is currently a lack of standard validation methods for TSLs, especially when multiple conflicting TSLs exist. To address this issue, the Oak Ridge National Lab Nuclear Data group has been working on utilizing inelastic neutron scattering (INS) measurements combined with transmission (i.e., total cross section) measurements to evaluate and validate TSLs for different materials. We plan to demonstrate how this method has worked on materials such as polyethylene, lucite, and polystyrene. In addition, we will compare the newly created libraries to ENDF libraries for these materials and explain why integral benchmarks should not be used for validation when multiple TSLs exist.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2014

Electron impact rotationally elastic total cross section for formamide

This paper reports computational results of the total cross sections for electron impact on formamide (HCONH₂) over a wide range of energies from 0.01 eV to 5 keV. Total cross sections over such a wide range are reported for the first time as the earlier reported data is up to maximum of 12 eV. Below ionization threshold of the target, we performed ab initio calculations using UK molecular R-Matrix code within static, exchange plus polarization (SEP), and close coupling approximations. Twenty eight target states are included in close coupling formalism. Total 350 channels and 2410 configuration state functions are included in the calculations. We observe a π* shape resonance at 3.41 eV and a σ* resonance at 15.3 eV as against similar resonances reported at 3.77 eV and 14.9 eV, respectively, by Goumans et al. [J. Chem. Theory Comput. 5, 217 (2009)] using SEP model. The cross sections at higher energies are evaluated using the spherical complex optical potential formalism. The two methods are found to be consistent with a smooth cross over at 18 eV. The vertical excitation energies, electronic excitation cross sections, differential cross sections, momentum transfer, and total cross sections are computed. In absence of experimental data, we compared our computed total cross sections with available other theoretical results.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Modeling the thermodynamics of the FeTi hydrogenation under para-equilibrium: An ab-initio and experimental study

We report FeTi-based hydrides have recently re-attracted attention as stationary hydrogen storage materials due to favorable reversibility, good sorption kinetics and relatively low costs compared to alternative intermetallic hydrides. Employing the OpenCalphad software, the thermodynamics of the (FeTi) 1-x H x (0 ≤ x ≤ 1) system were assessed as a key basis for modeling hydrogenation of FeTi-based alloys. New thermodynamic data were acquired from our experimental pressure-composition-isotherm (PCI) curves, as well as first-principles calculations utilizing density functional theory (DFT). The thermodynamic phase models were carefully selected based on critical analysis of literature information and ab-initio investigations. Key thermodynamic properties such as dissociation pressure, formation enthalpies and phase diagrams were calculated in good agreement to our performed experiments and literature-reported data. This work provides an initial perspective, which can be extended to account for higher-order thermodynamic assessments and subsequently enables the design of novel FeTi-based hydrides. In addition, the assessed thermodynamic data can serve as key inputs for kinetic models and hydride microstructure simulations.

08 HYDROGEN↗
DOE OSTI2018

Thermal Conductivity of Metallic Uranium

This project has developed a modeling and simulation approaches to predict the thermal conductivity of metallic fuels and their alloys. We focus on two methods. The first method has been developed by the team at the University of Wisconsin Madison. They developed a practical and general modeling approach for thermal conductivity of metals and metal alloys that integrates ab-initio and semi-empirical physics-based models to maximize the strengths of both techniques. The second method has been developed by the team at Virginia Tech. This approach consists of a determining the thermal conductivity using only ab-initio methods without any fitting parameters. Both methods were complementary. The models incorporated both phonon and electron contributions. Good agreement with experimental data over a wide temperature range were found. The models also provided insight into the different physical factors that govern the thermal conductivity under different temperatures. The models were general enough to incorporate more complex effects like additional alloying species, defects, transmutation products and noble gas bubbles to predict the behavior of complex metallic alloys like U-alloy fuel systems under burnup. 3 Introduction Thermal conductivity is an important thermal physical property affecting the performance and efficiency of metallic fuels. Some experimental measurement of thermal conductivity and its correlation with composition and temperature from empirical fitting are available for U, Zr and their alloys with Pu and other minor actinides. However, as reviewed in by Kim, Cho and Sohn, due to the difficulty in doing experiments on actinide materials, thermal conductivities of metallic fuels have only been measured at limited alloy compositions and temperatures, some of them even being negative and unphysical. Furthermore, the correlations developed so far are empirical in nature and may not be accurate when used for prediction at conditions far from those used in the original fitting. Moreover, as fuels burn up in the reactor and fission products are built up, thermal conductivity is also significantly changed. Unfortunately, fundamental understanding of the effect of fission products is also currently lacking. In this project, we probe thermal conductivity of metallic fuels with ab initio calculations, a theoretical tool with the potential to yield better accuracy and predictive power than empirical fitting. This work will both complement experimental data by determining thermal conductivity in wider composition and temperature ranges than is available experimentally, and also develop mechanistic understanding to guide better design of metallic fuels in the future. So far, we focused on α-U perfect crystal, the ground-state phase of U metal. We focus on two methods. The first method has been developed by the team at the University of Wisconsin Madison. They developed a practical and general modeling approach for thermal conductivity of metals and metal alloys that integrates ab-initio and semi-empirical physics-based models to maximize the strengths of both techniques. The second method has been developed by the team at Virginia Tech. This approach consists of a determining the thermal conductivity using only ab-initio methods without any fitting parameters. Both methods were complementary and very helpful to understand the physics behind the thermal conductivity in metallic uranium and other materials with similar characteristics. In Section I, the combined model developed at UWM is explained. In Section II, the ab-initio method developed at VT is described along with the uranium pseudo-potential and its validation. Section III is devoted to the work done by Jianguo Yu at INL. Finally, we will present the performance of the project in terms of milestones, publications, and presentations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Accurate thermoelastic tensor and acoustic velocities of NaCl

Despite the importance of thermoelastic properties of minerals in geology and geophysics, their measurement at high pressures and temperatures are still challenging. Thus, ab initio calculations are an essential tool for predicting these properties at extreme conditions. Owing to the approximate description of the exchange-correlation energy, approximations used in calculations of vibrational effects, and numerical/methodological approximations, these methods produce systematic deviations. Hybrid schemes combining experimental data and theoretical results have emerged as a way to reconcile available information and offer more reliable predictions at experimentally inaccessible thermodynamics conditions. Here we introduce a method to improve the calculated thermoelastic tensor by using highly accurate thermal equation of state (EoS). The corrective scheme is general, applicable to crystalline solids with any symmetry, and can produce accurate results at conditions where experimental data may not exist. We apply it to rock-salt-type NaCl, a material whose structural properties have been challenging to describe accurately by standard ab initio methods and whose acoustic/seismic properties are important for the gas and oil industry.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Electro-Oxidation of Methane on Platinum under Ambient Conditions

Herein, we investigate the electrochemical conversion of methane to CO 2 on platinum electrodes under ambient conditions. Through a combination of experimentation, density functional theory (DFT) calculations, and ab initio kinetic modeling, we have developed an improved understanding of the reaction mechanism and the factors that determine catalyst activity. We hypothesized that the rate-determining methane activation step is thermochemical (i.e., CH 4 (g) → CH 3 * + H * ) as opposed to electrochemical based on a fitted barrier of approximately 0.96 eV that possesses minimal potential dependence. We developed a simple kinetic model based on the assumption of thermochemical methane activation as the rate-determining step, and the results match well with experimental data. Namely, the magnitude of the maximum current density and the electrode potential at which it is realized agree with our ab initio kinetic model. Finally, we expanded our kinetic model to include other transition metals via a descriptor-based analysis and found platinum to be the most active catalyst for the oxidation of methane, which is in line with previously published experimental observations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

High-Precision Spectroscopy of 20 O Benchmarking Ab Initio Calculations in Light Nuclei

The excited states of unstable 20 O were investigated via γ-ray spectroscopy following the 19 O(d, p) ⁢20 O reaction at 8 A⁢ MeV. By exploiting the Doppler shift attenuation method, the lifetimes of the $2^+_2$ and $3^+_1$ states were firmly established. From the γ-ray branching and E⁢2/M⁢1 mixing ratios for transitions deexciting the $2^+_2$ and $3^+_1$ states, the B⁡(E⁢2) and B⁡(M⁢1) were determined. Various chiral effective field theory Hamiltonians, describing the nuclear properties beyond ground states, along with a standard USDB interaction, were compared with the experimentally obtained data. Such a comparison for a large set of γ-ray transition probabilities with the valence space in medium similarity renormalization group ab initio calculations was performed for the first time in a nucleus far from stability. It was shown that the ab initio approaches using chiral effective field theory forces are challenged by detailed high-precision spectroscopic properties of nuclei. Finally, the reduced transition probabilities were found to be a very constraining test of the performance of the ab initio models.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Ab-initio molecular dynamics study of eutectic chloride salt: MgCl2–NaCl–KCl

Ionic liquid materials are viable candidates as a heat transfer fluid (HTF) in a wide range of applications, notably within concentrated solar power (CSP) technology and molten salt reactors (MSRs). For next-generation CSP and MSR technologies that strive for higher power generation efficiency, a HTF with wide liquid phase range and energy storage capabilities is crucial. Studies have shown that eutectic chloride salts exhibit thermal stability at high temperatures, high heat storage capacity, and are less expensive than nitrate and carbonate salts. However, the experimental data needed to fully evaluate the potential of eutectic chloride salts as a HTF contender are scarce and entail large uncertainties. Considering the high cost and potential hazards associated with the experimental methods used to determine the properties of ionic liquids, molecular modeling can be used as a viable alternative resource. In this study, the eutectic ternary chloride salt MgCl 2 –NaCl–KCl is modeled using ab-initio molecular dynamics simulations (AIMDs) in the liquid phase. Using the simulated data, the thermophysical and transport properties of eutectic chloride salt can be calculated: density, viscosity, heat capacity, diffusion coefficient, and ionic conductivity. For an initial model validation, experimental pair-distribution function data were obtained from X-ray total scattering techniques and compared to the theoretical pair-distribution function. Additionally, theoretical viscosity values are compared to experimental viscosity values for a similar system. The results provide a starting foundation for a MgCl 2 –NaCl–KCl model that can be extended to predict other fundamental properties.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2014

The structure of CO{sub 2} hydrate between 0.7 and 1.0 GPa

A deuterated sample of CO{sub 2} structure I (sI) clathrate hydrate (CO{sub 2}·8.3 D{sub 2}O) has been formed and neutron diffraction experiments up to 1.0 GPa at 240 K were performed. The sI CO{sub 2} hydrate transformed at 0.7 GPa into the high pressure phase that had been observed previously by Hirai et al. [J. Phys. Chem. 133, 124511 (2010)] and Bollengier et al. [Geochim. Cosmochim. Acta 119, 322 (2013)], but which had not been structurally identified. The current neutron diffraction data were successfully fitted to a filled ice structure with CO{sub 2} molecules filling the water channels. This CO{sub 2}+water system has also been investigated using classical molecular dynamics and density functional ab initio methods to provide additional characterization of the high pressure structure. Both models indicate the water network adapts a MH-III “like” filled ice structure with considerable disorder of the orientations of the CO{sub 2} molecule. Furthermore, the disorder appears to be a direct result of the level of proton disorder in the water network. In contrast to the conclusions of Bollengier et al., our neutron diffraction data show that the filled ice phase can be recovered to ambient pressure (0.1 MPa) at 96 K, and recrystallization to sI hydrate occurs upon subsequent heating to 150 K, possibly by first forming low density amorphous ice. Unlike other clathrate hydrate systems, which transform from the sI or sII structure to the hexagonal structure (sH) then to the filled ice structure, CO{sub 2} hydrate transforms directly from the sI form to the filled ice structure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Sr{sub 4}Ru{sub 6}ClO{sub 18}, a new Ru{sup 4+/5+} oxy-chloride, solved by precession electron diffraction: Electric and magnetic behavior

The crystal structure of Sr{sub 4}Ru{sub 6}ClO{sub 18}, a new Ru{sup 4+/5+} oxo-chloride, has been determined from Precession Electron Diffraction (PED) data acquired on a nanocrystal in a transmission electron microscope using the technique of electron diffraction tomography. This approach is described in details following a pedagogic route and a systematic comparison is made of this rather new method with other experimental methods of electron diffraction, and with the standard single crystal X-ray diffraction technique. Both transport and magnetic measurements, showed a transition at low temperature that may be correlated to Ru{sup 4+}/Ru{sup 5+} charge ordering. - Graphical abstract: Structure of Sr{sub 4}Ru{sub 6}ClO{sub 18}, determined using Precession Electron Diffraction data. - Highlights: • Structure of Sr{sub 4}Ru{sub 6}ClO{sub 18} was solved ab initio using precession electron diffraction. • This was done both on a nanometric sample and on a micrometric one. • Different type of experimental methods of electron diffraction are compared. • Single crystal X-ray diffraction was used to confirm the results. • Transport properties were characterized and show “exotic” behavior.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Reactive Force Field for Simulations of the Pyrolysis of Polysiloxanes into Silicon Oxycarbide Ceramics

We provide a new reactive force field (ReaxFF) for simulations of silicon oxycarbide (SiCO) ceramics and of their syntheses from inorganic polymer precursors. The validity of the force field is extensively tested against experimental and computational thermochemical data. Its performance in simulation at elevated temperatures is gauged by the results of comprehensive ab initio molecular dynamics simulations. We apply the force field to the formation of amorphous SiCO in a simulated polymer pyrolysis. Modeling results are in good agreement with experimental observations and allow new insights into the formation of graphene segregations embedded in an amorphous oxycarbide matrix. The new ReaxFF for Si-C-O-H compounds enables large- scale and long-time atomistic simulations with unprecedented fidelity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Origin of short- and medium-range order in supercooled liquid Ge 3 Sb 2 Te 6 from ab initio molecular dynamics simulations

Phase-change materials such as Ge–Sb–Te compounds have attracted much attention due to their potential value in electrical data storage. In contrast to the amorphous and crystalline phases, supercooled liquids are far from being deeply understood despite their inevitable role in both amorphization and crystallization processes. To this end, we have studied the dynamics properties and structural characteristics of liquid and supercooled liquid Ge 3 Sb 2 Te 6 during the fast cooling process. As the temperature decreases, chemical bonds become more homogeneous, but coordination numbers of Ge, Sb and Te atoms change very little. Meanwhile, the structural order of short-range configuration is obviously enhanced. Further studies suggest that Ge-centered, Sb-centered and Te-centered configurations change to the more ordered defective octahedrons mainly by adjusting the bond-angle relationship and bond length, rather than just by changing the coordination environment. It is the more ordered octahedrons that promote the formation of medium-range order. Our findings provide a deep insight into the origin of local structural order in supercooled liquid Ge 3 Sb 2 Te 6 , which is of great importance for the comprehensive understanding of amorphization and crystallization processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Thermodynamically constrained correction to ab initio equations of state

We show how equations of state generated by density functional theory methods can be augmented to match experimental data without distorting the correct behavior in the high- and low-density limits. The technique is thermodynamically consistent and relies on knowledge of the density and bulk modulus at a reference state and an estimation of the critical density of the liquid phase. We apply the method to four materials representing different classes of solids: carbon, molybdenum, lithium, and lithium fluoride. It is demonstrated that the corrected equations of state for both the liquid and solid phases show a significantly reduced dependence of the exchange-correlation functional used.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Electronic and thermoelectric properties of InN studied using ab initio density functional theory and Boltzmann transport calculations

The thermoelectric properties of indium nitride in the most stable wurtzite phase (w-InN) as a function of electron and hole concentrations and temperature were studied by solving the semiclassical Boltzmann transport equations in conjunction with ab initio electronic structure calculations, within Density Functional Theory. Based on maximally localized Wannier function basis set and the ab initio band energies, results for the Seebeck coefficient are presented and compared with available experimental data for n-type as well as p-type systems. Also, theoretical results for electric conductivity and power factor are presented. Most cases showed good agreement between the calculated properties and experimental data for w-InN unintentionally and p-type doped with magnesium. Our predictions for temperature and concentration dependences of electrical conductivity and power factor revealed a promising use of InN for intermediate and high temperature thermoelectric applications. The rigid band approach and constant scattering time approximation were utilized in the calculations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Spectral function for 4 He using the Chebyshev expansion in coupled-cluster theory

Here, we compute spectral function for 4 He by combining coupled-cluster theory with an expansion of integral transforms into Chebyshev polynomials. Our method allows us to estimate the uncertainty of spectral reconstruction. The properties of the Chebyshev polynomials make the procedure numerically stable and considerably lower in memory usage than the typically employed Lanczos algorithm. We benchmark our predictions with other calculations in the literature and with electron-scattering data in the quasi-elastic peak. The spectral function formalism allows one to extend ab initio lepton-nucleus cross sections into the relativistic regime. This makes it a promising tool for modeling this process at higher-energy transfers. The results we present open the door for studies of heavier nuclei, important for the neutrino oscillation programs.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗