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At least 1,297 records · Page 72
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Far ultraviolet absorption spectra of N{sub 3} and N{sub 2}{sup +} generated by electrons impacting gaseous N{sub 2}

Electron bombardment of gaseous N{sub 2} produces N{sub 2} {sup +} and N{sub 3}, which are subsequently trapped in the N{sub 2} matrix at 10 K. Both the infrared and ultraviolet absorption spectra of the matrix sample at various stages of electron irradiation were recorded. Apart from a progression observed below 192 nm, with intervals ∼900 cm{sup –1}, corresponding to the transition of D {sup 2} Π {sub g} ← X {sup 2} Σ {sub g} {sup +} of N{sub 2} {sup +}, three new progressions were recorded in the range 225-192 nm, with intervals ∼1000 cm{sup –1}, that correlated well with variations in intensities of the electronic absorption band of N{sub 3} at 272.7 nm; an absorption coefficient of 3.76 × 10{sup –17} cm molecule{sup –1} for the transition A {sup 2}Σ{sub u} {sup +}← X {sup 2}Π{sub g} of N{sub 3} was estimated for the first time. These newly observed progressions were characterized and the vertical excitation energy and oscillator strength were calculated using time-dependent, density-functional theory. This was based on assigning the three progressions to electronic transitions of N{sub 3} from the ground state to 2 {sup 2}Π{sub u}, 1 {sup 2}Σ{sub g} {sup +}, and 1 {sup 2}Σ{sub g} {sup –}, respectively.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2016

Simulation of fission gas diffusion in UO{sub 2} by vacancy clusters

The low solubility of fission gas in nuclear fuel leads to inter- and intra-granular bubbles. These bubbles affect performance of the fuel rod and increase the fuel temperature through the increase of porosity in the fuel pellets and decreased thermal conductivity across the pellet-clad gap as gas is released into the plenum. The nucleation, growth, and inter-connectivity of the fission gas bubbles ultimately depend on the diffusivity of gas atoms through the fuel matrix. Using mechanisms and data previously established from density functional theory (DFT) and empirical potential calculations, diffusion and reaction models have been derived for xenon atoms, uranium atoms, and vacancies in the substitutional and interstitial locations. Although similar to previous models, the diffusion and reaction rates have been re-derived in a more robust manner. Previous studies have under-predicted the experimentally observed diffusivity of xenon atoms in UO{sub 2}, however it has been previously shown that by including xenon atoms bound to two vacancies, the calculated diffusivity approaches the measured data. The derived model for species diffusion and inter-species reactions has been implemented in the MARMOT phase-field code in a modular structure so as to capture the enhanced diffusion of xenon due to bound gas + vacancy-cluster movement. The MARMOT code allows for the diffusion, reaction, and source rates to be solved simultaneously, resulting in steady state or transient concentrations of each species, and ultimately the diffusion behavior of xenon atoms. By including the diffusion of clusters of different combinations of xenon and vacancies, the calculated diffusivity more closely captures the measured diffusivity of xenon when using preliminary parameters. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS2001

Radiation dosimetry using three-dimensional optical random access memories

Three-dimensional optical random access memories (3D ORAMs) are a new generation of high-density data storage devices. Binary information is stored and retrieved via a light induced reversible transformation of an ensemble of bistable photochromic molecules embedded in a polymer matrix. This paper describes the application of 3D ORAM materials to radiation dosimetry. It is shown both theoretically and experimentally, that ionizing radiation in the form of heavy charged particles is capable of changing the information originally stored on the ORAM material. The magnitude and spatial distribution of these changes are used as a measure of the absorbed dose, particle type and energy. The effects of exposure on 3D ORAM materials have been investigated for a variety of particle types and energies, including protons, alpha particles and 12C ions. The exposed materials are observed to fluoresce when exposed to laser light. The intensity and the depth of the fluorescence is dependent on the type and energy of the particle to which the materials were exposed. It is shown that these effects can be modeled using Monte Carlo calculations. The model provides a better understanding of the properties of these materials. which should prove useful for developing systems for charged particle and neutron dosimetry/detector applications. c2001 Published by Elsevier Science B.V.

Non-NASA Center↗
DOE OSTI2025

Surrogate models for linear response

Linear response theory is a well-established method in physics and chemistry for exploring excitations of many-body systems. In particular, the quasiparticle random-phase approximation (QRPA) provides a powerful microscopic framework by building excitations on top of the mean-field vacuum; however, its high computational cost limits model calibration and uncertainty quantification studies. Here, we present two complementary QRPA surrogate models and apply them to study response functions of finite nuclei. One is a reduced-order model that exploits the underlying QRPA structure, while the other utilizes the recently developed parametric matrix model algorithm to construct a map between the system’s Hamiltonian and observables. Our benchmark applications, the calculation of the electric dipole polarizability of 180 Yb and the 𝛽-decay half-life of 80 Ni, show that both emulators can achieve 0.1%–1% accuracy while offering a 6–7 orders of magnitude speedup compared to state-of-the-art QRPA solvers. These results demonstrate that the developed QRPA emulators are well positioned to enable Bayesian calibration and large-scale studies of computationally expensive physics models describing the properties of many-body systems.

Beta decay↗
DOE OSTI2011

Report on Sodium Compatibility of Advanced Structural Materials

This report provides an update on the evaluation of sodium structural materials. The report is a deliverable (level 3) in FY11 (M3A11AN04030403), under the Work Package A-11AN040304, “Sodium Compatibility of Advanced Structural Materials” performed by Argonne National Laboratory (ANL), as part of Advanced Structural Materials Program for the Advanced Reactor Concepts. This work package supports the advanced structural materials development by providing corrosion and tensile data from the standpoint of sodium compatibility of advanced structural alloys. The scope of work involves exposure of advanced structural alloys such as G92, mod.9Cr-1Mo (G91) ferritic-martensitic steels and HT-UPS austenitic stainless steels to a flowing sodium environment with controlled impurity concentrations. The exposed specimens are analyzed for their corrosion performance, microstructural changes, and tensile behavior. Previous reports examined the thermodynamic and kinetic factors involved in the design, fabrication, and construction of a forced convection sodium loop for sodium compatibility studies of advanced materials. This report presents the results on corrosion performance, microstructure, and tensile properties of advanced ferritic-martensitic and austenitic alloys exposed to liquid sodium at 550°C for up to 2700 h and at 650°C for up to 5064 h in the forced convection sodium loop. The oxygen content of sodium was controlled by the cold-trapping method to achieve ~1 wppm oxygen level. Four alloys were examined, G92 in the normalized and tempered condition (H1 G92), G92 in the cold-rolled condition (H2 G92), G91 in the normalized and tempered condition, and hot-rolled HT-UPS. G91 was included as a reference to compare with advanced alloy, G92. It was found that all four alloys showed weight loss after sodium exposures at 550 and 650°C. The weight loss of the four alloys was comparable after sodium exposures at 550°C; the weight loss of ferritic-martensitic steels, G92 and G91 is more significant than that of austenitic stainless steel, HT-UPS after sodium exposures at 650°C. Sodium exposures up to 2700 h at 550°C had no significant influence on tensile properties, while sodium exposures up to 5064 h at 650°C dramatically lowered the tensile strengths of the four alloys. The ultimate tensile strength of H1 G92, H2 G92, and G91 ferritic-martensitic steels was reduced to as much as nearly half of its initial value after sodium exposures at 650°C. Though the uniform elongation was recovered to some extent, these three ferritic-martensitic steels showed considerable strain softening after sodium exposures. The yield stress of HT-UPS austenitic stainless steel increased, the ultimate tensile strength decreased, and the total elongation was reduced after sodium exposures at 650°C. The dynamic strain aging effect observed in the as-received HT-UPS specimens became less pronounced after sodium exposures at 650°C. Microstructural characterization of sodium-exposed specimens showed no appreciable surface deterioration or grain structure changes under an optical microscope, except for the H2 G92 steel, in which the martensite structure transformed to large grain ferrite after sodium exposures at 650°C. TEM observations of the sodium-exposed H2 G92 steel showed significant recrystallization after sodium exposure for 2700 h at 550°C, and transformation of martensite to ferrite and high density of precipitates in nearly dislocation-free matrix after sodium exposures at 650°C. Further microstructural analysis and evaluation of decarburization/carburization behavior is needed to understand the dramatic changes in the tensile strengths of advanced ferritic-martensitic and austenitic steels after sodium exposures at 650°C.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Investigation of secondary γ -ray angular distributions using the N 15 ( p , α 1 γ ) C * 12 reaction

The observation of secondary γ-rays provides an alternative method of measuring cross sections that populate excited final states in nuclear reactions. The angular distributions of these γ-rays also provide information on the underlying reaction mechanism. Despite a large amount of data of this type in the literature, publicly available R-matrix codes do not have the ability to calculate these types of angular distributions. In this report, the mathematical formalism derived in Brune and deBoer is implemented in the R-matrix code AZURE2 and calculations are compared with previous data from the literature for the 15 N( p, α1γ ) 12 C* reaction. In addition, new measurements, made at the University of Notre Dame Nuclear Science Laboratory using the Hybrid Array of Gamma Ray Detectors (HAGRiD), are reported that span an energy range from E p = 0.88 to 4.0 MeV. Excellent agreement between data and the phenomenological fit is obtained up to the limit of the previous fit at E p = 2.0 MeV and the R-matrix fit is extended from E x ≈ 13.5 up to E x ≈ 15.3 MeV, where 15 N+p and 12 C+α reactions are fit simultaneously for the first time. An excellent reproduction of the 15 N( p, α1γ ) 12 C* and 12 C(α, α) 12 C data is achieved, but inconsistencies and difficulty in fitting other data is encountered and discussed.

6 ≤ A ≤ 19↗
DOE OSTI2014

Study of Plastic Scintillator Properties for Radioactive Sources Dosimetry - Paper 108

Plastic scintillator is a simple material which has the density close to that of human soft tissue (1.06 g/cm{sup 3}). Its energy response is close to that of human soft tissue and it is relatively energy independent. This prospect provide a desired characteristics in measuring dose by plastic scintillator either for radiation monitoring or personal dosimeter. Generally the energy calibration of organic scintillator will be done by using gamma ray sources. The positions of Compton edge in pulse height spectra, which have known energy values will be identified. However the Compton edge normally is very broad and difficult to determine the point corresponding to that particular Compton electron energies. Many researchers used several fitting functions and Monte Carlo simulations to determine the position of Compton edge. For example, Proctor and Wellman (2012) used a straight line fit to the linear part of Compton edge and extrapolated to zero count. While L. Swiderski et al. used a method based on a back-scattered coincidence measurement to measure in a wide energy range the position of Compton edge in organic scintillators. For a simple and quick approach of calibration, we used a Gauss-error function to fit the Compton edge region of interest by assumed that the location of maximum energy of Compton electrons is half-height of the Compton maximum (CM). The reasons is because the CM position could be determined easily from the spectra throughout wide energy range. Interpreting gamma dose rates from accumulated plastic scintillation detector spectra is often a complex task because the probability of a full energy deposition event in the detector is often negligible. Despite no full energy peaks in plastic scintillator spectra, several attempts have been made by the other researchers to obtain the dose from the energy distribution spectra of gamma radiation. For example, Proctor and Wellman used the modified spectrum dose index (SDI) to calculate the exposure rates by multiplying the energy corresponding to its channel and all products are summed before multiply by a calibration constant to yield an exposure rate. While Lobdell and Hertel calculated dose using a response matrix based on spectral unfolding technique. From these points of view, we have made an attempt to correlate the counts obtained in scintillator with absorbed dose or ambient dose equivalent. We aimed to calibrate the plastic scintillator energy deposition for dose, by correlate the counts obtained with a particular value of dose. By designed the scintillator to measure at 1 cm tissue depth might be helpful to be used as radiation monitoring or personal dosimeter since the energy response of plastic scintillator is relatively energy independent compared to that of inorganic scintillators. The energy calibration proposed from simple fitting approach had been verified with calculated spectra. This might be considered as a practical approach for technician or radiation workers with sufficient accuracy. The linear behavior of counts per absorbed dose give promising to calibrate scintillator energy deposition to read dose (equivalent dose or absorbed dose) for photons. Thus the scintillator could provide both the energy and dose response simultaneously, which may important in some radiation field of measurements. Currently the scintillator is able to give dose rate value for gamma sources of Cs-137 and Mn-54. The number of counts per unit absorbed dose would likely to vary somewhat with photon energy, although the plastic scintillator should have a tissue dose response that is relatively energy independent. Further analysis will be done on conversion factor parameters so that it could be used in such situations where the radiation field is complex or unknown. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Bayesian mixture model approach to quantifying the empirical nuclear saturation point

The equation of state (EOS) in the limit of infinite symmetric nuclear matter exhibits an equilibrium density, $n_0 \approx 0.16 \, \mathrm{fm}^{-3}$, at which the pressure vanishes and the energy per particle attains its minimum, $E_0 \approx -16 \, \mathrm{MeV}$. Although not directly measurable, the nuclear saturation point $(n_0,E_0)$ can be extrapolated by density functional theory (DFT), providing tight constraints for microscopic interactions derived from chiral effective field theory (EFT). However, when considering several DFT predictions for $(n_0,E_0)$ from Skyrme and Relativistic Mean Field (RMF) models together, a discrepancy between these model classes emerges at high confidence levels that each model prediction's uncertainty cannot explain. How can we leverage these DFT constraints to rigorously benchmark nuclear saturation properties of chiral interactions? To address this question, we present a Bayesian mixture model that combines multiple DFT predictions for $(n_0,E_0)$ using an efficient conjugate prior approach. The inferred posterior distribution for the saturation point's mean and covariance matrix follows a Normal-inverse-Wishart class, resulting in posterior predictives in the form of correlated, bivariate $t$-distributions. The DFT uncertainty reports are then used to mix these posteriors using an ordinary Monte Carlo approach. At the 95\% credibility level, we estimate $n_0 \approx 0.157 \pm 0.010 \, \mathrm{fm}^{-3}$ and $E_0 \approx -15.97 \pm 0.40 \, \mathrm{MeV}$ for the marginal (univariate) $t$-distributions. Combined with chiral EFT calculations of the pure neutron matter EOS, we obtain bivariate normal distributions for the nuclear symmetry energy and its slope parameter evaluated at $n_0$: $S_v \approx 32.0 \pm 1.1 \, \mathrm{MeV}$ and $L\approx 52.6\pm 8.1 \, \mathrm{MeV}$ (95\%), respectively. Furthermore, our Bayesian framework is publicly available, so practitioners can readily use and extend our results.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2013

THE ABUNDANCES OF HYDROCARBON FUNCTIONAL GROUPS IN THE INTERSTELLAR MEDIUM INFERRED FROM LABORATORY SPECTRA OF HYDROGENATED AND METHYLATED POLYCYCLIC AROMATIC HYDROCARBONS

Infrared (IR) absorption spectra of individual polycyclic aromatic hydrocarbons (PAHs) containing methyl (-CH{sub 3}), methylene (CH{sub 2}), or diamond-like CH groups and IR spectra of mixtures of methylated and hydrogenated PAHs prepared by gas-phase condensation were measured at room temperature (as grains in pellets) and at low temperature (isolated in Ne matrices). In addition, the PAH blends were subjected to an in-depth molecular structure analysis by means of high-performance liquid chromatography, nuclear magnetic resonance spectroscopy, and matrix-assisted laser desorption/ionization time-of-flight mass spectrometry. Supported by calculations at the density functional theory level, the laboratory results were applied to analyze in detail the aliphatic absorption complex of the diffuse interstellar medium at 3.4 μm and to determine the abundances of hydrocarbon functional groups. Assuming that the PAHs are mainly locked in grains, aliphatic CH {sub x} groups (x = 1, 2, 3) would contribute approximately in equal quantities to the 3.4 μm feature (N {sub CHx}/N {sub H} ≈ 10{sup –5}-2 × 10{sup –5}). The abundances, however, may be two to four times lower if a major contribution to the 3.4 μm feature comes from molecules in the gas phase. Aromatic ≅CH groups seem to be almost absent from some lines of sight, but can be nearly as abundant as each of the aliphatic components in other directions (N{sub ≅CH}/N {sub H} ∼< 2 × 10{sup –5}; upper value for grains). Due to comparatively low binding energies, astronomical IR emission sources do not display such heavy excess hydrogenation. At best, especially in protoplanetary nebulae, CH{sub 2} groups bound to aromatic molecules, i.e., excess hydrogens on the molecular periphery only, can survive the presence of a nearby star.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Partially polaron-transformed quantum master equation for exciton and charge transport dynamics

Polaron-transformed quantum master equation (PQME) offers a unified framework to describe the dynamics of quantum systems in both limits of weak and strong couplings to environmental degrees of freedom. Thus, the PQME serves as an efficient method to describe charge and exciton transfer/transport dynamics for a broad range of parameters in condensed or complex environments. However, in some cases, the polaron transformation (PT) being employed in the formulation invokes an over-relaxation of slow modes and results in premature suppression of important coherence terms. A formal framework to address this issue is developed in the present work by employing a partial PT that has smaller weights for low frequency bath modes. In this work, it is shown that a closed form expression of a second order time-local PQME including all the inhomogeneous terms can be derived for a general form of partial PT, although more complicated than that for the full PT. All the expressions needed for numerical calculation are derived in detail. Applications to a model of a two-level system coupled to a bath of harmonic oscillators, with test calculations focused on those due to homogeneous relaxation terms, demonstrate the feasibility and the utility of the present approach.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Characterization of ZnO Nanoparticles using Superconducting Tunnel Junction Cryodetection Mass Spectrometry

Zinc oxide (ZnO) nanoparticles coated with either n-octylamine (OA) or α-amino poly(styrene-co-acrylonitrile) (PSAN) ligands (L) have been analyzed using laser desorption/ionization and matrix assisted laser desorption/ionization (MALDI) time-of-flight (TOF) superconducting tunnel junction (STJ) cryodetection mass spectrometry. STJ cryodetection has the advantage of high m/z detection and allows for the determination of average molecular weights and dispersities for 500–600 kDa ZnO-L nanoparticles. The ability to detect the relative energies deposited into the STJs has allowed for investigation of ZnO-L metastable fragmentation. ZnO-L precursor ions gain enough internal energy during the MALDI process to undergo metastable fragmentation in the flight tube. These fragments produced a lower energy peak, which was assigned as ligand-stripped ZnO cores whereas the individual ligands were at too low of an energy to be observed. From these STJ energy resolved peaks, the average weight percentage of inorganic material making up the nanoparticle was determined, where ZnO-OA and ZnO-PSAN nanoparticles are comprised of ~62% and ~68% wt ZnO, respectively. In one example, grafting densities were calculated based on the metastable fragmentation of ligands from the core to be 16 and 1.1 nm{sup –2} for ZnO-OA and ZnO-PSAN, respectively, and compared with values determined by thermogravimetric analysis (TGA) and transmission electron microscopy (TEM). .

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2013

Synthesis, crystal and electronic structures and magnetic properties of Li{sub 2}SnMo{sub 3}O{sub 8}: A novel reduced molybdenum oxide containing Mo{sub 3}O{sub 13} cluster units

Powder samples and single crystals of the quaternary oxide Li{sub 2}SnMo{sub 3}O{sub 8} were obtained by solid state reaction. The structure was determined by single-crystal X-ray diffraction. Li{sub 2}SnMo{sub 3}O{sub 8} crystallizes in the hexagonal space group P6{sub 3}mc with unit-cell parameters a=5.7720 (2) Å, c=10.3941 (3) Å and Z=2. Full-matrix least-squares refinement on F{sup 2} using 930 independent reflections for 31 refinable parameters results in R{sub 1}=0.0354 and wR{sub 2}=0.0643. The crystal structure consists of distorted hexagonal-close-packed oxygen layers with stacking sequence abac along [0 0 1] and that are held together by alternating lithium-tin and molybdenum layers. The Li{sup +} and Sn{sup 4+} ions occupy, respectively, tetrahedral and octahedral sites in the ratio 2:1. The Mo atoms occupy octahedral sites and form strongly bonded triangular clusters involving three MoO{sub 6} octahedra that are each shared along two edges, constituting a Mo{sub 3}O{sub 13} unit. Magnetic susceptibility measurements are in agreement with a spin-pairing of the eight d electrons per Mo{sub 3} cluster. The electronic structure of Li{sub 2}SnMo{sub 3}O{sub 8} is analyzed using periodic density functional calculations. - Graphical abstract: We present here the synthesis, the crystal and electronic structures, and the magnetic properties of the new quaternary compound containing Mo{sub 3}O{sub 13} units, Li{sub 2}SnMo{sub 3}O{sub 8}. - Highlights: • The new quaternary reduced molybdenum oxide containing Mo{sub 3} clusters, Li{sub 2}SnMo{sub 3}O{sub 8}, was synthesized by solid state reaction. • Eight electrons per Mo{sub 3} cluster. • Single-crystal X-ray study. • Magnetic susceptibility measurements. • Periodic density functional calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2004

Vibration Characteristics Determined for Stainless Steel Sandwich Panels With a Metal Foam Core for Lightweight Fan Blade Design

The goal of this project at the NASA Glenn Research Center is to provide fan materials that are safer, weigh less, and cost less than the currently used titanium alloy or polymer matrix composite fans. The proposed material system is a sandwich fan construction made up of thin solid face sheets and a lightweight metal foam core. The stiffness of the sandwich structure is increased by separating the two face sheets by the foam layer. The resulting structure has a high stiffness and lighter weight in comparison to the solid facesheet material alone. The face sheets carry the applied in-plane and bending loads (ref. 1). The metal foam core must resist the transverse shear and transverse normal loads, as well as keep the facings supported and working as a single unit. Metal foams have ranges of mechanical properties, such as light weight, impact resistance, and vibration suppression (ref. 2), which makes them more suitable for use in lightweight fan structures. Metal foams have been available for decades (refs. 3 and 4), but the difficulties in the original processes and high costs have prevented their widespread use. However, advances in production techniques and cost reduction have created a new interest in this class of materials (ref. 5). The material chosen for the face sheet and the metal foam for this study was the aerospace-grade stainless steel 17-4PH. This steel was chosen because of its attractive mechanical properties and the ease with which it can be made through the powder metallurgy process (ref. 6). The advantages of a metal foam core, in comparison to a typical honeycomb core, are material isotropy and the ease of forming complex geometries, such as fan blades. A section of a 17-4PH sandwich structure is shown in the following photograph. Part of process of designing any blade is to determine the natural frequencies of the particular blade shape. A designer needs to predict the resonance frequencies of a new blade design to properly identify a useful operating range. Operating a blade at or near the resonance frequencies leads to high-cycle fatigue, which ultimately limits the blade's durability and life. So the aim of this study is to determine the variation of the resonance frequencies for an idealized sandwich blade as a function of its face-sheet thickness, core thickness, and foam density. The finite element method is used to determine the natural frequencies for an idealized rectangular sandwich blade. The proven Lanczos method (ref. 7) is used in the study to extract the natural frequency.

Ghosn, Louis J.↗
DOE OSTI2018

Quantum thermodynamics from the nonequilibrium dynamics of open systems: Energy, heat capacity, and the third law

In a series of papers, we intend to take the perspective of open quantum systems and examine from their nonequilibrium dynamics the conditions when the physical quantities, their relations, and the laws of thermodynamics become well defined and viable for quantum many-body systems. We first describe how an open-system nonequilibrium dynamics (ONEq) approach is different from the closed combined system + environment in a global thermal state (CGTs) setup. Only after the open system equilibrates will it be amenable to conventional thermodynamics descriptions, thus quantum thermodynamics (QTD) comes at the end rather than assumed in the beginning. The linkage between the two comes from the reduced density matrix of ONEq in that stage having the same form as that of the system in the CGTs. We see the open-system approach having the advantage of dealing with nonequilibrium processes as many experiments in the near future will call for. Because it spells out the conditions of QTD's existence, it can also aid us in addressing the basic issues in quantum thermodynamics from first principles in a systematic way. We then study one broad class of open quantum systems where the full nonequilibrium dynamics can be solved exactly, that of the quantum Brownian motion of N strongly coupled harmonic oscillators, interacting strongly with a scalar-field environment. In this paper, we focus on the internal energy, heat capacity, and the third law. We show for this class of physical models, amongst other findings, the extensive property of the internal energy, the positivity of the heat capacity, and the validity of the third law from the perspective of the behavior of the heat capacity toward zero temperature. These conclusions obtained from exact solutions and quantitative analysis clearly disprove claims of negative specific heat in such systems and dispel allegations that in such systems the validity of the third law of thermodynamics relies on quantum entanglement. They are conceptually and factually unrelated issues. As a result, entropy and entanglement will be the main theme of our second paper on this subject matter.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Neutron Absorber Plate Characterization Plan for Criticality Experiments Design

After being used in nuclear installations, depleted fuel can still be highly reactive and must be handled securely to prevent any radiological or criticality concerns. In particular, spent fuel from use in nuclear power reactors must be stored and transported in specifically designed containers using neutron absorber materials to prevent criticality. Various neutron absorber material types exist and are manufactured by various entities, as thoroughly described in the Handbook of Neutron Absorber Materials for Spent Nuclear Fuel Storage and Transportation Applications written by EPRI. Presently, one of the most modern and most widely used types of neutron absorber material contains particles of boron carbide, or B 4 C, embedded in aluminum matrix: Boralcan, manufactured by Rio Tinto. It is very important for the community to know as much as possible about such neutron absorber materials. Therefore, in the recent years, a US Department of Energy National Nuclear Security Administration–Nuclear Criticality Safety Program funded project initiated design of an experiment that places Boralcan neutron-absorbing plates in an established critical assembly using low-enriched uranium fuel at the Sandia Pulsed Reactor Facility/Critical Experiments (SPRF/CX) apparatus at Sandia National Laboratories. The goal of the experiment is to produce high-quality benchmark data to submit to the International Criticality Safety Benchmark Evaluation Project (ICSBEP), for use in validating calculational tools and nuclear data by criticality safety analysts. The project, named IER-554, is currently in its final design stage, following a successful preliminary design. In the work documented in the design study, ten critical configurations using Boralcan neutron absorber plates were designed, and the experiment was proven to be feasible, with a predicted low k eff uncertainty around 100 pcm. An overview of the modeled cutout of the critical assembly with a Boralcan plate is shown in Figure 1, representing one of the configurations planned for the critical experiments. Before the plates are inserted in the critical assembly, it is necessary to know more about their composition and uniformity. This summary focuses on the plate characterization plans. Each plate will undergo (1) neutron transmission measurements at different locations to determine the 10 B areal density and (2) an in-depth x-ray computed tomography (XCT) examination to obtain the exact Sizes and distribution of the B4C powder particles inside the plates. In parallel, plate modeling studies are performed with a goal to determine the validity of the currently used approximation of modeling the neutron absorber plates as a homogeneous mixture of Aluminum 1100 alloy and B4C— instead of explicitly modeling the B4C particles. By using the experimental 10 B areal density measurements, and the exact size and location of the B4C particles obtained by XCT, a plate model can theoretically be built that reproduces the plate with extremely high fidelity. The results of this modeling study could increase the confidence of the criticality safety community in its modeling methods when using this type of neutron absorber material, and the industry could use these validations to change the boron loading credit limits from the U.S. Nuclear Regulatory Commission standard review plan for dry cask storage of spent nuclear fuel. The modeling calculations are performed with SCALE 6.3.0 using the KENO V.a sequence for criticality calculations with the ENDF/B-VIII.0 continuous-energy cross section library.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

A theoretical approach for transient shock strengthening in high-energy-density laser compression experiments

In high-energy-density shock compression experiments, the desired state of compression is typically achieved by passing shock waves through a sequence of different materials. Here, a theoretical approach for transiently strengthening such shocks passing through interfaces of experimentally relevant impedance ratios is examined. A semi-analytical method based on characteristics analysis is used to solve the problem of a shock passing from one material to another through an intermediate region of non-uniform impedance; by appropriately designing this region, a greater shock strength can be achieved in the second material for a finite duration than in the absence of this region. When a shock passes into a material of higher impedance, the shock strengthening increases to a maximum before decreasing to an asymptotic value as the strength of the incident shock is increased. For shocks passing into materials of decreasing impedance, the shock strengthening increases monotonically as the strength of the incident shock is increased when the impedance ratio is above a critical threshold. Incorporating multiple intermediate materials can further increase the strength of the transmitted shock, with an exponential discretization of intermediate material impedances being the most effective distribution for strengthening strong shocks. The results suggest that up to 25% and 9% increases in pressure behind the leading shock can be achieved for materials of increasing and decreasing impedance, respectively. The technique is applied to the design of laser-driven dynamic compression experiments, and the results of the analysis are verified via comparison to simulations performed with the HYADES hydrodynamics code.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2012

Structure of AgI-doped Ge-In-S glasses: Experiment, reverse Monte Carlo modelling, and density functional calculations

We report an investigation of the structure and vibrational modes of Ge-In-S-AgI bulk glasses using X-ray diffraction, EXAFS spectroscopy, Reverse Monte-Carlo (RMC) modelling, Raman spectroscopy, and density functional theoretical (DFT) calculations. The combination of these techniques made it possible to elucidate the short- and medium-range structural order of these glasses. Data interpretation revealed that the AgI-free glass structure is composed of a network where GeS{sub 4/2} tetrahedra are linked with trigonal InS{sub 3/2} units; S{sub 3/2}Ge-GeS{sub 3/2} ethane-like species linked with InS{sub 4/2}{sup -} tetrahedra form sub-structures which are dispersed in the network structure. The addition of AgI into the Ge-In-S glassy matrix causes appreciable structural changes, enriching the Indium species with Iodine terminal atoms. The existence of trigonal species InS{sub 2/2}I and tetrahedral units InS{sub 3/2}I{sup -} and InS{sub 2/2}I{sub 2}{sup -} is compatible with the EXAFS and RMC analysis. Their vibrational properties (harmonic frequencies and Raman activities) calculated by DFT are in very good agreement with the experimental values determined by Raman spectroscopy. - Graphical abstract: Experiment (XRD, EXAFS, RMC, Raman scattering) and density functional calculations are employed to study the structure of AgI-doped Ge-In-S glasses. The role of mixed structural units as illustrated in the figure is elucidated. Highlights: Black-Right-Pointing-Pointer Doping Ge-In-S glasses with AgI causes significant changes in glass structure. Black-Right-Pointing-Pointer Experiment and DFT are combined to elucidate short- and medium-range structural order. Black-Right-Pointing-Pointer Indium atoms form both (InS{sub 4/2}){sup -} tetrahedra and InS{sub 3/2} planar triangles. Black-Right-Pointing-Pointer (InS{sub 4/2}){sup -} tetrahedra bond to (S{sub 3/2}Ge-GeS{sub 3/2}){sup 2+} ethane-like units forming neutral sub-structures. Black-Right-Pointing-Pointer Mixed chalcohalide species (InS{sub 3/2}I){sup -} offer vulnerable sites for the uptake of Ag{sup +}.

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DOE OSTI2014

Universal tight binding model for chemical reactions in solution and at surfaces. I. Organic molecules

As is now well established, a first order expansion of the Hohenberg–Kohn total energy density functional about a trial input density, namely, the Harris–Foulkes functional, can be used to rationalize a non self consistent tight binding model. If the expansion is taken to second order then the energy and electron density matrix need to be calculated self consistently and from this functional one can derive a charge self consistent tight binding theory. In this paper we have used this to describe a polarizable ion tight binding model which has the benefit of treating charge transfer in point multipoles. This admits a ready description of ionic polarizability and crystal field splitting. It is necessary in constructing such a model to find a number of parameters that mimic their more exact counterparts in the density functional theory. We describe in detail how this is done using a combination of intuition, exact analytical fitting, and a genetic optimization algorithm. Having obtained model parameters we show that this constitutes a transferable scheme that can be applied rather universally to small and medium sized organic molecules. We have shown that the model gives a good account of static structural and dynamic vibrational properties of a library of molecules, and finally we demonstrate the model's capability by showing a real time simulation of an enolization reaction in aqueous solution. In two subsequent papers, we show that the model is a great deal more general in that it will describe solvents and solid substrates and that therefore we have created a self consistent quantum mechanical scheme that may be applied to simulations in heterogeneous catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗