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303 records · Page 17
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

High-pressure phase diagram of beryllium from ab initio free-energy calculations

In this report we use first-principles molecular dynamics simulations coupled with the thermodynamic integration method to study the hexagonal close-packed (hcp) to body-centered cubic (bcc) transition and melting of beryllium up to a pressure of 1600 GPa. We derive the melting line by equating solid and liquid Gibbs free energies and represent it by a Simon-Glatzel fit T m = 1564 K [1 + P/(15.6032 GPa)] 0.383 , which is in good agreement with previous two-phase simulations <6000 K. We also derive the hcp-bcc solid-solid phase boundary and show that the quasiharmonic approximation underestimates the stability of the hcp structure, predicting lower transition pressures between hcp and bcc phases. Our results are consistent with the stability regime predicted by the phonon quasiparticle method. We also predict that the hcp-bcc-liquid triple point is located at 164.7 GPa and 4314 K. In addition, we compute the shock Hugoniot curve and show that it is in good agreement with experiments, intersecting our derived melting curve at ~235 GPa and 4900 K. Finally, we make predictions for future ramp compression experiments. Starting with an isentropic compression of the liquid, we predict the path to intersect the melting line at low pressure and temperature, then to continue along the melting line over a large temperature interval of 7000 K as the sample remains in the mixed solid-liquid state before it enters the solid phase.

36 MATERIALS SCIENCE↗
DOE OSTI2023

A New Plasma Radar Concept for Simultaneous Magnetic and Density Measurements

An innovative, compact 288GHz interferometer has been fabricated, tested, installed and successfully demonstrated on the LAPD-U magnetized plasma at UCLA. The system takes advantage of frequency modulated (FM) radar techniques to deliver a compact heterodyne system. In addition, the reflected power from the source is taken advantage of to eliminate the need for additional quasi-optical components. Electron density in LAPD-U plasma has recently been increased substantially thereby requiring a higher frequency/shorter wavelength interferometer to avoid deleterious refractive effects. This system satisfies those needs. The system uses a 96GHz varactor tuned Gunn oscillator which passes to a passive tripler. This tripler has ~3% conversion efficiency. The 288GHz radiation is then coupled to free space using a so-called dual-mode or Pickett horn. The output 288GHz beam is then coupled to an aspheric lens manufactured from low-loss, high-density polyethylene. This lens is employed to collimate the emerging beam. Small axial adjustment of the lens position can also be used to create a slowly focusing beam so as to optimize the measured signal. In addition, up-down or side-to-side adjustment of the lens can be utilized to steer the beam vertically or horizontally – again to optimize alignment. The propagating beam passes through a beam splitter and then through a water-free, bubble-free fused quartz window into the LAPD-U vacuum vessel. The beam-splitter is a thin sheet of G10 which reflects a small fraction of the incident power (~5 %) towards a zero-bias detector optimized for the frequency range from 220 to 300GHz. Note that waveguides at this frequency have dimensions of ~0.9mm x 0.45mm and so have very large conductive losses. This drives the use of quasi-optical propagation. The detector requires no DC bias and is very responsive (> 1V/mW into 1MΩ). Radiation is coupled to the detector via a similar lens-horn arrangement used for the launch. This reflected beam acts as the local oscillator or reference millimeter-wave beam for the detector. The remainder of the launched source beam then enters the LAPD-U vacuum vessel and passes through the plasma at the mid-plane until reaching the opposing port which is closed off with an aluminum flange. This flange is used as a mirror to retroreflect the incident 288GHz beam back along its path. The retroreflected beam exits the input port but does NOT couple directly into the zero-bias detector. Instead, the majority of the return power continues towards the 288GHz source. As mentioned above the transmitted beam enters the source a second time. This would appear undesirable. However, at these frequencies multipliers are highly non-linear elements which results in a significant portion of the return beam (~20%) re-emerging from the multiplier and horn and then coupling via the G10 beam-splitter to the zero-bias detector. This approach eliminated the need for a second quasi-optical beam-splitter. The system is extremely compact measuring approximately 28 inches x 20 inches. The above did not explain how heterodyne operation was achieved. As mentioned above the Gunn oscillator is able to be varactor tuned. This allows a low voltage to be applied to control the operating frequency of the Gunn oscillator. During heterodyne operation a sawtooth shaped voltage is applied to the varactor at 750kHz using an 80MHz Arbitrary Waveform Generator (AWG). This voltage changes the Gunn frequency linearly during the up-sweep which is then reset abruptly at the sawtooth crash to be immediately followed by another linear sweep. Passage through the 288GHz multiplier triples the frequency change experienced by the electromagnetic wave. These frequency changes are small – tens of megahertz. This FM radar approach results in the launched electromagnetic wave frequencies at the detector for the reference and plasma wave to be different. The approximately 10 ns delay propagation delay for the plasma beam results in the local oscillator and plasma beams NOT having an identical frequency – there is in fact a fixed difference frequency. The frequency tuning level of the Gunn oscillator is then adjusted so that there is ONE cycle of this difference frequency during each linear ramp. During the sawtooth crash or downward re-sweep this one cycle replays in reverse but on a very fast timescale. The process then repeats. Low-pass filtering eliminates the fast re-sweep to leave a pure sine wave heterodyne signal. When the plasma is present it introduces a phase delay in the sine wave (caused by the extremely small Doppler shift resulting from the optical path length change). Of course, to measure this phase change we need a reference. This is simply obtained from an arbitrary waveform generator which provides a synchronized output pulse train which again is low pass filtered to obtain a 750kHz sinusoidal voltage reference for the interferometer. The interferometer was installed on LAPD-U where it has worked reliably and has established that electron densities exceeding 1x10 13 cm -3 are routinely achieved. In addition, the system sensitivity was able to easily observe density fluctuation at frequencies up to 50kHz. FM Radar techniques have enabled a full demonstration of a compact, sensitive, high frequency (288GHz/1mm) heterodyne interferometer.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

First observation of a shape isomer and a low-lying strongly-coupled prolate band in neutron-deficient semi-magic 187 Pb

Prompt and delayed gamma-ray spectroscopy of the neutron-deficient, semi-magic isotope 187Pb has been performed using the recoil-decay and isomer-decay tagging techniques at the Argonne Gas-Filled Analyzer. A new 5.15(15)-mu s isomeric state at only 308 keV above the spherical 3/2 - ground state is identified and classified as a shape isomer. A strongly-coupled band is observed on top of the isomer, which is nearly identical to the one built on the prolate 7/2 - [514] Nilsson state in the isotone 185 Hg. Based on this similarity and on the result of the potential-energy surface calculations, the new isomer in 187 Pb is proposed to originate from the same configuration. The retarded character of the 308-keV (7/2( - )→ 3/2$_{gs}^{-}$ transition with a deduced B(E2) = 5.6(2) x 10 -4 W.u. can be well explained by the significant difference between the prolate parent and spherical daughter configurations, leading to the shape isomerism. The excitation energy of the isomer is surprisingly low, being roughly half of the excitation energies of the known 0 + intruder bandheads in the neighboring 186,188 Pb isotopes. The combined results of the present work and the previous alpha-decay and laser spectroscopy studies present evidence for triple shape coexistence at low energy in the negative-parity configurations of 187 Pb, which is well reproduced by the potential-energy surface calculations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Production and Performance of High Sulfur Concentration Waste Glasses (FY21)

In FY21 Savannah River National Laboratory (SRNL) was tasked to investigate the practical aspects of low activity waste (LAW) glass production with high sulfur loading for the Office of River Protection (ORP). Relationships between sulfur solubility, retention, and melter resonance need to be evaluated to refine waste loading limits and the super saturated melting (triple melt, grind, and wash) methodology. The impact of high sulfur concentration on durability and phase stability (crystallization and liquid-liquid immiscibility) during slow cooling also needs to be further evaluated. To accomplish this, SRNL proposed scaled melter testing using simulants with matched physicochemical properties to melter feed, as opposed to laboratory reagents. This type of testing is expected to validate applicability to design parameters and functional criteria expected during unit operations. This work was expected to commence in FY21, with the first melter tests being performed near the end of the FY. However, reduced access to Savannah River Site and personnel availability during the COVID-19 pandemic significantly reduced the amount of time and resources available to perform the task. This report documents the experimental plan and progress towards this task. The following is a summarized list of scheduled testing that will be performed on feed, condensate, cold cap and glass: 1) Melter runs; 2) Product consistency test (PCT); 3) Inductively coupled plasma optical emission spectroscopy (ICP-OES); and 4) Optical (OM) and scanning electron microscopy (SEM).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

Band structures and Z 2 invariants of two-dimensional transition metal dichalcogenide monolayers from fully relativistic Dirac-Kohn-Sham theory using Gaussian-type orbitals

Two-dimensional (2D) materials exhibit a wide range of remarkable phenomena, many of which owe their existence to the relativistic spin-orbit coupling (SOC) effects. To understand and predict properties of materials containing heavy elements, such as the transition-metal dichalcogenides (TMDs), relativistic effects must be taken into account in first-principles calculations. We present an all-electron method based on the four-component Dirac Hamiltonian and Gaussian-type orbitals (GTOs) that overcomes complications associated with linear dependencies and ill-conditioned matrices that arise when diffuse functions are included in the basis. Until now, there has been no systematic study of the convergence of GTO basis sets for periodic solids either at the nonrelativistic or the relativistic level. Here, in this study, we provide such a study of relativistic band structures of the 2D TMDs in the hexagonal (2H), tetragonal (1T), and distorted tetragonal (1T') structures, along with a discussion of their SOC-driven properties (Rashba splitting and Z 2 topological invariants). We demonstrate the viability of our approach even when large basis sets with multiple basis functions involving various valence orbitals (denoted triple- and quadruple-ζ) are used in the relativistic regime. Our method does not require the use of pseudopotentials and provides access to all electronic states within the same framework. Our study paves the way for direct studies of material properties, such as the parameters in spin Hamiltonians, that depend heavily on the electron density near atomic nuclei where relativistic and SOC effects are the strongest.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1998

Reciprocal Space Mapping of Macromolecular Crystals in the Laboratory

The technique of reciprocal space mapping applied to the physical measurement of macromolecular crystals will be described. This technique uses a triple axis diffractometer setup whereby the monochromator is the first crystal, the sample is the second and the third crystal (of the same material as the monochromator) analyzes the diffracted beam. The geometry is such that it is possible to separate mosaic volume effects from lattice strain effects. The deconvolution of the instrument parameters will also be addressed. Results from measurements at Brookhaven National Synchrotron Radiation Source carried out on microgravity and ground-grown crystals will be presented. The required beam characteristics for reciprocal space mapping are also ideal for topographic studies and the first topographs ever recorded from microgravity protein crystal samples will be shown. We are now working on a system which will enable reciprocal space mapping, mosaicity and topography studies to be carried out in the home laboratory. This system uses a rotating anode X-ray source to provide an intense beam then a Bartels double crystal, four reflection monochromator to provide the spectral and geometric beam conditioning necessary such that the instrument characteristics do not mask the measurement. This is coupled to a high precision diffractometer and sensitive detector. Commissioning data and first results from the system will be presented.

Snell, Edward H.↗
DOE OSTI2021

Non-Hermitian topological states in 2D line-graph lattices: evolving triple exceptional points on reciprocal line graphs

Non-Hermitian (NH) topological states, such as the doubly-degenerate nodes dubbed as exceptional points (EPs) in Bloch band structure of 2D lattices driven by gain and loss, have attracted much recent interest. We demonstrate theoretically that in the three-site edge-centered lattices, i.e. the so-called line-graph lattices, such as kagome lattice which is a line graph of hexagonal lattice, there exist three types of triply-degenerate EPs evolving intriguingly on another set of line graphs in the reciprocal space. A single TEP (STEP) with ±1/3 topological charge moves faithfully along the edges of reciprocal line graphs with varying gain and loss, while two STEPs merge distinctively into one unconventional orthogonal double TEP (DTEP) with ±2/3 charge at the vertices, which is characterized with two ordinary self-orthogonal eigenfunctions but one surprising 'orthogonal' eigenfunction. Differently, in a modified line-graph lattice with an off-edge-center site, the ordinary coalesced state of DTEPs emerges with three identical self-orthogonal eigenfunctions. Such NH states and their evolution can be generally realized in various artificial systems, such as photonic and sonic crystals, where light and sonic vortex beams with different fractional twisting can be found. Our findings shed new light on fundamental understanding of gapless topological states in NH systems in terms of creation and evolution of high-order EPs, and open up new research directions to further link line graph and flow network theory coupled with topological physics, especially under non-equilibrium gain/loss conditions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Perspective on Kramers symmetry breaking and restoration in relativistic electronic structure methods for open-shell systems

Without rigorous symmetry constraints, solutions to approximate electronic structure methods may artificially break symmetry. In the case of the relativistic electronic structure, if time-reversal symmetry is not enforced in calculations of molecules not subject to a magnetic field, it is possible to artificially break Kramers degeneracy in open shell systems. This leads to a description of excited states that may be qualitatively incorrect. Despite this, different electronic structure methods to incorporate correlation and excited states can partially restore Kramers degeneracy from a broken symmetry solution. For single-reference techniques, the inclusion of double and possibly triple excitations in the ground state provides much of the needed correction. Formally, however, this imbalanced treatment of the Kramers-paired spaces is a multi-reference problem, and so methods such as complete-active-space methods perform much better at recovering much of the correct symmetry by state averaging. Using multi-reference configuration interaction, any additional corrections can be obtained as the solution approaches the full configuration interaction limit. A recently proposed “Kramers contamination” value is also used to assess the magnitude of symmetry breaking.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1994

Close encounters of the third-body kind

We simulated encounters involving binaries of two eccentricities: e = 0 (i.e., circular binaries) and e = 0.5. In both cases the binary contained a point mass of 1.4 solar masses (i.e., a neutron star) and a 0.8 solar masses main-sequence star modeled as a polytrope. The semimajor axes of both binaries were set to 60 solar radii (0.28 AU). We considered intruders of three masses: 1.4 solar masses (a neutron star), 0.8 solar masses (a main-sequence star or a higher mass white dwarf), and 0.64 solar masses (a more typical mass white dwarf). Our strategy was to perform a large number (40,000) of encounters using a three-body code, then to rerun a small number of cases with a three-dimensional smoothed particle hydrodynamics (SPH) code to determine the importance of hydrodynamical effects. Using the results of the three-body runs, we computed the exchange across sections, sigma(sub ex). From the results of the SPH runs, we computed the cross sections for clean exchange, denoted by sigma(sub cx); the formation of a triple system, denoted by sigma(sub trp); and the formation of a merged binary with an object formed from the merger of two of the stars left in orbit around the third star, denoted by sigma(sub mb). For encounters between either binary and a 1.4 solar masses neutron star, sigma(sub cx) approx. 0.7 sigma(sub ex) and sigma(sub mb) + sigma(sub trp) approx. 0.3 sigma(sub ex). For encounters between either binary and the 0.8 solar masses main-sequence star, sigma(sub cx) approx. 0.50 sigma(sub ex) and sigma(sub mb) + sigma(sub trp) approx. 1.0 sigma(sub ex). If the main sequence star is replaced by a main-sequence star of the same mass, we have sigma(sub cx) approx. 0.5 sigma(sub ex) and sigma(sub mb) + sigma(sub trp) approx. 1.6 sigma(sub ex). Although the exchange cross section is a sensitive function of intruder mass, we see that the cross section to produce merged binaries is roughly independent of intruder mass. The merged binaries produced have semi-major axes much larger than either those of the original binaries or those of binaries produced in clean exchanges. Coupled with their lower kick velocities, received from the encounters, their larger size will enhance their cross section, shortening the waiting time to a subsequent encounter with another single star.

Davies, M. B.↗
DOE OSTI2021

Temporal characterization of fundamental plasma parameters in pulsed liquid electrode plasma (LEP) optical emission spectrometry

The fundamental characteristics of liquid electrode plasma (LEP), a pulsed plasma source for optical emission spectrometry, were investigated. Two distinct phases were observed during the process of pulsed plasma generation, namely bubble generation and active plasma discharge. Additionally the ionization efficiency of the LEP, with Mg as a representative analyte, was gauged from the ratio of Mg II 279.553 nm to Mg I 285.213 nm emission and was found to increase from about 5% to 20% in a close-to-linear fashion with the discharge voltage from 800 V to 1200 V. The Mg II/Mg I ratio of the LEP was 2.5 to 3 orders of magnitude less than that typically offered by an inductively coupled plasma (ICP) but was comparable to other solution-based glow discharges. It was found that an off-time interval of more than 150 ms between successive discharge pulses was required to obtain a stable pulse-to-pulse discharge current. Temporally resolved emissions of Mg II 279.6 nm, Mg I 285.2 nm, Fe I 373.5 nm, OH band head at 306 nm, and Hα line at 656.3 nm showed that the background species (OH band and Hα line) reached their maximum emission intensities at around 0.5 ms to 0.7 ms with respect to the onset of the discharge pulse whereas the maximum emissions were observed between 0.7 ms to 0.9 ms for analyte species (Mg and Fe lines). The electron density observed in the present work was in the range from 5.7 × 10 15 cm -3 to 8.2 × 10 15 cm -3 , which was similar to those found in an analytical ICP. The temporal averaged OH rotational temperature was 3300 K, which was comparable to the values of an analytical ICP and solution-based glow discharges. By contrast, the temporally averaged Fe I excitation temperature was around 8900 K, which was even higher than that of an analytical ICP and roughly triple the values obtained by techniques based on glow discharge of liquid samples.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Code-to-code comparison between FLASH and HYDRA in gas-puff Z-pinch modeling

The numerical modeling of gas-puff Z pinches involves the nonlinear coupling of a broad range of complex, multi-physics phenomena that makes such simulations challenging. The challenge is further compounded by nonlinear instabilities that can impact the dynamics of imploding gas-puff Z pinches, such as the magneto Rayleigh–Taylor instability (MRTI). If the growth rate and amplitude of the latter is comparable to the relevant timescales and properties of the imploding plasma, the MRTI can dramatically alter implosion dynamics, dictate pinch stability, and govern the plasma properties achievable in pulsed-power-driven laboratory experiments. National Laboratories and academic teams have developed numerical tools that can accurately model Z-pinch configurations and provide reliable design capabilities that can guide experimental choices and assist in interpreting experimental results. Most such tools, however, are not broadly available. Here, we present newly developed Z-pinch simulation capabilities of the publicly available FLASH code, applied in the study of MRTI growth and dynamical effects in gas-puff implosions. To verify the new implementations, we perform a comparison of FLASH gas-puff implosion simulations with previously published calculations with the HYDRA code from Lawrence Livermore National Laboratory, which have been validated with experimental data from the CESZAR pulsed-power driver at the University of California, San Diego. The experiments involved double- and triple-nozzle configurations, in an experimental attempt to stabilize the pinch to the MRTI. The code-to-code comparison shows similar results between the FLASH and HYDRA simulations, supporting the use of FLASH in the modeling of future gas-puff Z-pinch experiments at CESZAR.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Triple Emission of 5'-( para -R-Phenylene)vinylene-2-(2'-hydroxyphenyl)benzoxazole (PVHBO). Part I: Dual Emission from the Neutral Species

The effects of 5'-(para-R-phenylene)vinylene (PV) substituents on the emission properties of 2-(2'-hydroxyphenyl)benzoxazole (HBO) are analyzed using steady-state and time-resolved absorption and emission spectroscopies in addition to quantum chemical calculations. All members in the series of PVHBOs are capable of excited-state intramolecular proton transfer (ESIPT) with a solvent sensitivity that is typical of a HBO derivative to produce a normal (aka enol) emission and an excited-state tautomer (aka keto) emission. These two emission bands of the neutral dyes are discussed in the current paper. The intermolecular proton transfer, i.e., the deprotonation, of a PVHBO results in the third band of the triple emission, which is described in the succeeding paper. The placement of an electron-withdrawing substituent R on the PVHBO scaffold increases the intensity of the keto emission relative to the enol emission in hydrogen-bonding solvents. The R substituents do not significantly alter the wavelengths of the enol and keto emission bands, which are located in the blue and green regions, respectively, of the visible spectrum. The ultrafast time-resolved spectroscopies and quantum chemical calculations offer explanations on how the R group and the solvent affect the enol and keto emission properties (i.e., wavelength, lifetime, fluorescence quantum yield, and relative ratio of their emissions). Here, the key findings include the following: (1) the emission energies of both enol and keto forms are not sensitively dependent on the R substituent and (2) the solvent-engaged enol excited state is quenched more efficiently as the R substituent becomes more electron-withdrawing. A PVHBO acts as a fusion of HBO and stilbenoid that intersect at the hydroxyphenyl moiety. Depending on the solvent and other environmental conditions, PVHBOs may exhibit the ESIPT property of HBO or the substituent-dependent emission of stilbenoid. This paper and the succeeding article provide a photophysical model of PVHBOs to explain the wavelengths and relative abundances of the three emission bands (enol, keto, and anion) that these compounds are able to produce. Judicial selection of the environmental factors may drive the emission of a PVHBO into the spectral regions of blue, green, and, in a couple of cases, orange or red.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1985

Balloon-based interferometric techniques

A balloon-borne triple-etalon Fabry-Perot Interferometer, observing the Doppler shifts of absorption lines caused by molecular oxygen and water vapor in the far red/near infrared spectrum of backscattered sunlight, has been used to evaluate a passive spaceborne remote sensing technique for measuring winds in the troposphere and stratosphere. There have been two successful high altitude balloon flights of the prototype UCL instrument from the National Scientific Balloon Facility at Palestine, TE (May 80, Oct. 83). The results from these flights have demonstrated that an interferometer with adequate resolution, stability and sensitivity can be built. The wind data are of comparable quality to those obtained from operational techniques (balloon and rocket sonde, cloud-top drift analysis, and from the gradient wind analysis of satellite radiance measurements). However, the interferometric data can provide a regular global grid, over a height range from 5 to 50 km in regions of clear air. Between the middle troposphere (5 km) and the upper stratosphere (40 to 50 km), an optimized instrument can make wind measurements over the daylit hemisphere with an accuracy of about 3 to 5 m/sec (2 sigma). It is possible to obtain full height profiles between altitudes of 5 and 50 km, with 4 km height resolution, and a spatial resolution of about 200 km, along the orbit track. Below an altitude of about 10 km, Fraunhofer lines of solar origin are possible targets of the Doppler wind analysis. Above an altitude of 50 km, the weakness of the backscattered solar spectrum (decreasing air density) is coupled with the low absorption crosssection of all atmospheric species in the spectral region up to 800 nm (where imaging photon detectors can be used), causing the along-the-track resolution (or error) to increase beyond values useful for operational purposes. Within the region of optimum performance (5 to 50 km), however, the technique is a valuable potential complement to existing wind measuring systems and can provide a low cost addition to powerful active (LIDAR) wind measuring systems now under development.

Rees, David↗
DOE OSTI2024

Lattice Symmetry-Guided Charge Transport in 2D Supramolecular Polymers Promotes Triplet Formation

Singlet-to-triplet intersystem crossing (ISC) in organic molecules is intimately connected with their geometries: by modifying the molecular shape, symmetry selection rules pertaining to spin-orbit coupling can be partially relieved, leading to extra matrix elements for increased ISC. As an analog to this molecular design concept, the study finds that the lattice symmetry of supramolecular polymers also defines their triplet formation efficiencies. A supramolecular polymer self-assembled from weakly interacting molecules is considered. Its 2D oblique unit cell effectively renders it as a coplanar array of 1D molecular columns weakly bound to each other. Using momentum-resolved photoluminescence imaging in combination with Monte Carlo simulations, the study found that photogenerated charge carriers in the supramolecular polymer predominantly recombine as spin-uncorrelated carrier pairs through inter-column charge transfer states. This lattice-defined recombination pathway leads to a substantial triplet formation efficiency (≈60%) in the supramolecular polymer. These findings suggest that lattice symmetry of micro-/macroscopic structures relying on intermolecular interactions can be strategized for controlled triplet formation.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Calibration of the Diffusivity Predictions of Centipede Using Approximate Bayesian Computation and Applications in Nyx (Engineering Scale) and Xolotl-MARMOT (Meso-Scale) Simulations

Fission gas evolution and release in UO 2 nuclear fuel are important fuel performance metrics and occur in several distinct stages: 1) nucleation, growth and resolution of intra-granular bubbles, 2) diffusion to grain boundaries and 3) nucleation and growth of bubbles at grain boundaries, which eventually form a connected network (percolation) enabling release of gas from grain boundaries through connections to triple junctions, grain edges or free surfaces. The NE-SciDAC project is developing several computational tools to model this problem, which are connected in a hierarchical multi-scale framework. The information transfer in the multi-scale framework is a critical step that, in addition to best-estimates, should include uncertainty quantification. Despite taking a first-principles multi-scale approach, there is a need to perform parameter calibration to ensure consistency with available experimental data. In the present study, uncertainty quantification (UQ) and parameter calibration is demonstrated for one of the lower length scale codes in the multi-scale framework (Centipede) and then the results, including instances of the propagated uncertainties, are used in other codes within the framework, specifically Nyx and Xolotl-MARMOT. We calibrated the model parameters in Centipede, a computer code used to predict diffusivities of uranium (U) and xenon (Xe) in the context of the simulation of fission gas in uranium oxide (UO 2 ) nuclear fuel. The Centipede code depends on 183 parameters, all of which are subject to uncertainty. The three data sets used in our calibration effort are taken from the literature. This data is available as a set of measurements, including measurement errors. Our goal is to calibrate a statistical model that predicts both the value of the measurement and the uncertainty associated with the measurement. We perform a Bayesian calibration of the model parameters using a dedicated approximate Bayesian computation (ABC) likelihood function. To avoid excessive computational costs, we replace the expensive Centipede simulation code by a higher-order surrogate model, constructed using only the 9 most important parameters. These important parameters are identified by a preliminary global sensitivity analysis (GSA) study. Among the important parameters are T0 (the temperature at which UO 2 is perfectly stoichiometric) and Hf_pO2 (the temperature dependence of the oxygen (O) partial pressure) that should be considered as operating conditions to be estimated along with the other parameters. We consider two different cases: one where we define one set of these operating conditions for all data sets, and one where we define distinct operating condition parameters for each data set. The Xe diffusivities predicted by the latter case show distinct features that could not be observed in the former. Next, we use the diffusivity predictions by Centipede as input to Nyx, a reduced order fuel performance code focused on gas behavior alone, in order to estimate quantities associated with inter-granular bubble formation at conditions specified by the experiments. Finally, the diffusivities obtained from the calibrated Centipede runs were used in coupled Xolotl-MARMOT simulations of intra- and inter-granular gas evolution. The results are compared to simulations using the baseline diffusivities from Turnbull et al.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗