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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

SAS4A/SASSYS-1 Commercial Grade Dedication Example Report for a Generic Sodium Pool-Type Fast Reactor Application

In the U.S., a key component of the commercialization of advanced reactors is completion of a license application, which must ultimately be approved by the Nuclear Regulatory Commission (NRC). The approval of the license application by the NRC is contingent on satisfactory demonstration of the design basis and the response of the advanced reactor design to transient and accident scenarios using accepted codes and methods. This report describes the qualification and dedication requirements that the advanced reactor safety analysis system software SAS4A/SASSYS-1 are expected to need to fulfill to be used for sodium-cooled pool-type fast reactor licensing. The qualification and dedication requirements are identified through performance critical characteristics and evaluation model acceptance criteria representative of the advanced reactor design considered for licensing. This document captures, additionally, the verification process developed to demonstrate that the software fulfills the qualification and dedication requirements for a generic sodium-cooled pool-type fast reactor as part of the commercial grade dedication process. Like most software that has primarily existed in the research and development space, the most significant challenge facing SAS4A/SASSYS-1 for use in a licensing framework is the availability of a documentation basis describing the code pedigree. SAS4A/SASSYS-1 has been used for licensing of the fast flux test facility (FFTF) and the JOYO sodium-cooled fast reactor in Japan, as well as the design of the CRBR Plant. However, the historical verification and validation (V&V) activities supporting SAS4A/SASSYS-1 development do not align with modern software quality assurance (SQA) and V&V requirements. Two approaches to use of SAS4A/SASSYS-1 in a commercial licensing framework have been identified: commercial-grade dedication (CGD) and software qualification. The methods and requirements prescribed in the ASME NQA-1-2008/2009 Standard and Regulatory Guide 1.203 on the evaluation model development and assessment process (EMDAP) have been used as guidance to define the CGD and qualification processes, respectively. A qualification and dedication requirements matrix has been developed which utilizes fundamental software verification. In this process, software verification is defined as a software quality process aimed at defining software requirement specifications, developing software design documentation, and performing and documenting acceptance testing of the code against requirements. A key element of software qualification and dedication includes determination of software acceptance with respect to critical characteristics relevant to the functional requirements of the software. To assist with identification of cross-cutting transient phenomena and functional requirements, domestic SFR vendor designs have been reviewed to identify a reference SFR design. For this report, the reference design is defined as a pool-type reactor with metal alloy fuel, a liquid-metal intermediate heat transport system, and passive decay heat rejection systems. Given this reference, a series of high-level cross-cutting phenomena was identified for a general class of single-fault undercooling or reactivity insertion transients that scopes the design basis space, with the goal of assisting with prioritization of documentation development efforts for key transient models in SAS: 1) Reactivity feedback response prior to scram; 2) System-wide thermal inertia; 3) Transition in natural circulation flow regime in heat removal systems; 4) Decay heat generation; 5) Steady-state fuel characterization; 5) Clad/fuel behavior at elevated temperatures; 6) Point kinetics and decay heat; 7) Pump coastdown behavior; 8) Core flow redistribution in loss of forced convection; 9) Pool stratification. As a demonstration of CGD of SAS4A/SASSYS-1 for a sodium pool reactor, a software qualification and dedication gap analysis as it relates to code documentation has been performed. This effort leverages the framework established as part of the SAS4A/SASSYS-1 SQA Program. This CGD demonstration provides a framework that vendors can build upon to demonstrate the applicability of the SAS4A/SASSYS-1 software for licensing a sodium-cooled pool-type fast reactor.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2024

Controlling the Manifold of Polariton States Through Molecular Disorder

Exciton polaritons, arising from the interaction of electronic transitions with confined electromagnetic fields, have emerged as a powerful tool to manipulate the properties of organic materials. However, standard experimental and theoretical approaches overlook the significant energetic disorder present in most materials now studied. Using the conjugated polymer P3HT as a model platform, the degree of energetic disorder is systematically tuned and a corresponding redistribution of photonic character within the polariton manifold is observed. Based on these subtle spectral features, a more generalized approach is developed to describe strong light–matter coupling in disordered systems that captures the key spectroscopic observables and provides a description of the rich manifold of states intermediate between bright and dark. Finally, applied to a wide range of organic systems, the method challenges prevailing notions about ultrastrong coupling and whether it can be achieved with broad, disordered absorbers.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Heterointercalation in Chevrel-Phase Sulfides: A Model Periodic Solid for the Investigation of Chain Electron Transfer

Modulation of electron density localization on periodic crystal solids through electron transfer from interstitial cations can directly influence the bonding configurations of small-molecule intermediates at the catalyst binding site. This study presents the microwave-assisted solid-state synthesis of four heterointercalant Chevrel-phase (CP) sulfides with varying metal cation intercalants with compositional and electronic structure investigations of the electron density redistribution as a result of intercalation. The heterointercalant CP sulfides, with the general formula Cu x M y Mo 6 S 8 (where M = Cr, Mn, Fe, Ni; x, y = 1.5−2.5), are presented here for the probe reaction of electrochemical CO 2 reduction. A change in product selectivity is observed toward the production of methanol at low overpotentials of −0.5 V vs reversible hydrogen electrode (RHE), as a result of the intercalant combination present within the CP interstitial cavity. Structural confirmation of all materials was examined through Rietveld refinement of the powder X-ray diffraction (PXRD) data, high-resolution transmission electron microscopy (HR-TEM), and selected-area electron diffraction (SAED). Electron transfer from the intercalated metal cations to the Mo 6 S 8 cluster was investigated via X-ray photoelectron spectroscopy (XPS) of the intercalated metal cations and the chalcogenide cluster. Electron transfer was further confirmed through X-ray absorption analysis (XAS) of the K-edges of Mo and intercalants. Intermediate studies of electrochemical reduction of formaldehyde to methanol resulted in a faradaic efficiency of ∼78% methanol production on Cu x Ni y Mo 6 S 8 . The results presented herein identify distinct principles for materials design that can be utilized in other compositional spaces within the broad families of periodic crystal solids.

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

Understanding Fission Gas Bubble Distribution and Zirconium Redistribution in Neutron-irradiated U-Zr Metallic Fuel Using Machine Learning

U-10wt.% Zr (U-10Zr) based metallic fuel is the leading candidate for next-generation sodium cooled fast reactor in United States. Currently, Idaho National Laboratory (INL) has been the leading national laboratory for research, development, and demonstration (RD&D) on metallic fuel. Advanced post-irradiation characterization will help to understand fuel microstructure and property change during irradiation, benefiting fuel qualification for commercial application. Characterization capabilities ranging from sub-nanometer to micrometer, such as scanning electron microscopy (SEM), focused ion beam (FIB) sampling, transmission electron microscopy (TEM) characterization, and local thermal conductivity microscopy (TCM), have been utilized recently on irradiated U-10Zr fuel samples to gain a better understanding of nuclear fuel microstructure and property evolution inside a reactor. The FIB/SEM coupled with energy dispersive X-ray spectroscopy (EDS) can capture the essential information to achieve better understanding of fuel behaviors. Inside a nuclear reactor, the phase and microstructure of U-10Zr is constantly changing under neutron bombardment. For example, the gaseous fission product atoms have a limited solubility inside fuel matrix and tend to precipitate out in bubble form, which not only contribute to fuel thermal conductivity degradation but also provide a shortcut for movement of fission products, i.e. lanthanides. The resultant deposition of lanthanides at the cladding inner surface will potentially trigger a chemical reaction/interaction between nuclear fuel and cladding at reactor operational conditions, threatening fuel integrity and safety. FIB/SEM coupled with EDS can provide the fission bubble information as well as probe into phase separation or Zr redistribution, which is fundamental to predict the fuel performance. With high velocity image data generating method, such as FIB/SEM, an automatic way to extract the microstructural information quantitively can better serve the needs from post irradiation characterization. A trained machine learning model, named Decision Tree, is employed to generate a bubble classifier and to categorize bubbles into three categories: isolated bubble, connected without lanthanides, and connected with lanthanides bubbles[3]. This work presents a showcase of this approach on six regions of a fuel cross-section along the radial temperature gradient. We obtained distributions of bubble categories and porosity rates along the six regions. Moreover, a secondary phase U-Zr2 was determined and found on regions 5 and 6. The secondary phase fraction was increasing from 15.61% in region 5 to 34.79% in region 6 based on this approach . This quantitative data offers insights into the lanthanide migration and potentially thermal conductivity degradation. This information from machine learning will be fed into fuel design code for better prediction of fuel performance.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

A new and alternative look at nonlinear Alfvénic states

The formulation for studying nonlinear Alfvenic states, sustainable in Hall Magnetohydrodynamics (HMHD), becomes considerably simpler and more tractable when circularly polarized Beltrami vectors (the eigenstates of linear HMHD) are used as the basis functions. Nonlinear HMHD is, then, reduced to a rather simple looking set of scalar equations from which a model problem of three interacting Beltrami modes is formulated and analytically solved. The triplet interactions span a variety of familiar nonlinear processes leading to a redistribution as well as periodic exchange of energy. The energy exchange processes (whose strength is measured by an energy exchange/depletion time) will, perhaps, play a dominant role in determining the spectral content of an eventual Alfvenic state. All nonlinearities (sensitive functions of the interacting wave vectors) operate at par, and none is dominant over any substantial region of k-space; their intricate interplay prevents a “universal” picture from emerging; few generalizations on the processes that may, for instance, lead to a turbulent state, are possible. However, the theory can definitely claim: (1) the energy tends to flow from lower to higher k and (2) the higher k z (in the direction of the ambient magnetic field) components of a mode with a given k are depleted/oscillate faster—in some cases much faster. It is noteworthy that the mode coupling is the strongest (with the shortest depletion time) when the participating wave vectors are nearly perpendicular; perhaps, an expected consequence of the curl (cross product) nonlinearities. Numerical simulations will be necessary to help create a fully reliable picture.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Exciton-vibrational dynamics induces efficient self-trapping in a substituted nanoring

Cycloparaphenylenes, being the smallest segments of carbon nanotubes, have emerged as prototypes of the simplest carbon nanohoops. Their unique structure–dynamics–optical properties relationships have motivated a wide variety of synthesis of new related nanohoop species. Studies of how chemical changes, introduced in these new materials, lead to systems with new structural, dynamics and optical properties, expand their functionalities for optoelectronics applications. Herein, we study the effect that conjugation extension of a cycloparaphenylene through the introduction of a satellite tetraphenyl substitution has on its structural and dynamical properties. Our non-adiabatic excited state molecular dynamics simulations suggest that this substitution accelerates the electronic relaxation from the high-energy band to the lowest excited state. This is partially due to efficient conjugation achieved between specific phenyl units as introduced by the tetraphenyl substitution. We observe a particular exciton redistribution during relaxation, in which the tetraphenyl substitution plays a significant role. As a result, an efficient inter-band energy transfer takes place. Besides, the observed phonon-exciton interplay induces a significant exciton self-trapping. Finally, our results encourage and guide the future studies of new phenyl substitutions in carbon nanorings with desired optoelectronic properties.

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

3D simulations of inertial confinement fusion implosions part 1: inline modeling of polarized cross beam energy transfer and subsequent drive anomalies on OMEGA and NIF

Inertial confinement fusion experiments are sensitive to cross-beam energy transfer (CBET), a laser-plasma instability that redistributes laser energy in the coronal plasma through self-generated ion acoustic wave (IAW) gratings. The detailed CBET coupling depends on the polarization state of the crossing wavefields. CBET itself can also scramble the beam polarizations by inducing ellipticity through the IAW grating, and rotating the seed polarization toward that of the pump. We develop a ray-based model that describes the polarized CBET coupling and that is compatible with the framework of 3D inline radiative hydrodynamics simulations. The model is implemented in the ASTER/IFRIIT code and verified against an academic test case and an offline polarized CBET post-processor. It is then applied to the detailed configuration of the distributed polarization rotator system on OMEGA, where results highlight how polarized CBET induces significant low modes in the collisional absorption source term. Finally, the modeling is applied to a simple indirect-drive configuration, comparing CBET calculations with 96 unpolarized or polarized beams with 24 unpolarized quads. It is shown that these cases produce similar power amplification per cone of beams grouped with similar polar angles. However, the 96 beam geometry itself is found to reduce azimuthal variations in quad power after the interaction and favors beams with larger polar angles within the cones, an effect that is amplified by the polarized CBET. Application of the model to inline calculations of OMEGA implosions are presented in a companion paper.

3D inline modeling↗
DOE OSTI2026

Sub-melt nanosecond pulsed-laser induced densification and strain-field relaxation in single-crystal diamond

Dislocations and polishing-induced defect networks in synthetic diamond introduce local strain fields and broaden Raman features, limiting performance in optical, thermal, and electronic applications. Laser annealing is emerging as a promising approach to repair surface and near-surface defects in diamond without entering the melt regime, yet surface densification, defect-state modification, and associated structural changes have not been well quantified. In this work, we show that sub-melt nanosecond pulsed-laser annealing (PLA) induces near-surface densification and defect-mediated strain relaxation in single-crystal Chemical Vapor Deposition (CVD) diamond. Single- and two-pulse PLA were applied, and structural evolution was quantified using co-registered ISO 25,178 white-light interferometry, depth-resolved Raman spectroscopy, and cross-sectional STEM with geometric phase analysis (GPA). Across a 5 × 6 grid (n = 30), responsive regions exhibit large reductions in local slope (Sdq 45–65%), developed area (Sdr 60–90%), height spread (Sp, Sz 30–65%), void volume (Vv 57–60%), and roughness amplitude (Sa, Sq 48–57%), consistent with densification of ∼4–6.5 nm. Raman profiling shows narrowing of the diamond line and improved spectral uniformity to depths of ∼2–3 μm. Given that the Raman probing depth significantly exceeds the densified layer thickness, this response is interpreted as consistent with long-range strain-field redistribution originating from the near-surface region. STEM-GPA strain maps further support this interpretation, showing smoother strain fields, suppressed hotspots, and redistribution of localized strain concentrations following PLA. These results are consistent with defect-mediated strain relaxation and densification-driven modification of the near-surface energy state. The approach provides a scalable pathway for improving near-surface structural quality in diamond relevant to electronic, photonic, and quantum applications.

Areal surface metrology (ISO 25,178)↗
DOE OSTI2026

Excited-state vibronic coherences and intramolecular charge transfer dynamics of the photoinactive cyanobacteriochrome NpF2164g5

We have characterized the excited-state structural dynamics that follow optical excitation of the photoinactive cyanobacteriochrome (CBCR) NpF2164g5 to determine the first events along the photoisomerization reaction coordinate of the phycocyanobilin (PCB) chromophore in red-to-green photoactive CBCRs. Within 25 fs of photoexcitation to the first excited singlet state, S1, a cross peak begins to develop below the diagonal of the broadband two-dimensional electronic spectrum (2DES) owing to the formation of a twisted conformation of the PCB chromophore with an enhanced intramolecular charge-transfer (ICT) character. Excited-state coherent wavepacket motions, including a torsion of the methine bridge between rings C and D and the carbon–hydrogen out-of-plane (HOOP) wagging vibration, are rapidly damped as the cross peak forms. This finding supports an assignment of the torsional and HOOP modes to the reaction coordinate of a coherent nonadiabatic mechanism. The ICT process is accompanied by an ultrafast Stokes shift and rapidly damped oscillations at the torsional mode’s frequency, which are sensed by measurements of the energy gap of the cross peak using its first moment with respect to the detection frequency axis of the 2DES spectrum. Furthermore, these results have the further implication that polar side chains of nearby amino acid residues in the binding site of the PCB chromophore can manipulate the barrier height for photoisomerization in red-to-green photoactive CBCRs and in phytochromes by redistributing the π-electron density along the methine bridge between the C and D rings.

Charge transfer↗
DOE OSTI2026

Shifting Valencies and Magnetic Responses in La-Based High-Entropy Oxide Perovskite Thin Films with Variable Mn Presence

Chemical disorder in compositionally complex perovskite oxides generates a broad distribution of exchange pathways and spin states, but the microscopic origin and spatial homogeneity of the resulting magnetic phases remain debated. Here, we tune the Mn fraction (x = 0.2–0.6) in epitaxial La(Cr, Mn, Fe, Co, Ni)O3 thin films and resolve the coupled evolution of valence, spin state, and magnetism using element-specific x-ray absorption spectroscopy and x-ray magnetic circular dichroism (XMCD). Mn enrichment drives an internal redistribution of charge, in which Mn evolves toward a Mn3+-rich mixed valence, while Co converts from predominantly Co3+ to high-spin Co2+. This valence/spin-state coupling amplifies the Mn- and Co-derived ferromagnetic response by nearly an order of magnitude while increasing the magnetic onset temperature to at least 250 K, whereas Fe and Cr remain essentially trivalent with weak dichroism. Depth-resolved low-energy muon spin spectroscopy (LE-μSR) shows magnetic homogeneity through the film thickness, with a secondary relaxation maximum near 25 K indicating a low-temperature dynamical crossover consistent with frustrated magnetism in a strongly disordered spin lattice.

Miertschin, Duncan [Baylor University]↗
DOE OSTI2025

Scalable multilevel Monte Carlo methods exploiting parallel redistribution on coarse levels

Here, we study an element agglomeration coarsening strategy that requires data redistribution at coarse levels when the number of coarse elements becomes smaller than the number of MPI processes used on the finest level. The overall procedure generates coarse elements (general unstructured unions of fine grid elements) within the framework of element-based algebraic multigrid methods (or AMGe) studied previously. The AMGe-generated coarse spaces have the ability to exhibit approximation properties of the same order as the fine-level spaces since by construction they contain the piecewise polynomials of the same order as on the fine level. These approximation properties are key for the successful use of AMGe in multilevel solvers for nonlinear partial differential equations as well as for multilevel Monte Carlo (MLMC) simulations. The ability to coarsen without being constrained by the number of MPI processes, as described in the present paper, allows to improve the scalability of these solvers as well as the overall MLMC method. The paper illustrates this latter fact with detailed scalability study of MLMC simulations applied to model Darcy equations with a stochastic log-normal permeability field.

AMGe↗
DOE OSTI2022

Initial transient stage of pin-to-pin nanosecond repetitively pulsed discharges in air

In this work, evolution of parameters of nanosecond repetitively pulsed (NRP) discharges in pin-to-pin configuration in air was studied during the transient stage of initial 20 discharge pulses. Gas and plasma parameters in the discharge gap were measured using coherent microwave scattering, optical emission spectroscopy, and laser Rayleigh scattering for NRP discharges at repetition frequencies of 1, 10, and 100 kHz. Memory effects (when perturbations induced by the previous discharge pulse would not decay fully until the subsequent pulse) were detected for the repetition frequencies of 10 and 100 kHz. For 10 kHz NRP discharge, the discharge parameters experienced significant change after the first pulse and continued to substantially fluctuate between subsequent pulses due to rapid evolution of gas density and temperature during the 100 μs inter-pulse time caused by intense redistribution of the flow field in the gap on that time scale. For 100 kHz NRP discharge, the discharge pulse parameters reached a new steady-state at about five pulses after initiation. Further, this new steady-state was associated with well-reproducible parameters between the discharge pulses and substantial reduction in breakdown voltage, discharge pulse energy, and electron number density in comparison to the first discharge pulse. For repetition frequencies 1–100 kHz considered in this work, the memory effects can be likely attributed to the reduction in gas number density and increase in the gas temperature that cannot fully recover to ambient conditions before subsequent discharge pulses.

42 ENGINEERING↗
DOE OSTI2026

Ultrafast x-ray scattering of photodissociation dynamics in 2-iodothiophene

Here, a time-resolved x-ray scattering (TRXS) investigation of the photodissociation dynamics of gas-phase 2-iodothiophene molecules following 252 nm excitation is presented. Structural evolution of the molecule and dynamical information on the resulting photofragments were captured using femtosecond x-ray free-electron laser pulses. Two dissociation pathways were identified, arising via excitation to ππ* and (n/π)σ* states, respectively, yielding distinct interfragment recoil velocities of ∼6.4 Åps −1 and 17.0 Åps −1 . A comparison of asymptotic scattering data with simulated patterns indicates that the thiophene ring remains closed following dissociation at this wavelength. Modeling the experimental data yields a branching ratio of ∼3:1 in favor of the high velocity channel. These findings demonstrate the capability of TRXS to disentangle concurrent ultrafast reaction pathways and provide detailed structural insight into energy redistribution during photoinduced bond fission in complex molecular systems.

Razmus, Weronika O. [Univ. of Southampton (United ↗
DOE OSTI2021

Ultrafast conformational dynamics of Rydberg-excited N -methyl piperidine

We have observed the ultrafast conformational dynamics of electronically excited N-methyl piperidine (NMP) using time-resolved Rydberg fingerprint spectroscopy. Optical excitation at various wavelengths ranging from 212 nm to 229 nm leads to the 3s or 3p Rydberg states and induces coherent oscillatory motions with periods of about 700 fs. Furthermore, these coherent motions survive the internal conversion from 3p to 3s but then dephase on a time scale of a few oscillations. Intramolecular vibrational energy redistribution on a picosecond time scale leads to an equilibrium between two conformeric structures that are separated in binding energy by 0.09 eV. Model calculations using the DFT-SIC method are in excellent agreement with the experiments and identify the conformers as the chair and twist structures of NMP. The analysis of the equilibrium parameters at long time delays as a function of excitation wavelength allows for the extraction of thermodynamic parameters for the conformeric transformation. We derive an enthalpy of the chair to twist reaction in the 3s excited state of 62 meV with an entropy of 19.70 J mol –1 K –1 . An activation energy of 276 meV is also obtained with a kinetic model.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Anomalous stability of non-van der Waals bonded B4C nanosheets through surface reconstruction

Boron carbide (B4C) has been well studied both theoretically and experimentally in its bulk form due to its exceptional hardness and use as a high-temperature thermoelectric. However, the properties of its two-dimensional nanosheets are not well established. In this paper, using van der Waals-corrected density-functional theory simulations, we show that bulk B4C can be cleaved along different directions to form B4C nanosheets with low formation energies. We find that there is minimal dependence of formation energies on cleavage planes and surface terminations, even though the bulk is not van der Waals layered. This anomalous stability of B4C nanosheets is found to be a result of surface reconstructions that are unique to B-rich systems. While the density of states of the bulk B4C indicate that it is a semiconductor, the B4C nanosheets are found to be predominantly metallic. We attribute this metallic behavior to a redistribution of charges on the surface bonds of the films. The Seebeck coefficients of the B4C films remain comparable to those of the bulk and are nearly constant as a function of temperature. Our results provide guidance for experimental synthesis efforts and future application of B4C nanosheets in nanoelectronic and thermoelectric applications.

Physics↗
DOE OSTI2025

Symmetrization of Strong Hydrogen Bond under High Pressure in Bihydroxide-Ion-Containing NaCu 2 (SO 4 ) 2 ·H 3 O 2 Revealed by Experimental Charge Density, Single-Crystal Electron Diffraction, and Neutron Diffraction Studies

In minerals and inorganic compounds, strong hydrogen bonding can lead to the formation of complex ionic species such as the H 3 O 2 – bihydroxide anion and Zundel cation H 5 O 2 + . We studied [NaCu 2 (SO 4 ) 2 ·H 3 O 2 ] natrochalcite, which contains bihydroxide anions and undergoes hydrogen bond symmetrization at the lowest pressure reported so far among inorganic compounds. Hydrogen bond symmetrization leads to changes in the bulk modulus, seismic wave velocities, and proton mobility and plays a primary role in high-temperature superconductivity, but its characteristics are not well understood due to a lack of systematic studies and limitations of experimental methods sensitive to this subtle change. In this work, we applied experimental charge density analysis based on in situ single-crystal X-ray diffraction data, along with the single-crystal neutron and electron diffraction experiments, to probe the behavior of hydrogen atoms during the hydrogen bond symmetrization process under high-pressure conditions. On the way to the symmetrical H-bonding, natrochalcite undergoes a series of complex redistributions of electron density, which we trace with multipole refinement and detailed analysis of changes in the Laplacian of electron density values. Additionally, we deconvoluted the equation of state (volume of the unit cell vs pressure relation) into the atomic equation of states describing dependencies of atomic charges or volumes vs pressure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Dynamic Surface Restructuring in Cu(Au) Alloys Driven by Oxygen-Mediated Au Mobility

Alloying plays a crucial role in tuning the surface properties of metals, but the atomic-level mechanisms by which alloying elements influence surface structure dynamics under reactive conditions remain elusive. Using Cu(Au) in oxidizing environments as a model system, we reveal a dynamic oxygen-induced transformation of the topmost atomic layer into a periodically hill-and-valley morphology with reversible switching between undulated and flattened surface states. These interconversions are driven by the retreat of surface Au to the subsurface during oxygen adsorption and its resegregation to the surface upon oxygen desorption. This cyclical mobility establishes a feedback loop, allowing the surface to dynamically reconfigure in response to changes in the oxygen pressure. The results offer a broadly applicable framework for understanding atomic-scale surface restructuring in alloy systems, where differences in the chemical reactivity of alloying elements drive dynamic redistribution between surface and subsurface regions. As a result, this dynamic coupling has practical implications for designing corrosion-resistant coatings and metastable nanostructures with tunable catalytic properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Porous Flow Modeling of Axial Gas Redistribution in Fragmented LWR Fuel Rods using MOOSE

Understanding how gas axially redistributes within fragmented fuel pellets is crucial for predicting the behavior of Light Water Reactor (LWR) fuel rods, particularly during transient and accidental scenarios. The time scale of this phenomenon plays a fundamental role in determining the progression and hazard of a Loss Of Coolant Accident (LOCA), especially when high burn-up fuel in a severe state of fragmentation is involved. Here, this study presents a Computational Fluid Dynamics (CFD) model developed within the Multiphysics Object-Oriented Simulation Environment (MOOSE) to predict the time-scale of plenum depressurization in Light-Water Reactor (LWR) fuel rods driven by axial gas transport through fragmented pellets. The model examines the effects of incorporating non-linearities in the friction term by comparing the results with experimental data. The experiment employed surrogate fuel rods containing pellets subjected to mechanical and/or thermal loadings to simulate various severity of cracking, and aimed at studying the influence of fuel conditions on axial gas redistribution. The results of this analysis indicate that under certain flow regime conditions - determined by the value of an equivalent Reynolds number - accounting for the non-linear friction term in Navier-Stokes equations guarantees better predictions for the time-scale of plenum depressurization. Also, the model enabled the simulation of the pressure decay by assigning distinct permeability values to each pellet instead of a single uniform value. Multiple simulations were run across all possible pellet position combinations, having each pellet assigned with values of permeability extracted from the experimental data. This allows to quantify the impact of the considering various non-uniform distributions of permeability on the dynamics of axial gas redistribution. The present work findings enhance the understanding of axial gas transport, and provide valuable insights for the integration of a model for predicting the axial gas redistribution during a LOCA scenario into the BISON fuel performance code.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗