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

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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Revisiting Artifacts of Kohn–Sham Density Functionals for Biosimulation

We revisit the problem of unphysical charge density delocalization/fractionalization induced by the self-interaction error of common approximate Kohn–Sham (KS) density functional theory functionals on simulation of small to medium-sized proteins in a vacuum. Aside from producing unphysical electron densities and total energies, the vanishing of the HOMO–LUMO gap associated with the unphysical charge delocalization leads to an unphysical low-energy spectrum and catastrophic failure of most popular solvers for the KS self-consistent field (SCF) problem. We apply a robust quasi-Newton SCF solver to obtain solutions for some of these difficult cases. The anatomy of the charge delocalization is revealed by the natural deformation orbitals obtained from the density matrix difference between the Hartree–Fock and KS solutions; the charge delocalization not only can occur between charged fragments (such as in zwitterionic polypeptides) but also involves neutral fragments. The vanishing-gap phenomenon and troublesome SCF convergence are both attributed to the unphysical KS Fock operator eigenspectra of molecular fragments (e.g., amino acids or their side chains). Analysis of amino acid pairs suggests that the unphysical charge delocalization can be partially ameliorated by the use of some range-separated hybrid functionals but not by semilocal or standard hybrid functionals. Last, we demonstrate that solutions without the unphysical charge delocalization can be located even for semilocal KS functionals highly prone to such defects, but such solutions have non-Aufbau character and are unstable with respect to mixing of the non-overlapping “frontier” orbitals. Caution should be exercised when unexpectedly small (or vanishing) HOMO–LUMO gaps and atypical SCF convergence patterns (e.g., oscillatory) are observed in KS DFT simulations in any context (bio or otherwise).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Field-Coupled Water Splitting with Metal-Free Donor–Acceptor Covalent Organic-Framework Junctions

Advancing metal-free electrocatalysts for hydrogen and oxygen evolution reactions (HER/OER) across acidic and alkaline media requires coordinated control of intermediate binding thermodynamics, interfacial charge delivery, and near-electrode transport dynamics. Here, we design amide-linked benzene–triazine covalent organic frameworks (BTA/TzTA-Hz COFs) and integrate them with carbon nanotubes (CNTs) to form COF–CNT junctions that establish a built-in interfacial electric field. Density functional theory (DFT) and electrostatic potential maps indicate complementary active motifs, with benzene-proximal fragments associated with HER and triazine-proximal motifs associated with OER. CNT integration shifts the contact-potential difference by ≈0.20 V, while operando electrochemical impedance spectroscopy suggests partially separable high-frequency junction-charging and lower-frequency Faradaic/transport responses. A 300 mT static magnetic field lowers the HER and OER overpotentials by tens of millivolts. Under anodic bias, the effective interfacial charging capacitance increases, and Mott–Schottky analysis shows an apparent ∼0.15 V flat-band shift with an essentially unchanged slope. Together, these observations are consistent with field-perturbed interfacial charging and altered bias partitioning. Field-dependent impedance and bubble imaging are consistent with magnetohydrodynamic convection that promotes bubble detachment and near-electrode mass transport for both half-reactions, and they reveal an OER-specific high-frequency perturbation under anodic bias. Under field, the heterostructure reaches an OER onset overpotential of ∼261 mV and requires an overpotential of 366 mV at 10 mA cm –2 in alkaline electrolyte. These results illustrate how reticular-framework chemistry, junction engineering, and both built-in and applied fields can program reactivity through interfacial electrostatics and near-electrode transport in organic-framework electrocatalysts.

Garcia-Enriquez, Lissette [Univ. of Texas at El Pa↗
DOE OSTI2024

IRIS: Exploring Performance Scaling of the Intelligent Runtime System and its Dynamic Scheduling Policies

High-Performance Computing is becoming increasingly heterogeneous, relying on a diverse mix of hardware to achieve good performance. Paradoxically, current drivers and frameworks for these devices typically require separate languages and implementations for each vendor. Furthermore, there are few tools and little support to schedule codes between these devices in a truly heterogeneous manner-partly because of this fragmentation between vendors and the languages each supports. To overcome both limitations, the Intelligent Runtime System (IRIS) was developed. It allows a common task abstraction to automatically be shared among contemporary vendors and is run from a single host-side API. At runtime, IRIS queries the host system and registers which frameworks and drivers are available, these determine which kernels can be used by the scheduler-CPUs via OpenMP, Nvidia GPUs (CUDA), AMD GPUs (HIP), and Intel and Xilinx FPGAs with OpenCL. IRIS enables tasks to be scheduled to any heterogeneous device and resolves to the appropriate kernel binary at runtimeit only uses the devices supported by the system on which it is run. IRIS supports single-task and graph-based expressions of dependencies of tasks. Additionally, IRIS features a range of dynamic scheduling policies, allowing complex chains of tasks and interactions to be executed, relieving the programmer/user from considering the system to assign tasks to devices optimally. This paper presents the peak performance attainable by IRIS over a range of systems-each with different numbers and types of accelerator devices, it highlights the flexibility of IRIS since these devices are truly heterogeneous, relying on different backends (drivers, frameworks, and languages) which historically required unique implementations to utilize them. We then use this peak performance as a baseline to compare increasingly complex chains of tasks (with increasingly complex task dependencies) and evaluate how IRIS copes. Finally, we consider the performance of different IRIS scheduling policies on this range of task graphs.

Johnston, Beau↗
DOE OSTI2020

Status, Challenges, and Plans for Consistent Modeling and Evaluation of Fission Data: Nubar, PFNS, and FPY [Slides]

This presentation discusses the importance of consistent evaluations for fission observables. Currently, prompt fission quantities (e.g., neutron multiplicity, neutron energy spectrum, and fission product yields) are evaluated independently of one another, either with separate models or data-only/non-model evaluations (few – if any – shared model inputs) and inconsistencies can arise in evaluated data (e.g. NSE 190, 258 (2018)). They have found that consistent, model-based evaluations lead to more physical constraints on free parameters in the model, more robust predictions for other observables and other isotopes, that there are correlations between the uncertainties on different observables, and that uncertainties can be propagated to unmeasured quantities. They are working on developing models to the point where fission observables are calculated at the quality needed for an evaluation. They are striving to consistently calculate fission observables, such as $\bar{v}$, PFNS, and FPY, to a quality suitable for an evaluation. Current evaluations for fission observables use separate models for each observable (with minimal shared input) or are purely data driven. LANL models, such as the Monte Carlo CGMF and deterministic BeoH, have different strengths; the similar fission fragment initial conditions and decay models leads to consistency between the two codes (FPY can be connected to $\bar{v}$ and PFNS, even when calculated by different codes). Work is underway by Lovell to optimize the models and Neudecker is working to perform detailed uncertainty quantification. The PFNS, in particular, presents a significant challenge.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

A Dual-Gated Structures for Lossless Ion Manipulations-Ion Mobility Orbitrap Mass Spectrometry Platform for Combined Ultra-High-Resolution Molecular Analysis

High-resolution ion mobility spectrometry-mass spectrometry (HR-IMS-MS) instruments have enormously advanced the ability to characterize complex biological mixtures. Unfortunately, HR-IMS and HR-MS measurements are typically performed independently due to mismatches in analysis time scales. Here we overcome this limitation by using a dual-gated ion injection approach to couple an 11-meter path length structures for lossless ion manipulations (SLIM) module to a Q-Exactive Plus Orbitrap MS. The dual-gate setup was implemented by placing one ion gate before the SLIM module and a second ion gate after. The dual-gated ion injection approach allowed the new SLIM-Orbitrap platform to simultaneously perform an 11-meter SLIM separation, Orbitrap mass analysis using the highest selectable mass resolution setting (up to 140k), and high-energy collision induced dissociation (HCD) in ~25 minutes over an $m/z$ range of ~1500 amu. The SLIM-Orbitrap was initially characterized using a mixture of standard phosphazene cations and demonstrated an average SLIM CCS resolving power (Rp CCS ) of ~218 and SLIM peak capacity of ~156 while simultaneously obtaining high mass resolutions. SLIM-Orbitrap analysis with fragmentation was then performed on mixtures of standard peptides and two reverse peptides (SDGRG 1+ , GRGDS 1+ , Rp CCS = 305) to demonstrate the utility of combined HR-IMS-MS/MS measurements for peptide identification. Our new HR-IMS-MS/MS capability was further demonstrated by analyzing a complex lipid mixture and showcasing SLIM separations on isobaric lipids. In conclusion, this new SLIM-Orbitrap platform demonstrates a critical new capability for proteomics and lipidomics applications, and the high-resolution multimodal data obtainable with this system establishes the foundation for reference-free identification of unknown ion structures.

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

Discovery of new isotopes in the fragmentation of 82 Se and insights into their production

The production cross sections of neutron-rich nuclei for elements just above 60 Ca were measured at the Facility for Rare Isotope Beams (FRIB). Four previously unobserved isotopes ( 63 Sc, 65,66 Ti, and 68 V) were produced, separated, and identified for the first time using the Advanced Rare Isotope Separator (ARIS). One event was found to be consistent with 61 Ca . The new isotopes were created through the interaction of an 82 Se beam with a carbon target at an energy of 228 MeV/𝑢 and a primary beam current of 1.07 p⁢µ⁢A. The event-by-event particle identification of the mass number (𝐴), atomic number (𝑍), and ionic charge state (𝑞) for the reaction products was achieved by combining measurements of energy loss, time of flight, magnetic rigidity, and total kinetic energy. This successful search for new isotopes, conducted at the beginning of FRIB's third year of operation, highlights the facility's discovery potential, which will continue to grow as the beam current increases. The production cross sections were analyzed in the context of the newly developed Δ⁢𝐵⁢𝐸 systematics that provides trends in neutron-rich regions and increased sensitivity to nuclear binding, an important nuclear structure observable. Furthermore, the new systematics addresses gaps in 𝑄 𝑔 -based methods commonly used to interpret the production cross sections of light neutron-rich elements, and provides an efficient empirical approach to describe cross-section trends across isotopic chains. Good agreement with the measured data was obtained when the Δ⁢𝐵⁢𝐸 systematics and abrasion-ablation calculations were performed using the Hartree-Fock-Bogoliubov (HFB-22) mass table.

59 ≤ A ≤ 89↗
DOE OSTI2022

Westinghouse Accident Tolerant Fuel Phase 2B with Higher Enriched and Higher Burnup Add-On Project Final Technical Report Deliverable Volume 1

The Westinghouse Electric Company LLC (Westinghouse) accident tolerant fuel (ATF) program funded by Westinghouse and the US Department of Energy (DOE) utilized chromium (Cr) coated zirconium alloy cladding with doped UO 2 (ADOPT(TM)) and uranium silicide (U 3 Si 2 ) high density/high thermal conductivity fuel for its lead test rod (LTR) program with irradiation beginning in 2019. ADOPT is a Cr 2 O 3 +Al 2 O 3 doped UO 2 pellet with increased oxidation resistance and density, and increased resistance to fission gas release. Due to the issues with U 3 Si 2 fuel reaction in pressurized water reactor (PWR) environments, uranium nitride (U 15 N) has been substituted for U 3 Si 2 as a long-term fuel option. Cr coated cladding with ADOPT fuel is the near-term Westinghouse EnCore fuel product. The long-term EnCore ® fuel product is SiGA ® SiC/SiC composite cladding with high density/high thermal conductivity UN fuel. In 2020, the higher burnup and higher enriched and (HBHE) program was integrated into the ATF program. The objective of this expanded program is to extend ATF burnups to at least 75 MWd/kgU to economically facilitate 24-month cycles in PWRs. The ATF program now includes ADOPT fuel with enrichments >5% 235 U. Over the past several years, Westinghouse has tested the Cr coated zirconium (Zr) and silicon carbide (SiC) claddings in Westinghouse Churchill autoclaves and the Massachusetts Institute of Technology (MIT) reactor. Additionally, the Cr coated cladding has been tested in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) and in LTR programs at the Doel 4 and Bryon 2 commercial reactors. High temperature tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried out to determine the time and temperature limits for the Cr coated zirconium claddings. These tests indicate that Cr coated Zr cladding can take temperatures up to about 1500°C for short periods of time without becoming totally oxidized. The main issue is the formation of the Cr-Zr eutectic at 1333°C resulting in the migration of this eutectic inward with the formation of ZrCr 2 which rapidly oxidizes to ZrO 2 on the outside of the tube. The Cr coated Zr cladding also delays the bursting of the tube, reduces the burst area, and reduces hydriding and embrittlement of the Zr which is a major benefit for reducing fuel fragmentation, redistribution, and dispersal (FFRD), the major licensing issue faced by HBHE. The manufacturing parameters for the SiC have been found to have a significant effect on the corrosion rate of the SiC in light water reactor (LWR) conditions and significant improvements have been made in the yield, quality, and oxidation resistance of the SiC cladding by identifying and tightening manufacturing process parameters. Current autoclave results for SiC composite claddings indicate that a corrosion rate of fewer than 2 micrometers per year can be achieved which meets corrosion requirements under normal operating conditions. High temperature steam oxidation tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried and determined that SiC cladding can withstand temperatures up to about 1800°C to 1900°C before excessive corrosion reactions begin, and that the SiC will not balloon and burst. ADOPT fuel pellets were incorporated into the Westinghouse ATF program because of their increased density and oxidation resistance. A topical report supporting the use of ADOPT pellets has been submitted to the NRC and will be approved shortly. ADOPT pellets have been a product in Europe for over 15 years. The additives work to make larger grain sizes which appear to reduce fission gas release during transients as well as increase the density of the pellet. Fuel rod and assembly design in preparation for the lead test rod (LTR) and lead test assembly (LTA) programs is underway as well as licensing efforts with the Nuclear Regulatory Commission (NRC). Finally, accident analyses coupled with economic evaluations for both operating savings as well as fuel savings have been initiated. Modular Accident Analysis Program 5 (MAAP5) calculations indicate that both Cr coated cladding and SiC composite cladding can increase the time to fuel rod loss of geometry for up to two hours longer than current Zr based cladding in a station blackout scenario. This additional time is due to the much higher oxidation resistance of the SiC and Cr coated cladding. These two hours can be used to implement additional response options instituted through the Diverse and Flexible Mitigation Capability (FLEX) program by reactor operators. Both ATF cladding options also reduce hydrogen production which dramatically reduces primary system and containment pressure and the risk of fission product release beyond containment in the unlikely event of an accident. The lower pressure in the system allows more time to feed cooling water to the core, resulting in the avoidance of fuel melting. The coping time is extended indefinitely if the modest water flow provided by FLEX continues. Experimental work on methods to rapidly fabricate SiC composite structures with high density and reduce the fabrication price of SiC fibers while maintaining a high level of performance is needed. Methods for mitigating or stopping the Cr-Zr eutectic are also needed to further improve the oxidation resistance of Cr coated Zr. Minimal (<1%) swelling of U 3 Si 2 and subsequent fission gas release has been demonstrated up to 20 MWd/kgU. Irradiation experiments with U 3 Si 2 fuel in ATR to determine these properties at 40 MWd/kgU were completed but post irradiation examinations were not done since U 3 Si 2 has been replaced by UN. UN has three issues that are being addressed. The first is increasing the oxidation resistance so that there is not excessive reaction up to ~1500°C. While UN increases the pellet density and additives to the UN postponed the temperature at which rapid oxidation occurred by ~100°C to 200°C, this is not enough, and pellet coating options are now being pursued. The second is developing a method to manufacture that does not require the multi-step process of UF 6 to UO 2 to UC to UN. Efforts are underway looking at UF 6 to UN 2 to UN and UF 6 to UF 4 to UN 2 to UN reactions. Finally, an economically acceptable process for potentially enriching the 15 N content of the nitrogen used to make UN to >95% 15N was identified though not experimentally validated. In addition to the work supported by the DOE, research and testing activities are being carried on in a world-wide effort funded by many countries such as Sweden, United Kingdom, Belgium, Netherlands, Spain, Germany, Japan, and France. This work is being facilitated through the Westinghouse led Collaboration for Advanced Research on Accident Tolerant Fuel (CARAT) program. Annual meetings were organized in 2018 and 2019 by Westinghouse as a venue for presentation of this work and to provide for the cross-fertilization of ideas among the many outstanding researchers in the ATF area. No meetings were held in 2020 and 2021 due to the COVID-19 related restrictions on traveling and gatherings. Since SiC, coated cladding, and high-density fuel options are not currently used in the nuclear industry; support from the government and industry members is needed to further the significant effort of setting new standards. The same is true for the Nuclear Regulatory Commission (NRC) which must review and approve the commercial use of these new fuels since all current regulations are oriented toward Zr/UO 2 fuel. Several meetings have been held with the NRC to generate a fast-track approach to licensing ATF using a combination of atomic modeling, in-rod sensors, and in-reactor testing. This approach was memorialized in an “Accelerated Fuel Qualification White Paper” prepared by the Accelerated Fuel Qualification Working Group lead by General Atomics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Westinghouse Accident Tolerant Fuel Phase 2B with Higher Enriched and Higher Burnup Add-On Project Final Technical Report Deliverable Volume 2

The Westinghouse Electric Company LLC (Westinghouse) accident tolerant fuel (ATF) program funded by Westinghouse and the US Department of Energy (DOE) utilized chromium (Cr) coated zirconium alloy cladding with doped UO 2 (ADOPT(TM)) and uranium silicide (U 3 Si 2 ) high density/high thermal conductivity fuel for its lead test rod (LTR) program with irradiation beginning in 2019. ADOPT is a Cr 2 O 3 +Al 2 O 3 doped UO 2 pellet with increased oxidation resistance and density, and increased resistance to fission gas release. Due to the issues with U 3 Si 2 fuel reaction in pressurized water reactor (PWR) environments, uranium nitride (U 15 N) has been substituted for U 3 Si 2 as a long-term fuel option. Cr coated cladding with ADOPT fuel is the near-term Westinghouse EnCore ® fuel product. The long-term EnCore fuel product is SiGA ® SiC/SiC composite cladding with high density/high thermal conductivity UN fuel. In 2020, the higher burnup and higher enriched and (HBHE) program was integrated into the ATF program. The objective of this expanded program is to extend ATF burnups to at least 75 MWd/kgU to economically facilitate 24-month cycles in PWRs. The ATF program now includes ADOPT fuel with enrichments >5% 235 U. Over the past several years, Westinghouse has tested the Cr coated zirconium (Zr) and silicon carbide (SiC) claddings in Westinghouse Churchill autoclaves and the Massachusetts Institute of Technology (MIT) reactor. Additionally, the Cr coated cladding has been tested in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) and in LTR programs at the Doel 4 and Bryon 2 commercial reactors. High temperature tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried out to determine the time and temperature limits for the Cr coated zirconium claddings. These tests indicate that Cr coated Zr cladding can take temperatures up to about 1500°C for short periods of time without becoming totally oxidized. The main issue is the formation of the Cr-Zr eutectic at 1333°C resulting in the migration of this eutectic inward with the formation of ZrCr 2 which rapidly oxidizes to ZrO 2 on the outside of the tube. The Cr coated Zr cladding also delays the bursting of the tube, reduces the burst area, and reduces hydriding and embrittlement of the Zr which is a major benefit for reducing fuel fragmentation, redistribution, and dispersal (FFRD), the major licensing issue faced by HBHE. The manufacturing parameters for the SiC have been found to have a significant effect on the corrosion rate of the SiC in light water reactor (LWR) conditions and significant improvements have been made in the yield, quality, and oxidation resistance of the SiC cladding by identifying and tightening manufacturing process parameters. Current autoclave results for SiC composite claddings indicate that a corrosion rate of fewer than 2 micrometers per year can be achieved which meets corrosion requirements under normal operating conditions. High temperature steam oxidation tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried and determined that SiC cladding can withstand temperatures up to about 1800°C to 1900°C before excessive corrosion reactions begin, and that the SiC will not balloon and burst. ADOPT fuel pellets were incorporated into the Westinghouse ATF program because of their increased density and oxidation resistance. A topical report supporting the use of ADOPT pellets has been submitted to the NRC and will be approved shortly. ADOPT pellets have been a product in Europe for over 15 years. The additives work to make larger grain sizes which appear to reduce fission gas release during transients as well as increase the density of the pellet. Fuel rod and assembly design in preparation for the lead test rod (LTR) and lead test assembly (LTA) programs is underway as well as licensing efforts with the Nuclear Regulatory Commission (NRC). Finally, accident analyses coupled with economic evaluations for both operating savings as well as fuel savings have been initiated. Modular Accident Analysis Program 5 (MAAP5) calculations indicate that both Cr coated cladding and SiC composite cladding can increase the time to fuel rod loss of geometry for up to two hours longer than current Zr based cladding in a station blackout scenario. This additional time is due to the much higher oxidation resistance of the SiC and Cr coated cladding. These two hours can be used to implement additional response options instituted through the Diverse and Flexible Mitigation Capability (FLEX) program by reactor operators. Both ATF cladding options also reduce hydrogen production which dramatically reduces primary system and containment pressure and the risk of fission product release beyond containment in the unlikely event of an accident. The lower pressure in the system allows more time to feed cooling water to the core, resulting in the avoidance of fuel melting. The coping time is extended indefinitely if the modest water flow provided by FLEX continues. Experimental work on methods to rapidly fabricate SiC composite structures with high density and reduce the fabrication price of SiC fibers while maintaining a high level of performance is needed. Methods for mitigating or stopping the Cr-Zr eutectic are also needed to further improve the oxidation resistance of Cr coated Zr. Minimal (<1%) swelling of U 3 Si 2 and subsequent fission gas release has been demonstrated up to 20 MWd/kgU. Irradiation experiments with U 3 Si 2 fuel in ATR to determine these properties at 40 MWd/kgU were completed but post irradiation examinations were not done since U 3 Si 2 has been replaced by UN. UN has three issues that are being addressed. The first is increasing the oxidation resistance so that there is not excessive reaction up to ~1500°C. While UN increases the pellet density and additives to the UN postponed the temperature at which rapid oxidation occurred by ~100°C to 200°C, this is not enough, and pellet coating options are now being pursued. The second is developing a method to manufacture that does not require the multi-step process of UF 6 to UO 2 to UC to UN. Efforts are underway looking at UF 6 to UN 2 to UN and UF 6 to UF 4 to UN 2 to UN reactions. Finally, an economically acceptable process for potentially enriching the 15 N content of the nitrogen used to make UN to >95% 15 N was identified though not experimentally validated. In addition to the work supported by the DOE, research and testing activities are being carried on in a world-wide effort funded by many countries such as Sweden, United Kingdom, Belgium, Netherlands, Spain, Germany, Japan, and France. This work is being facilitated through the Westinghouse led Collaboration for Advanced Research on Accident Tolerant Fuel (CARAT) program. Annual meetings were organized in 2018 and 2019 by Westinghouse as a venue for presentation of this work and to provide for the cross-fertilization of ideas among the many outstanding researchers in the ATF area. No meetings were held in 2020 and 2021 due to the COVID-19 related restrictions on traveling and gatherings. Since SiC, coated cladding, and high-density fuel options are not currently used in the nuclear industry; support from the government and industry members is needed to further the significant effort of setting new standards. The same is true for the Nuclear Regulatory Commission (NRC) which must review and approve the commercial use of these new fuels since all current regulations are oriented toward Zr/UO 2 fuel. Several meetings have been held with the NRC to generate a fast-track approach to licensing ATF using a combination of atomic modeling, in-rod sensors, and in-reactor testing. This approach was memorialized in an “Accelerated Fuel Qualification White Paper” prepared by the Accelerated Fuel Qualification Working Group lead by General Atomics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

A phase-field model of quasi-brittle fracture for pressurized cracks: Application to UO 2 high-burnup microstructure fragmentation

Here, in this paper, we present a phase-field model of quasi-brittle fracture with pressurized cracks, with dedicated applications for polycrystalline materials. The model is formulated as a minimization problem within the variational framework. The external work done by pressure on the crack surfaces is included in the objective function. Several careful modeling choices lead to a regularization-length-independent critical strength. The model is constructed to give a softening response with an underlying linear traction-separation law. The pressure-dependent softening response and the regularization of the prescribed pressure are demonstrated with a (quasi) one-dimensional numerical analysis. In a two-dimensional numerical analysis under plane strain assumptions, the critical stress corresponding to crack propagation (as predicted by our quasi-brittle fracture model) is compared with linear elastic fracture mechanics (LEFM) analytical solutions. Our model is further utilized to simulate fission-gas-induced fragmentation of the UO 2 high-burnup structure (HBS). Simulation results show that pressurized bubbles can cause crack nucleation and propagation, and that the bubble size and the surrounding external pressure affect the critical pressure corresponding to crack nucleation. Simulations of a partial HBS at different recrystallization stages show that different grain structures (due to recrystallization) also influence crack paths and fragmentation morphology.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Pulse Energy and Pulse Duration Effects in the Ionization and Fragmentation of Iodomethane by Ultraintense Hard X Rays

The interaction of intense femtosecond x-ray pulses with molecules sensitively depends on the interplay between multiple photoabsorptions, Auger decay, charge rearrangement, and nuclear motion. Here, we report on a combined experimental and theoretical study of the ionization and fragmentation of iodomethane (CH 3 I) by ultraintense (~10 19 W/cm 2 ) x-ray pulses at 8.3 keV, demonstrating how these dynamics depend on the x-ray pulse energy and duration. We show that the timing of multiple ionization steps leading to a particular reaction product and, thus, the product’s final kinetic energy, is determined by the pulse duration rather than the pulse energy or intensity. While the overall degree of ionization is mainly defined by the pulse energy, our measurement reveals that the yield of the fragments with the highest charge states is enhanced for short pulse durations, in contrast to earlier observations for atoms and small molecules in the soft x-ray domain. Finally, we attribute this effect to a decreased charge transfer efficiency at larger internuclear separations, which are reached during longer pulses.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Conservation laws and effective hadronization models

Hadronization models based on local string-breaking dynamics are typically Markovian by construction, yet the physical ensemble of final states is shaped by global constraints that couple the entire fragmentation trajectory. Recasting hadronization as a conditioned stochastic diffusion process provides a precise mathematical resolution to this tension. In particular, this language reveals explicitly that constraints stemming from conservation laws induce non-Markovian correlations between otherwise independent fragmentation steps, and that these correlations can be absorbed exactly into a renormalization of the local dynamics through a Doob $h$-transform. We develop this formalism for a $q\bar{q}$ string in the chiral limit, where the longitudinal-transverse factorization of the Lund kernel becomes exact, enabling systematic power counting and clean ultraviolet (UV)/infrared (IR) separation. The dynamics organize naturally into a tower of effective theories distinguished by the remaining string mass, spanning a UV fixed point with scale-invariant transport coefficients, an intermediate regime where transverse phase space induces controlled running, and an IR boundary layer where non-local effects enter at leading order. The tower exhibits genuine Wilsonian structure, including $β$-functions, anomalous dimensions, and systematic matching conditions. The resulting framework achieves a clean factorization of universal microscopic fragmentation dynamics from infrared constraint effects, and opens new directions for both the theoretical analysis and practical simulation of hadronization.

Menzo, Tony [Alabama U.; Fermilab] (ORCID:00000002↗
DOE OSTI2023

Population Subdivision in the Gopher Frog (Rana capito) across the Fragmented Longleaf Pine-Wiregrass Savanna of the Southeastern USA

Delineating genetically distinct population segments of threatened species and quantifying population connectivity are important steps in developing effective conservation and management strategies aimed at preventing extinction. The gopher frog (Rana capito) is a xeric-adapted, pond-breeding species endemic to the Gulf and Atlantic coastal plains of the southeastern United States. This species has experienced extensive habitat loss and fragmentation in the formerly widespread longleaf pine-wiregrass savanna where it lives, resulting in individual abundance declines and population extinctions throughout its range. We used individual-based clustering methods along with Bayesian inference of historical migration based on almost 1500 multilocus microsatellite genotypes to examine genetic structure in this taxon. Clustering analyses identified panhandle and peninsular populations in Florida as distinct genetic clusters separated by the Aucilla River, consistent with the division between the Coastal Plain and peninsular mitochondrial lineages, respectively. Analysis of historical migration indicated an east–west population divergence event followed by immigration to the east. Together, our results indicate that the genetically distinct Coastal Plain and peninsular Florida lineages should be considered separately for conservation and management purposes.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Elucidating Biomass-Derived Pyrolytic Lignin Structures from Demethylation Reactions through Density Functional Theory Calculations

Pyrolytic lignin is a fraction of pyrolysis oil that contains a wide range of phenolic compounds that can be used as intermediates to produce fuels and chemicals. However, the characteristics of the raw lignin structure make it difficult to establish a pyrolysis mechanism and determine pyrolytic lignin structures. Herein this study proposes dimer, trimer, and tetramer structures based on their relative thermodynamic stability for a hardwood lignin model in pyrolysis. Different configurations of oligomers were evaluated by varying the positions of the guaiacyl (G) and syringyl (S) units and the bonds βO4 and β5 in the hardwood model lignin through electronic structure calculations. The homolytic cleavage of βO4 bonds is assumed to occur and generate two free radical fragments. These can stabilize by taking hydrogen radicals that may be in solution during the intermediate liquid (pathway 1) formation before the thermal ejection. An alternative pathway (pathway 2) could occur when the radicals use intramolecular hydrogen, turning themselves into stable products. Subsequently, a demethylation reaction can take place, thus generating a methane molecule and new oligomeric lignin-derived molecules. The most probable resulting structures were studied. We used FTIR and NMR spectra of selected model compounds to evaluate our calculation approach. Thermophysical properties were calculated using group contribution methods. The results give insights into the lignin oligomer structures and how these molecules are formed. They also provide helpful information for the design of pyrolysis oil separation and upgrading equipment.

09 BIOMASS FUELS↗
DOE OSTI2021

Advancements in modeling fuel pulverization and cladding behavior during a LOCA

During a loss of coolant accident (LOCA), there is the possibility of nuclear fuel rods to undergo a three step process known as fuel fragmentation, relocation, and dispersal (FFRD). The chance of FFRD occurring increases as the fuel burnup increases. To support the nuclear industry's desire to increase the discharge burnup of nuclear fuels in light water reactors (LWRs) it is imperative to understand the mechanisms driving the evolution of FFRD. In this work, a multiscale modeling modeling approach is used to garner insight into underlying mechanisms leading to the ne fragmentation (also known as pulverization) of nuclear fuel during a LOCA. This report includes a summary of the atomistic and phase-field studies to develop a new pulverization criterion for use in the engineering scale Bison fuel performance code. Details are also provided on cladding modeling improvements related to hydrogen/hydride embrittlement and damage, and anisotropic thermal creep. The new models are used on the existing integral and separate effects LOCA validation cases available in Bison.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Comparison of Gas Phase Fragmentation Behaviors of Nuclear Fuel Cycle Ligands in Lanthanide and Americium Metal Ligand Nitrate Clusters

Introduction (120 words): Transport of metal ions across the aqueous-organic phase boundary is an essential step in a hydrometallurgical nuclear fuel reprocessing strategy. The study of transport agents for nuclear fuel elements is imperative to guide the design of ligands that boost the separation efficiency of the recovery process from fission products. However, limited studies have been made on the chemistry of these transport agents when complexing with transuranic elements in gas-phase where all surrounding factors are essentially excluded. This work investigates the reagent ligand complexations to transuranic and other metals and their dissociations in the gas phase. Comparisons are made between 4f and 5f elements and between ligands. Methods (120 words): (N,N-diisobutylcarbamoylmethyl)phenyloctylphosphine oxide (CMPO) and N,N,N',N'-tetraoctyldiglycolamide (TODGA) have been selected to complex with metal nitrates. The actinide americium and lanthanides neodymium, samarium, and europium were investigated as part of this work. The lanthanides were selected to act as size and electron configuration analogues of the minor actinides. Metal complexes with two ligands and two nitrates ([M(NO3)2(CMPO)2]+, for example) are studied in Bruker micrOTOF-Q II mass spectrometer equipped with collision-induced dissociation capability. The comparisons of the mass spectra are made in groups of homogenous ligands and mixed TODGA-CMPO ligands clusters. Comparisons are also made based on the complexed metals (Am and lanthanides). Preliminary data (300 words): Collision-induced dissociation mass spectrometry data are collected on two ligands complexed with metal nitrates where the two ligands are homogenous, with (CMPO)2 or (TODGA)2, or heterogeneous, with (TODGA)(CMPO). Several fragmentation patterns are observed among complexes with the CMPO ligand whereas the TODGA ligand commonly dissociates intact from the complex. Most of the metal complexes exhibit similar fragmentation patterns, but there are a few notable deviations in fragmentation patterns between the Am and Ln-bearing complexes. For the [M(CMPO)2(NO3)2]+ complexes, the initial loss of nitrate in the form of nitric acid is observed in all four complexes. However, [Am(CMPO)2(NO3)2]+ exhibits an additional fragmentation not found in the lanthanide complexes. Also, a significantly different ratio of the second nitric acid loss is found in the Am complex. These deviations may indicate the different interaction behaviors between actinides and lanthanides. The [M(TODGA)2(NO3)2]+ complexes exhibit the fragmentation as the loss of one TODGA ligand as an intact form and the loss of nitrate as nitric acid. The Am complex exhibits an additional fragmentation after losing the TOGDA ligand, which is not observed among the Ln complexes. The heterogeneous [M(TODGA)(CMPO)(NO3)2]+ complexes exhibit both similarities and differences between the Am and Ln complexes. For example, the heterogenous Am complex does not exhibit the loss of an intact TODGA ligand while all three Ln complexes do. This indicates that TODGA may bind more strongly to Am than Ln. Additionally, the intensity of the loss of CMPO ligand (as partially or whole) is found to be significantly larger than that of the loss of TODGA (as partially of whole) indicating that TODGA is bound to the metal significantly stronger than CMPO. Planned computational analysis will help understand the deviation in fragmentation behaviors between americium and lanthanide metal centers, or between TODGA and CMPO ligands. Novel aspect (20 words): Gas-phase actinide and lanthanide complex formation and fragmentation provide insight into the coordination environment differences of f-element metals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Understanding the Origin of Structural Diversity of DNA Double Helix

Deciphering the contribution of DNA subunits to the variability of its 3D structure represents an important step toward the elucidation of DNA functions at the atomic level. In the pursuit of that goal, our previous studies revealed that the essential conformational characteristics of the most populated “canonic” BI and AI conformational families of Watson–Crick duplexes, including the sequence dependence of their 3D structure, preexist in the local energy minima of the elemental single-chain fragments, deoxydinucleoside monophosphates (dDMPs). Those computations have uncovered important sequence-dependent regularity in the superposition of neighbor bases. The present work expands our studies to new minimal fragments of DNA with Watson–Crick nucleoside pairs that differ from canonic families in the torsion angles of the sugar-phosphate backbone (SPB). To address this objective, computations have been performed on dDMPs, cdDMPs (complementary dDMPs), and minimal fragments of SPBs of respective systems by using methods of molecular and quantum mechanics. These computations reveal that the conformations of dDMPs and cdDMPs having torsion angles of SPB corresponding to the local energy minima of separate minimal units of SPB exhibit sequence-dependent characteristics representative of canonic families. In contrast, conformations of dDMP and cdDMP with SPB torsions being far from the local minima of separate SPB units exhibit more complex sequence dependence.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

Towards the development of resonantly enhanced laser-based diagnostics for molten salt reactor safeguards

The adoption of Generation IV molten salt reactors (MSRs) depends on the ability to implement compatible monitoring instrumentation to ensure adherence to nuclear safeguards. This task is nontrivial due to the high temperature, reactive, and chemically complex fuel and coolant components contained within these systems. Optical spectroscopy techniques such as laser-induced fluorescence (LIF) and laser-induced breakdown spectroscopy (LIBS) are candidates for monitoring instrumentation. They offer many advantages for continuous monitoring, including the ability to operate at a standoff and compatibility with liquid-phase analytes. We discuss the use of LIF for the detection of Nd, a common fission fragment, within a liquid matrix. Results show that for NdCl3 dissolved in water, the Nd I 492.45 nm resonant transition is detectable without the need to induce a plasma and that the fluorescence emission can be separated in the time domain from the laser scatter signal. Additionally, we present a setup and preliminary results for measurements of solid Nd and U using resonant LIBS. The results demonstrate element-selective measurement capabilities and provide the foundational data necessary to continue the development of laser-based MSR diagnostics. This work also helps address gaps in the literature regarding energy level assignments of Nd.

98 - NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL↗
DOE OSTI2021

Advancements in modeling fuel pulverization and cladding behavior during a LOCA

During a loss-of-coolant accident (LOCA), it is possible for nuclear fuel rods to undergo a three-step process known as fuel fragmentation, relocation, and dispersal (FFRD). The chance of FFRD occurring increases as the fuel burnup increases. To support the nuclear industry's desire to increase the discharge burnup of nuclear fuels in light-water reactors (LWRs), it is imperative to understand the mechanisms driving the evolution of FFRD. In this work, a multiscale modeling approach is used to garner insight into underlying mechanisms leading to the fine fragmentation (also known as pulverization) of nuclear fuel during a LOCA. This report includes a summary of the atomistic and phase-field studies to develop a new pulverization criterion for use in the engineering-scale Bison fuel performance code. Details are also provided on cladding model improvements related to hydrogen/hydride embrittlement and damage and anisotropic thermal creep. The new models are used on the existing integral and separate effects LOCA validation cases available in Bison.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗