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At least 415 records · Page 23
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Predicting Dexter Energy Transfer Interactions from Molecular Orbital Overlaps

Dexter energy transfer (DET), also known as spin forbidden energy transfer (e.g., 3 D 1 A → 1 D 3 A), is undergoing renewed interest because of its utility in energy science, photocatalysis, and biomedical imaging. The DET reactions enable exciton fission and fusion and have been recently used to facilitate nanoscale imaging of protein assemblies on cell surfaces. While DET and Förster energy transfer rates are often well described using Fermi’s golden rule, the donor–acceptor couplings for DET may be bridge-state-mediated and depend on the electronic structure of and interactions among the donor, bridge, and acceptor. We provide a simple approach to approximate DET couplings using a product of molecular orbital overlap factors. This approach may be used to guide the design of DET systems with targeted energy-transfer kinetics.

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

Uncertainty quantification of optical models in fission fragment deexcitation

Here, we take the first step towards incorporating compound nuclear observables at astrophysically relevant energies into the experimental evidence used to constrain optical models, by propagating the uncertainty in two global optical potentials, one phenomenological and one microscopic, to correlated fission observables using the Monte Carlo Hauser-Feshbach formalism. We compare to a wide range of historic and recent experimental fission measurements, and discuss in detail regions of disagreement. We find that the parametric optical model uncertainty in neutron-fragment correlated observables involving neutron energy is significant. On the other hand, we observe that other experimental features, particularly neutron-fragment correlations near the 132 Sn shell closure and the high energy component of neutron spectra, are unlikely to be explained by the optical potential, and will require further experimental and theoretical effort to explain.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Influence of nonstatistical properties in nuclear structure on emission of prompt fission neutrons

We report the Hauser-Feshbach fission-fragment decay (HF 3 D) model is extended to calculate the prompt fission neutron spectrum (PFNS) for the thermal-neutron-induced fission on 235 U, where the evaporated neutrons from all possible fission-fragment pairs are aggregated. By studying model parameter sensitivities on the calculated PFNS as well as nonstatistical behavior of low-lying discrete level spin distribution, we conclude that discrepancies between the aggregation calculation and the experimental PFNS seen at higher neutron emission energies can be attributed to both the primary fission-fragment yield distribution and the possible high spin states that are not predicted by the statistical theory of nuclear structure.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Initial Development of Fusion Magnet Simulation Capabilities for Performance and Safety Evaluation Using the MOOSE Framework

Fusion energy holds the promise of being a transformative technology as a carbon-neutral, sustainable source of energy. Whole device modeling and the development of fusion digital twins will be increasingly important for emerging fusion device concepts at both national laboratories and within the commercial fusion industry. However, meeting the challenge of whole device modeling of fusion energy devices requires robust, multiphysics, multiscale modeling and simulation technologies capable of running on large-scale supercomputers. Detailed analysis of individual systems at-scale is also required to ensure safe and efficient operation as well as provide the safety basis for future device designs and licensing activities. In a tokamak, toroidal and poloidal magnets confine and shape the fusion plasma to promote the fusion reaction. High plasma temperatures and high magnetic field requirements in modern design concepts (leading to high amounts of energy stored within each magnet) impose electrical, thermal, and mechanical loads on the magnet components, which in turn impacts the safety considerations of the magnet and their supporting systems. Idaho National Laboratory (INL) has a history of working in this space, including development and benchmarking of the Magnetic System Circuitry Analysis Program (MSCAP) and Magnet Arcing (MAGARC) codes to study magnet quench events; notably, MAGARC was used to study quenching during the ITER Engineering Design Activity. However, these legacy codes and capabilities are not parallel and scalable, and new tools are required for future advances in this area, which leads to the INL-developed Multiphysics Object-Oriented Simulation Environment (MOOSE) framework. Developed originally for fission reactor systems under United States Department of Energy, Office of Nuclear Energy modeling and simulation programs, the MOOSE framework has been well-suited to multiscale, multiphysics modeling and simulation needs for nuclear systems. The framework is open-source, well-tested, under continuous development and deployment, and developed to a Nuclear Quality Assurance, Level 1 software quality standard. MOOSE has also been used in the fusion space previously in several projects: INL’s Tritium Migration Analysis Program, Version 8 (TMAP8) for tritium migration, UK Atomic Energy Authority’s A Unified Resource for OpenMC (fusion) Reactor Applications (AURORA) code for fusion thermo-mechanical and neutronics analysis, and Argonne National Laboratory’s Cardinal for high-fidelity computational fluid dynamics and neutronics. However, to model superconducting magnets, several MOOSE enhancements are required: additions to the current MOOSE electromagnetic capabilities, new material libraries for superconductors of interest (such as YBCO), as well as fusion-specific models for thermo-mechanics. This talk will discuss initial development activities to build these capabilities in MOOSE, focusing on initial validation and benchmarking activities. Proposed coupling workflows and future work to support the simulation of fusion magnets and magnet structural assemblies for performance and safety evaluation in MOOSE will also be discussed.

70 - PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Triplet Exciton Sensitization of Silicon Mediated by Defect States in Hafnium Oxynitride

Singlet exciton fission has the potential to increase the efficiency of crystalline silicon solar cells beyond the conventional single junction limit. Perhaps the largest obstacle to achieving this enhancement is uncertainty about energy coupling mechanisms at the interfaces between silicon and exciton fission materials such as tetracene. Here, the previously reported silicon‐hafnium oxynitride‐tetracene structure is studied and a combination of magnetic‐field‐dependent silicon photoluminescence measurements and density functional theory calculations is used to probe the influence of the interlayer composition on the triplet transfer process across the hafnium oxynitride interlayer. It is found that hafnium oxide interlayers do not show triplet exciton sensitization of silicon, and that nitrogen content in hafnium oxynitride layers is correlated with enhanced sensitization. Calculation results reveal that defects in hafnium oxynitride interlayers with higher nitrogen content introduce states close to the band‐edge of silicon, which can mediate the triplet exciton transfer process. Some defects introduce additional deleterious mid‐gap states, which may explain observed silicon photoluminescence quenching. These results show that band‐edge states can mediate the triplet exciton transfer process, potentially through a sequential charge transfer mechanism.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Multi-scale fission product release model with comparison to AGR data

TRistructural ISOtropic (TRISO) particle fuel is central to several advanced, high-temperature reactor designs. Each particle consists of a fuel kernel encapsulated by three layers of carbon and ceramics that prevent the release of fission products and ensure physical integrity. Despite outstanding retention properties, fission product release has been observed from intact particles. To better understand and quantify fission product release from TRISO particles, a multiscale, mechanistic model of fission product transport is being developed by the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program. Previous work focused on silver (Ag) transport and improved Ag release predictions. The work described in this report builds on this experience to better understand cesium (Cs) transport in silicon carbide (SiC), the main barrier to the release of fission products. Atomistic simulations provide bulk and grain boundary (GB) Cs diffusivities in SiC, which are used by phase field simulations in the mesoscale code Marmot to determine the temperature, microstructure, and irradiation-dependent Cs diffusivity at the mesoscale in SiC. This approach attributes the different temperature regimes experimentally observed for Cs diffusivities in SiC to a transition from bulk-dominated diffusivity at high temperatures to a GB-dominated regime at low temperatures, providing new insight. The multiscale, mechanistic effective diffusivity is then implemented in the fuel performance code BISON and further validated by comparing Cs release predictions from Advanced Gas Reactor (AGR)-1 and AGR-2 post-irradiation measurements. The new model improves BISON’s predictability. This document also reports improvements made on Ag transport modeling by accounting for different GB types having different diffusivities. Moreover, this report details preliminary efforts to model palladium (Pd) attack of the SiC at the mesoscale using a phase field approach. Pd attack and its impact on accelerated Ag transport remains a misunderstood phenomenon, and we use the model to demonstrate that the formation of lamellae that has been observed in experiments can be explained by the reaction of Pd with SiC to form alternating layers of graphite and Pd 2 Si. This effort aims to improve our understanding of the reaction and eventually provide a model for BISON to account for Pd penetration and its effects on fission product release.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Structure in the event-by-event energy-dependent neutron-$γ$ multiplicity correlations in 252 Cf(sf)

The emission of neutrons and γ rays by fission fragments reveal important information about the properties of fragments immediately following scission. The initial fragment properties, correlations between fragments, and emission competition give rise to correlations in neutron-γ emission. Recent theoretical and experimental advances have been proposed to explain the mechanism of angular momentum generation in fission, which would result in observable signature in neutron-γ emission correlations. In this paper, we present a novel analysis method of neutrons and γ rays emitted by fission fragments that allows us to discern structure in the observed correlations. We have analyzed data collected on 252 Cf (sf) at the Chi-Nu array at the Los Alamos Neutron Science Center. Through our analysis of the energy-differential neutron-γ multiplicity covariance, we have observed enhanced neutron-γ correlations, corresponding to rotational band γ-ray transitions, at γ-ray energies of 0.7 and 1.2 MeV. To shed light on the origin of this structure, we compare the experimental data with the predictions of three model calculations. The origin of the observed correlation structure is understood in terms of a positive spin-energy correlation in the generation of angular momentum in fission.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Generation of Fission Fragment Angular Momentum

In the last two years FREYA has been updated to study fission fragment angular momentum generation. We have also introduced integer and half integer spins, not specified in FREYA previously, and required to specify fragments more precisely. With these changes, FERYA still conserves energy as well as linear and angular momentum throughout the fission event. It is now possible to use FREYA to study a number of correlated quantities related to fragment spin, some of which can be directly measured. The spin-spin correlation was a major point of discussion at the Fission Fragment Angular Momentum workshop in Seattle in June 2022.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Status Report on Development of a Cask to Enable Pulsed Neutron Characterization of Irradiated Fuel

We present the design of a shielding cask that allows pulsed neutron characterization of irradiated fuel rodlets prior to their destructive examination in hot cells. The goal is to provide complementary and informative measurements that will inform subsequent hot cell PIE examinations by identifying typical and atypical regions with respect to microstructure, tomographic data, or isotope densities. Time-of-flight neutron diffraction has the potential to offer efficient, non-destructive and non-contact microstructural characterization of irradiated fuel pins with spatial resolution of 1 mm3 to 1 cm3 while for energy-resolved neutron imaging (and by extension tomography) a resolution of 100 μm was demonstrated. The potential results include crystallinity vs. amorphous volumes and microstructural information such as phase compositions and textures from the diffraction data as well as distances (e.g. pellet to cladding), cracks, and isotopic distributions of minor actinides, fission products as well as fission gas partial pressures e.g. in the plenum from energy resolved neutron imaging. The capability will identify regions of atypical behavior and provide cost effective bulk characterization of entire samples prior to destructive evaluation in hot cells. This effort is a collaboration between LANL, INL, ORNL, and UC Berkeley. A key facet of the initiative is the ability to cost effectively ship irradiated fuels from INL to the pulsed spallation neutron source at LANSCE. The irradiated fuel would be loaded in the custom designed cask (designated RaMHaM) at INL hot cells which then could be shipped in a BRR Type B shipment container between INL and LANL. No hot cell is required after the loading of the sample at INL in the pathway laid out in this report, greatly simplifying handling at LANL.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1980

Sources of high-energy protons in Saturn's magnetosphere

The passage of Pioneer 11 through Saturn's magnetosphere revealed an especially intense region of high-energy particle fluxes that places unique constraints on models for sources of high-energy protons in the innermost radiation zones. Of special interest is the flux of protons with energies above 35 MeV which was measured with a fission cell in the innermost magnetosphere between the A ring and the orbit of Mimas. The negative phase space density gradients derived from the proton and electron observations in this region imply that steady-state inward diffusion from the outer magnetosphere is not an adequate source for these high-energy protons. In the present paper, the nature of the Crand source at Saturn is examined, and its significance for injection of high-energy protons into the region inside L = 4 is estimated.

Cooper, J. F.↗
DOE OSTI2024

Isospin composition of fission barriers

We employ a microscopic method to study how isospin affects the fission potential of 240 Pu. Our approach uses constrained Hartree-Fock theory (CHF) which allows us to separately investigate the isoscalar and isovector properties of the nuclear energy density functional (EDF). By analyzing the isoscalar and isovector components of the EDF along the fission path we can assess the isovector contribution to fission barriers. Here, we study this effect for the fully adiabatic path to scission. The isovector component of the fission potential is found to increase in magnitude as the nucleus evolves towards scission, exemplifying the importance of stringent constraints on the isovector sector of the nuclear EDF for reliable predictions of fission properties.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Examination of decay heat measurements and their relevance for understanding the origin of the reactor antineutrino anomaly

Measurements of the decay energy released as a function of time following the thermal neutron induced fission of 235 U and 239,241 Pu were performed in the 1970s at Oak Ridge National Laboratory with the purpose of quantifying possible loss of coolant accident scenarios. The derivative of this decay energy with respect to time, known in technical parlance as decay heat, is mainly composed of two terms, that of the electrons produced together with antineutrinos in the $β$-minus decay of the neutron-rich fission products, and that of the $γ$ rays produced in the subsequent decay of excited nuclear levels. In this work we study if this extensive set of decay energy measurements can be used to assess the reactor antineutrino anomaly, that is, the approximately 5% deficit of electron antineutrinos produced by nuclear reactors, first deduced by Mention and collaborators in 2011, and observed by the major reactor antineutrino experiments since. Furthermore, with the assistance of nuclear databases, we are able to obtain the ratio of electron spectra under equilibrium conditions for 235 U to 239 Pu, in better agreement with the lower trend recently reported by Kopeikin and collaborators, as well as those for 235 U to 241 Pu and 241 Pu to 239 Pu, which do not agree well with those measured at the Institut Laue-Langevin in the 1980s. We conclude that a new experimental campaign is needed to measure the electron spectra utilizing a high resolution and signal-to-noise-ratio electron spectrometer and a highly precise fission normalization procedure.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Fission Fragment Intrinsic Spins and Their Correlations

The intrinsic spins and their correlations are the least understood characteristics of fission fragments from both theoretical and experimental points of view. In many nuclear reactions, the emerging fragments are typically excited and acquire an intrinsic excitation energy and an intrinsic spin depending on the type of the reactions and interaction mechanism. Both the intrinsic excitation energies and the fragments’ intrinsic spins and parities are controlled by the interaction mechanism and conservations laws, which lead to their correlations and determines the character of their deexcitation mechanism. We outline here a framework for the theoretical extraction of the intrinsic spin distributions of the fragments and their correlations within the fully microscopic real-time density-functional theory formalism and illustrate it on the example of induced fission of 236 U and 240 Pu, using two nuclear energy density functionals. Here, these fission fragment intrinsic spin distributions display new qualitative features previously not discussed in literature. Within this fully microscopic framework, we extract for the first time the intrinsic spin distributions of fission fragments of 236 U and 240 Pu as well as the correlations of their intrinsic spins, which have been debated in literature for more than six decades with no definite conclusions so far.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Neutron-Neutron Correlations in the Photofission of 238U

Background: In the fission of actinides, the nearly back-to-back motion of the fission fragments has a strong effect on the kinematics of fission neutrons. This leads to a favoring of opening angles near 0? and 180? in the neutron-neutron (n-n) opening angle distributions of correlated neutron pairs from the same fission event. Purpose: To measure the n-n opening angle and energy correlations in the photofission of 238U. As of this writing, measurements of correlated n-n opening angle distributions have been reported only for the spontaneous and neutron-induced fission of actinides. This work is the first to report such a measurement using photofission and will provide useful experimental input for photofission models used in codes such as MCNP and FREYA. Method: Fission is induced using bremsstrahlung photons produced via a low duty factor, pulsed, linear electron accelerator. The bremsstrahlung photon beam impinges upon a 238U target that is surrounded by a large neutron scintillation detection system capable of measuring particle position and time of flight, from which n-n opening angle and energy are measured. Neutron-neutron angular correlations are determined by taking the ratio between a correlated neutron distribution and an uncorrelated neutron distribution formed by the pairing of neutrons produced during different beam pulses. This analysis technique greatly diminishes effects due to detector efficiencies, acceptance, and experimental drifts. Results: The angular correlation of neutrons from the photofission of 238U shows a high dependence on neutron energy as well as a dependence on the angle of the emitted neutrons with respect to the incoming photon beam. Angular correlations were also measured using neutrons from the spontaneous fission of 252Cf, showing good agreement with past measurements. Conclusions: The measured angular correlations reflect the underlying back-to-back nature of the fission fragments. An anomalous decline in n-n yield was observed for opening angles near 180? for 238U.

Burggraf, Jeff↗
DOE OSTI2025

Perspective Chapter: Safe Disposal and Storage of Nuclear Waste

The use of nuclear energy inevitably generates nuclear waste as the byproduct of fission reactions. Depending on the initial composition of the fuel that goes into the reactor and the subsequent burn-up level, the chemistry of the resulting nuclear waste can vary substantially. This waste typically exhibits a broad spectrum of radioactivity and half-lives, making effective management one of the most critical challenges for global nuclear energy. This chapter provides a comprehensive overview of the origin and classification of nuclear waste and various strategies for its safe immobilization and disposal. The short- and long-term storage of waste with varying radioactivity is addressed. The significant technical and political complexities involving primarily long-term disposal are also discussed. To ensure the safe and permanent disposal of hazardous waste with extremely long half-lives, future efforts should focus on both technical innovation and public engagement.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Commissioning of a Cask Enabling Characterization of Irradiated Nuclear Fuels with Pulsed Neutrons

Irradiation tests are a key component of nuclear fuel development and identifying typical and atypical regions in the irradiated fuel volume relies on very few characterization techniques. The goal of the effort reported here is to provide complementary measurements adding to the available parameter space for post irradiation examination as well as to inform subsequent hot cell PIE examinations by identifying typical and atypical regions with respect to microstructure, tomographic data, or isotope densities. Pulsed neutrons, enabling diffraction as well as energy-resolved neutron imaging and neutron absorption resonance spectroscopy, offer unique capabilities for this purpose. Time-of-flight neutron diffraction has the potential to offer efficient, non-destructive and non-contact microstructural characterization of irradiated fuel pins with spatial resolution of 1 mm 3 to 1 cm 3 while for energy-resolved neutron imaging (and by extension tomography) a resolution of 100 μm was demonstrated. The potential results include crystallinity vs. amorphous volumes and microstructural information such as phase compositions, lattice strains (indicative of residual stresses or chemistry variations) and textures from the diffraction data as well as distances (e.g. pellet to cladding), cracks, and isotopic distributions of minor actinides, fission products as well as fission gas partial pressures e.g. in the plenum from energy resolved neutron imaging.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Characterizing the Performance of Fission Chambers for Local Neutron Flux and Spectrum Measurement

Three fission chambers were tested at The Ohio State University Research Reactor (OSURR) to evaluate fission chambers for neutron flux and spectrum measurements. Two of the fission chambers are commercial Photonis CFUR43 fission chambers—one utilizing highly enriched uranium-235 fissile deposits for thermal neutron detection and the other with highly depleted uranium-238 for fast neutron detection. This experiment was also performed in collaboration with French Alternative Energies and Atomic Energy Commission (CEA) with CEA suppling a uranium-235 loaded fission chamber built from the Photonis CFPR CE8/9 kit. The fission chambers were irradiated in a movable 6.5 inch dry tube at reactor powers of 50 kW, 200 kW, and 450 kW at ambient temperature and at 350°C. While all sensors demonstrated good linear sensitivity to reactor power, a leakage current of 6 nA was measured for the CFUR43 detectors. Additionally, the measured signal ratios of the two CFUR43 detectors did not match the theoretical values and are subject to further investigation on individual signal contributors.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Structure of even-even Sr isotopes with 50 ≤ N ≤ 58 neutrons

Excited levels in Sr 90 , Sr 92 , Sr 94 , and Sr 96 nuclei were reinvestigated using high-statistics multiple- γ coincidence data from neutron-induced fission of U 235 and spontaneous fission of Cf 252 , measured using Exogam at Institut Laue Langevin and Gammasphere arrays, respectively. The experimental goal was the search for new excited levels and firm spin-parity assignments to known levels. A total of 23 new levels with 30 new or corrected decays and 39 new or improved spin-parity assignments were obtained in the four nuclei. Negative-parity structures on top of 3 - excitation were firmly identified and extended to higher spins. New positive-parity structures in Sr 94 and Sr 96 were observed with 3 + excitations characteristic of γ collectivity. The 277.7-keV, E 2 decay from the 1507.0-keV level to the second 0 + level in Sr 96 , found in this paper, completes the coexisting deformed band in this nucleus. To learn about the microscopic structure of levels in the Sr 88 - 96 nuclei, we performed large-scale shell-model calculations. The calculations compared to the experiment, helped the discussion of the evolution of collectivity in strontium isotopes, highlighting the important role of various single-particle excitations in phase transitions and shape coexistence in the region. The special role of the neutron 9 / 2 + [ 404 ] extruder as a catalyst of the deformation change in the region is highlighted.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗