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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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DOE OSTI2019

Hyperfine Interaction and Shockley–Read–Hall Recombination in Semiconductors

Experimental and theoretical studies on optical orientation and spin-dependent recombination in a semiconductor in a magnetic field under the normal incidence of circularly polarized radiation onto the sample surface are reviewed. The experiments were carried out on GaAs{sub 1 –x}N{sub x} solid solutions, in which Ga{sup 2+} interstitial displacement defects play the role of deep paramagnetic centers responsible for spin-dependent recombination. It is established that, in the investigated materials, the hyperfine interaction of a localized electron with one nucleus of the paramagnetic center remains strong even at room temperature. The theory is compared with an experiment conducted in the steady-state excitation mode and under two-pulse pump-probe conditions. An analytical formula for spin beats in a magnetic field is derived.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Formation of Nanosized Surface Layers of 03Kh17N12M2 Stainless Steel by Implantation of N{sup +} Ions

Accumulation of nitrogen in nanosized surface layers of 03Kh17N12M2 stainless steel has been detected upon N{sup +} ion implantation up to 14 at % together with metal nitrides, mainly of chromium nitride CrN and interstitial solid solution. It has been demonstrated that N{sup +} ion implantation accompanied by preliminary irradiation by Ar{sup +} and O{sup +} ions decreases maximum nitrogen concentration by at least two times. It is assumed that this is stipulated by segregation to surface layers of iron atoms upon irradiation by Ar{sup +} ions as well as formation of chromium oxide Cr{sub 2}O{sub 3} and chromium hydroxide CrOOH upon irradiation by O{sup +} ions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Differing behaviors of point defects in Fe–36Ni alloy during annealing after low-temperature deformation and irradiation

Fe–36Ni alloy is studied in states in which it is quenched, irradiated with electrons at 70 K, and deformed at 77 K. It is shown that similar structure-phase transformations occur in the investigated alloy during annealing at the temperature range of 70–570 K both after preliminary low-temperature electron irradiation and after preliminary low-temperature deformation. Migration of interstitial atoms (70–140 K) and vacancies (180–570 K), which induce phase transformations and are the results of atomic separation and ordering of zones with increased nickel content, is observed. Mechanisms of structure-phase changes under deformation and annealing are discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

The Effect of Hydrogen on Fluctuation Embrittlement of Aluminum

In this paper, we describe the main processes occurring during the generation of vacancies in aluminum in the presence of hydrogen by ab initio methods using the SCAN functional. Hydrogen is shown to reduce the generation energy of vacancies from 2.8 to 0.8 eV. In this case, the eight hydrogen atoms located in the tetrahedral lattice voids around single aluminum atom greatly facilitate its movement to the interstitial site. The dependence of the activation energy of hydrogen embrittlement of aluminum on the hydrogen concentration in aluminum and temperature is calculated based on the kinetic strength concept. Hydrogen is shown to reduce the time of aluminum destruction only if its mole fraction in aluminum is greater than the critical level (~ 3 × 10{sup –4} at T = 293 K).

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Understanding irradiation growth through atomistic simulations: Defect diffusion and clustering in α-zirconium and the influence of alloying elements - 2016-0093

Irradiation-induced structural changes of α-zirconium alloys and in particular the effect of iron were investigated by molecular dynamics simulations using embedded atom potentials derived from first-principles calculations. The simulations revealed that at temperatures between 500 and 600 K self-interstitial atoms (SIAs) diffuse rapidly in a cooperative movement, preferably parallel to basal planes (a directions; ), forming nano-clusters with an extension in and . Vacancies diffuse more slowly than SIAs and remain isolated for a longer period of time. Nano-clusters associated with SIAs cause a pronounced overall expansion in a directions, as well as local strains. Under compressive strain in the c direction, vacancy diffusivity increases in the c direction. In contrast, the diffusivity of SIAs increases in the c direction under a tensile strain in the c direction. SIA nano-clusters are highly mobile within basal planes. Vacancy clusters grow by merging, leading to a contraction in the a direction, compensating for the expansion caused by SIA nano-clusters and possibly contributing to the plateau in growth after the initial rapid expansion. At the onset of breakaway growth, possibly due to stress buildup, the vacancy nano-clusters can condense into c loops, thereby diminishing the compensation effect. The alloying elements iron, nickel, chromium, and niobium liberated from secondary phase particles under irradiation or already in solution are attracted to vacancies and SIAs and are found inside vacancy and SIA loops. The interaction of alloying elements with defect clusters is discussed, with a particular focus on iron. Iron has been found to promote cluster formation in zirconium, and the structures of zirconium-iron clusters have been analyzed. Tin is repelled by SIA clusters and only weakly attracted by vacancies. Niobium impedes the diffusion of SIAs (and therefore may increase annihilation rates with nearby vacancies) and does not destabilize vacancy or SIA clusters. Ab initio calculations of the dimensional and elastic coefficients of the intermetallic phases occurring in secondary phase particles, such as Zr{sub 2}Fe and Zr{sub 3}Fe, are presented, allowing an assessment of local strains in a zirconium matrix. Thus, novel results from extended molecular dynamics simulations provide new insights and contribute to a deeper understanding of the complex mechanisms causing irradiation-induced dimensional changes and the breakaway growth of zirconium alloys. (authors)

36 MATERIALS SCIENCE↗
DOE OSTI2016

Equivalent radiation damage in zirconium irradiated in various reactors - 2016-0101

The physical properties and in-reactor performance of core components made from zirconium alloys are a function of the radiation-induced atomic displacements that occur during service. The vacancy and interstitial point defects and their clusters created by the atomic displacements modify the microstructure, and therefore physical properties such as strength and ductility, by forming dislocation loops. The rate of production of point defects also affects time-dependent properties such as creep and diffusion (mass transport). To simulate the effect of irradiation on core components, researchers have used materials test reactors for many years to irradiate and test materials. Such reactor tests can target an accumulated displacement damage dose to simulate the state of a material at a given stage in reactor life but at an accelerated rate. Each nuclear reactor has a specific neutron energy spectrum that also depends on the in-reactor location. Therefore, to use test reactor data to determine the effect of radiation damage on power reactor materials, one must convert the accumulated dose into a unit that is common in its effect on the material properties. For many property changes in nuclear reactor cores, this unit is displacements per atom. This paper compares the damage production for zirconium irradiated under differing neutron energy spectra in various power and test reactors. The damage rates as a function of different measures of neutron flux were used to relate atomic displacements in various materials test reactors to CANDU and light-water reactor conditions. (authors)

36 MATERIALS SCIENCE↗
DOE OSTI2023

Artificial intelligence models, photos, and data associated with the manuscript “Quantifying Streambed Grain Size, Uncertainty, and Hydrobiogeochemical Parameters Using Machine Learning Model YOLO” (v2)

This data package is associated with the manuscript “Quantifying Streambed Grain Size, Uncertainty, and Hydrobiogeochemical Parameters Using Machine Learning Model YOLO” published in Water Resources Research (Chen et al., 2024). This data package includes the training, validation, testing, and prediction data used by the artificial intelligence (AI) model for automated grain size and hydro-biogeochemistry quantification using streambed photos. The grain size data are extracted for each photo using You Look Only Once (YOLO), a pre-trained object detection model. This data package was originally published in October 2023. It was updated August 2025 (v2; new and modified files). File and folder names were not revised to indicate changes. See the change history section in the readme for more details. Please see flmd.csv for a list of all files contained in this data package and descriptions for each. Please see dd.csv for a data dictionary that defines the column headers of .csv files in the data package. This dataset is comprised of one data folder containing (1) file-level metadata; (2) data dictionary; (3) readme; and (4) six subfolders. Subfolders 1 to 4 include the training, validation, testing, and prediction data. Subfolder 5_Summary includes the summary results of different combinations of training, validation, testing, and prediction data. Subfolder 6_SupplementalData includes additional data downloaded from public sources (Kaufman et al., 2023a; Kaufman et al., 2023b; Garefalakis et al., 2023; Mair et al., 2024; https://github.com/river-corridors-sfa/Geospatial_variables). In total, the data package includes 110 folders and 44,283 files. These files include 9,047 .jpg photos, 1 .png photo, 3 .tif photos; 26,639 photo labels and individual grain sizes and probability from AI (.txt); 8,447 grain size distribution data (.dat); and 126 CSV files for results summary, and 14 required metadata files (.xlsx). The summary CSV files contain 68 columns and approximately 2,200 rows that represent photo names, site locations, recording time, GPS coordinates, grains sizes (D10, D50, D60, and D84), number of grains, and additional hydro-biogeochemical data such as water depth, flow velocity, Manning’s coefficient, friction factor, hydraulic conductivity, permeability, streambed interstitial velocity magnitude, mass transfer rate, and nitrate uptake velocity. The photos were obtained from 75 sites in the Yakima River Basin and the Columbia River shorelines, and other associated data from samples and sensors obtained when the photos were taken are publicly available (Fulton et al. 2022; Grieger et al. 2023). All files are .csv, .txt, .dat, .jpg, or .pdf. We acknowledge the Yakama Nation as owners and caretakers of the lands where we collected some of these data. We thank the Confederated Tribes and Bands of the Yakama Nation Tribal Council and Yakama Nation Fisheries for working with us to facilitate sample collection and optimization of data usage according to their values and worldview.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2011

Effects of the crystallographic orientation of Sn on the electromigration of Cu/Sn-Ag-Cu/Cu ball joints

Electromigration behavior and fast circuit failure with respect to crystallographic orientation of Sn grains were examined. The test vehicle was Cu/Sn-3.0 wt% Ag-0.5 wt% Cu/Cu ball joints, and the applied current density was 15 kA/cm 2 at 160 °C. The experimental results indicate that most of the solder bumps show different microstructural changes with respect to the crystallographic orientation of Sn grains. Fast failure of the bump occurred due to the dissolution of the Cu circuit on the cathode side caused by the fast interstitial diffusion of Cu atoms along the c-axis of the Sn grains when the c-axis was parallel to the electron flow. Slight microstructural changes were observed when the c-axis was perpendicular to the electron flow. In addition, Cu 6 Sn 5 intermetallic compound (IMC) was formed along the direction of the c-axis of the Sn grains instead of the direction of electron flow in all solder ball joints.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Diffusional exchange of isotopes in a metal hydride sphere.

This report describes the Spherical Particle Exchange Model (SPEM), which simulates exchange of one hydrogen isotope by another hydrogen isotope in a spherical metal hydride particle. This is one of the fundamental physical processes during isotope exchange in a bed of spherical metal particles and is thus one of the key components in any comprehensive physics-based model of exchange. There are two important physical processes in the model. One is the entropy of mixing between the two isotopes; the entropy of mixing is increased by having both isotopes randomly placed at interstitial sites on the lattice and thus impedes the exchange process. The other physical process is the elastic interaction between isotope atoms on the lattice. The elastic interaction is the cause for {beta}-phase formation and is independent of the isotope species. In this report the coupled diffusion equations for two isotopes in the {beta}-phase hydride are solved. A key concept is that the diffusion of one isotope depends not only on its concentration gradient, but also on the concentration gradient of the other isotope. Diffusion rate constants and the chemical potentials for deuterium and hydrogen in the {beta}-phase hydride are reviewed because these quantities are essential for an accurate model of the diffusion process. Finally, a summary of some of the predictions from the SPEM model are provided.

08 HYDROGEN↗
DOE OSTI2011

Anomalous X-ray Diffraction Studies for Photovoltaic Applications

Anomalous X-ray Diffraction (AXRD) has become a useful technique in characterizing bulk and nanomaterials as it provides specific information about the crystal structure of materials. In this project we present the results of AXRD applied to materials for photovoltaic applications: ZnO loaded with Ga and ZnCo{sub 2}O{sub 4} spinel. The X-ray diffraction data collected for various energies were plotted in Origin software. The peaks were fitted using different functions including Pseudo Voigt, Gaussian, and Lorentzian. This fitting provided the integrated intensity data (peaks area values), which when plotted as a function of X-ray energies determined the material structure. For the first analyzed sample, Ga was not incorporated into the ZnO crystal structure. For the ZnCo{sub 2}O{sub 4} spinel Co was found in one or both tetrahedral and octahedral sites. The use of anomalous X-ray diffraction (AXRD) provides element and site specific information for the crystal structure of a material. This technique lets us correlate the structure to the electronic properties of the materials as it allows us to probe precise locations of cations in the spinel structure. What makes it possible is that in AXRD the diffraction pattern is measured at a number of energies near an X-ray absorption edge of an element of interest. The atomic scattering strength of an element varies near its absorption edge and hence the total intensity of the diffraction peak changes by changing the X-ray energy. Thus AXRD provides element specific structural information. This method can be applied to both crystalline and liquid materials. One of the advantages of AXRD in crystallography experiments is its sensitivity to neighboring elements in the periodic tables. This method is also sensitive to specific crystallographic phases and to a specific site in a phase. The main use of AXRD in this study is for transparent conductors (TCs) analysis. TCs are considered to be important materials because of their efficiency and low risk of environmental pollution. These materials are important to solar cells as a result of their remarkable combination of optical and electrical properties, including high electrical conductivity and high optical transparency in the spectrum of visible light. TCs provide a transparent window, which allows sunlight to pass through while also allowing electricity to conduct out of the cell. Spinel materials have the chemical form AB{sub 2}O{sub 4}, and are made of a face-centered cubic (FCC) lattice of oxygen anions and cations in specific interstitial sites. A normal spinel has all A cations on tetrahedral sites and B cations on octahedral sites. In contrast; an inverse spinel has the A and half of the B cations on octahedral sites and the other half of the B cations on tetrahedral sites; a mixed spinel lies between. In the spinel structure, 8 of 64 possible tetrahedral sites and 16 of 32 possible octahedral sites are filled. Normal spinels have particularly high conduction as the linear octahedral chains of B cations likely serve as conduction paths. In this paper we present how the data obtained with AXRD is used to analyze TCs properties as they apply to photovoltaic applications. One of the materials used for this analysis is zinc oxide. It has been loaded with 5% and 10% of Ga, which has an absorption edge of 10367 eV. The peak (100) was measured for the zinc oxide loaded with 10% Ga. In the case of 5% Ga, we measured peaks (100) and (101). With the information provided by the AXRD we can identify if Ga is being incorporated in the ZnO crystal structure. The analysis of 311 plane in the ZnCo{sub 2}O{sub 4} spinel shows if Co is in tetrahedral or octahedral site.

14 SOLAR ENERGY↗
DOE OSTI2011

Mitigation of Hydrogen Gas Generation from the Reaction of Uranium Metal with Water in K Basin Sludge and Sludge Waste Forms

Prior laboratory testing identified sodium nitrate and nitrite to be the most promising agents to minimize hydrogen generation from uranium metal aqueous corrosion in Hanford Site K Basin sludge. Of the two, nitrate was determined to be better because of higher chemical capacity, lower toxicity, more reliable efficacy, and fewer side reactions than nitrite. The present lab tests were run to determine if nitrate’s beneficial effects to lower H2 generation in simulated and genuine sludge continued for simulated sludge mixed with agents to immobilize water to help meet the Waste Isolation Pilot Plant (WIPP) waste acceptance drainable liquid criterion. Tests were run at ~60°C, 80°C, and 95°C using near spherical high-purity uranium metal beads and simulated sludge to emulate uranium-rich KW containerized sludge currently residing in engineered containers KW-210 and KW-220. Immobilization agents tested were Portland cement (PC), a commercial blend of PC with sepiolite clay (Aquaset II H), granulated sepiolite clay (Aquaset II G), and sepiolite clay powder (Aquaset II). In all cases except tests with Aquaset II G, the simulated sludge was mixed intimately with the immobilization agent before testing commenced. For the granulated Aquaset II G clay was added to the top of the settled sludge/solution mixture according to manufacturer application directions. The gas volumes and compositions, uranium metal corrosion mass losses, and nitrite, ammonia, and hydroxide concentrations in the interstitial solutions were measured. Uranium metal corrosion rates were compared with rates forecast from the known uranium metal anoxic water corrosion rate law. The ratios of the forecast to the observed rates were calculated to find the corrosion rate attenuation factors. Hydrogen quantities also were measured and compared with quantities expected based on non-attenuated H2 generation at the full forecast anoxic corrosion rate to arrive at H2 attenuation factors. The uranium metal corrosion rates in water alone and in simulated sludge were near or slightly below the metal-in-water rate while nitrate-free sludge/Aquaset II decreased rates by about a factor of 3. Addition of 1 M nitrate to simulated sludge decreased the corrosion rate by a factor of ~5 while 1 M nitrate in sludge/Aquaset II mixtures decreased the corrosion rate by ~2.5 compared with the nitrate-free analogues. Mixtures of simulated sludge with Aquaset II treated with 1 M nitrate had uranium corrosion rates about a factor of 8 to 10 lower than the water-only rate law. Nitrate was found to provide substantial hydrogen mitigation for immobilized simulant sludge waste forms containing Aquaset II or Aquaset II G clay. Hydrogen attenuation factors of 1000 or greater were determined at 60°C for sludge-clay mixtures at 1 M nitrate. Hydrogen mitigation for tests with PC and Aquaset II H (which contains PC) were inconclusive because of suspected failure to overcome induction times and fully enter into anoxic corrosion. Lessening of hydrogen attenuation at ~80°C and ~95°C for simulated sludge and Aquaset II was observed with attenuation factors around 100 to 200 at 1 M nitrate. Valuable additional information has been obtained on the ability of nitrate to attenuate hydrogen gas generation from solution, simulant K Basin sludge, and simulant sludge with immobilization agents. Details on characteristics of the associated reactions were also obtained. The present testing confirms prior work which indicates that nitrate is an effective agent to attenuate hydrogen from uranium metal corrosion in water and simulated K Basin sludge to show that it is also effective in potential candidate solidified K Basin waste forms for WIPP disposal. The hydrogen mitigation afforded by nitrate appears to be sufficient to meet the hydrogen generation limits for shipping various sludge waste streams based on uranium metal concentrations and assumed waste form loadings.

08 HYDROGEN↗
DOE OSTI2011

The Ames Laboratory Annual Site Environmental Report: Calendar Year 2010

This report summarizes the environmental status of Ames Laboratory for calendar year 2010. It includes descriptions of the Laboratory site, its mission, the status of its compliance with applicable environmental regulations, its planning and activities to maintain compliance, and a comprehensive review of its environmental protection, surveillance and monitoring activities. In 2010, the Laboratory accumulated and disposed of waste under U.S. Environmental Protection Agency (EPA) issued generator numbers. All waste is handled according to all applicable EPA, State, Local regulations and DOE Orders. In 2006 the Laboratory reduced its generator status from a Large Quantity Generator (LQG) to a Small Quantity Generator (SQG). EPA Region VII was notified of this change. The Laboratory's RCRA hazardous waste management program was inspected by EPA Region VII in April 2006. There were no notices of violations. The inspector was impressed with the improvements of the Laboratory's waste management program over the past ten years. The Laboratory was in compliance with all applicable federal, state, local and DOE regulations and orders in 2010. There were no radiological air emissions or exposures to the general public due to Laboratory activities in 2010. See U.S. Department of Energy Air Emissions Annual Report in Appendix B. As indicated in prior SERs, pollution awareness, waste minimization and recycling programs have been in practice since 1990, with improvements implemented most recently in 2010. Included in these efforts were battery and CRT recycling, miscellaneous electronic office equipment, waste white paper and green computer paper-recycling and corrugated cardboard recycling. Ames Laboratory also recycles/reuses salvageable metal, used oil, foamed polystyrene peanuts, batteries, fluorescent lamps and telephone books. Ames Laboratory reported to DOE-Ames Site Office (AMSO), through the Laboratory's Performance Evaluation Measurement Plan, on its Affirmative Procurement Performance Measure. A performance level of 'A-' was achieved in 2010 for Integrated Safety, Health and Environmental Protection. As reported in Site Environmental Reports for prior years, the Laboratory's Environmental Management System (EMS) has been integrated into the Laboratory's Integrated Safety Management System since 2005. The integration of EMS into the way the Laboratory does business allows the Laboratory to systematically review, address and respond to the Laboratory's environmental impacts. The Laboratory's EMS was audited in April 2009 by DOE-CH. There were four 'Sufficiently in Conformity' findings as a result of the audit. All four findings were tracked in the Laboratory's corrective action database for completion. Beryllium was used routinely at Ames Laboratory in the 1940's and 1950's in processes developed for the production of highly pure uranium and thorium in support of the historic Manhattan Project. Laboratory metallurgists also worked on a process to produce pure beryllium metal from beryllium fluoride. In the early 1950's, beryllium oxide powder was used to produce shaped beryllium and crucibles. As a result of that work, beryllium contamination now exists in many interstitial spaces (e.g., utility chases) and ventilation systems in Wilhelm, Spedding and Metals Development buildings. Extensive characterization and remediation efforts have occurred in 2009 and 2010 in order to better understand the extent of the contamination. Analysis of extensive sampling data suggests that a fairly wide dispersion of beryllium occurred (most likely in the 1950's and 60's) in Wilhelm Hall and in certain areas of Spedding Hall and Metals Development. Area air-sampling results and work-area surface characterizations indicate the exposure potential to current workers, building visitors and the public remains extremely low. This information is now used to guide cleaning efforts and to provide worker protection during remodeling and maintenance activities. Results were shared with the DOE's Former Worker Program to support former worker medical testing and compensation programs. A complete discussion of the Laboratory's beryllium characterization and remediation efforts can be found at: http://www.ameslab.gov/operations/esha/beryllium-information.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2012

Theoretical Studies of Hydrogen Storage Alloys

Theoretical calculations were carried out to search for lightweight alloys that can be used to reversibly store hydrogen in mobile applications, such as automobiles. Our primary focus was on magnesium based alloys. While MgH 2 is in many respects a promising hydrogen storage material, there are two serious problems which need to be solved in order to make it useful: (i) the binding energy of the hydrogen atoms in the hydride is too large, causing the release temperature to be too high, and (ii) the diffusion of hydrogen through the hydride is so slow that loading of hydrogen into the metal takes much too long. In the first year of the project, we found that the addition of ca. 15% of aluminum decreases the binding energy to the hydrogen to the target value of 0.25 eV which corresponds to release of 1 bar hydrogen gas at 100 degrees C. Also, the addition of ca. 15% of transition metal atoms, such as Ti or V, reduces the formation energy of interstitial H-atoms making the diffusion of H-atoms through the hydride more than ten orders of magnitude faster at room temperature. In the second year of the project, several calculations of alloys of magnesium with various other transition metals were carried out and systematic trends in stability, hydrogen binding energy and diffusivity established. Some calculations of ternary alloys and their hydrides were also carried out, for example of Mg 6 AlTiH 16 . It was found that the binding energy reduction due to the addition of aluminum and increased diffusivity due to the addition of a transition metal are both effective at the same time. This material would in principle work well for hydrogen storage but it is, unfortunately, unstable with respect to phase separation. A search was made for a ternary alloy of this type where both the alloy and the corresponding hydride are stable. Promising results were obtained by including Zn in the alloy.

08 HYDROGEN↗
DOE OSTI2012

Heritable Genetic Changes in Cells Recovered From Irradiated 3D Tissue Constructs

Combining contemporary cytogenetic methods with DNA CGH microarray technology and chromosome flow-sorting increases substantially the ability to resolve exchange breakpoints associated with interstitial deletions and translocations, allowing the consequences of radiation damage to be directly measured at low doses, while also providing valuable insights into molecular mechanisms of misrepair processes that, in turn, identify appropriate biophysical models of risk at low doses. Specific aims apply to cells recovered from 3D tissue constructs of human skin and, for the purpose of comparison, the same cells irradiated in traditional 2D cultures. The project includes research complementary to NASA/HRP space radiation project.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2012

Improving the sampling efficiency of the Grand Canonical Simulated Quenching approach

Most common atomistic simulation techniques, like molecular dynamics or Metropolis Monte Carlo, operate under a constant interatomic Hamiltonian with a fixed number of atoms. Internal (atom positions or velocities) or external (simulation cell size or geometry) variables are then evolved dynamically or stochastically to yield sampling in different ensembles, such as microcanonical (NVE), canonical (NVT), isothermal-isobaric (NPT), etc. Averages are then taken to compute relevant physical properties. At least two limitations of these standard approaches can seriously hamper their application to many important systems: (1) they do not allow for the exchange of particles with a reservoir, and (2) the sampling efficiency is insufficient to allow the obtention of converged results because of the very long intrinsic timescales associated with these quantities. To fix ideas, one might want to identify low (free) energy configurations of grain boundaries (GB). In reality, grain boundaries are in contact the grains which act as reservoirs of defects (e.g., vacancies and interstitials). Since the GB can exchange particles with its environment, the most stable configuration cannot provably be found by sampling from NVE or NVT ensembles alone: one needs to allow the number of atoms in the sample to fluctuate. The first limitation can be circumvented by working in the grand canonical ensemble (TV ) or its derivatives (such as the semi-grand-canonical ensemble useful for the study of substitutional alloys). Monte Carlo methods have been the first to adapt to this kind of system where the number of atoms is allowed to fluctuate. Many of these methods are based on the Widom insertion method [Widom63] where the chemical potential of a given chemical species can be inferred from the potential energy changes upon random insertion of a new particle within the simulation cell. Other techniques, such as the Gibbs ensemble Monte Carlo [Panagiotopoulos87] where exchanges of particles are attempted to equilibrate the chemical potential between two cells and hence allow for the calculation of coexistence curves, exploit the same idea: particle insertion (or exchange) is attempted and accepted with a Metropolis-like rule that depends exponentially on the energy change upon insertion. A well known limitation of this kind of approach is that the probability of accepting such a move decreases extremely rapidly with increasing density, due to the extremely large short-range repulsion between atoms. In response to these difficulties it became apparent that a solution to the problem might be to avoid abrupt insertions but instead to proceed gradually, so as to allow the system to react and make way for the incoming particle. In this view of things, the 'occupation' of a certain atomic site can be viewed as a continuous variable, ranging between 0 and 1, representing 'how much' of the particle is present at any given time. These ideas proved ideal in Molecular Dynamics (MD) settings because equations of motions for these occupation variables can sometimes be obtained. For example, in the case of Grand Canonical Molecular Dynamics [Cagin91], one special particle is allowed to have a fractional occupation. This can lead to either its destruction (occupation = 0) or its complex creation (occupation = 1) so as to enforce a given chemical potential. These approaches proved useful, but mostly in the liquid state where the probability of successfully inserting a new particle is sufficiently high. At higher densities, convergence proved to be hampered by very inefficient sampling. In this work, we explore the use of a related MD-based grand canonical technique, the Grand Canonical Simulated Quenching (GCSQ) of Phillpot and Rickman [Phillpot92,Phillpot94], and explore its application to the grand canonical sampling of solid state systems. We show that, in conjunction with advanced sampling techniques, GCSQ can be a useful tool to sample conformations of complex systems, such as GBs, and assist in the identification of their most stable states and/or most likely defective states.

36 MATERIALS SCIENCE↗
DOE OSTI2012

Measure Guideline: Internal Insulation of Masonry Walls

This measure guideline provides recommendations for interior insulation assemblies that control interstitial condensation and durability risks; recommendations for acceptable thermal performance are also provided. An illustrated guide of high-risk exterior details (which concentrate bulk water), and recommended remediation details is provided. This is followed by a recommended methodology forrisk assessment of a masonry interior insulation project: a series of steps are suggested to assess the risks associated with this retrofit, with greater certainty with added steps.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2015

Review of Calculations on Point Defect Properties in Delta-Pu

The results of theoretical predictions of properties for vacancies and self-interstitial atoms (SIA) in δ-Pu are presented and reviewed. Three methods have been used for these predictions, namely the modified embedded atom method (MEAM), density functional theory (DFT) with and without spin polarization, and continuum mechanics (CM) models adapted to plutonium. The properties considered are formation and migration energies, and relaxation volumes of vacancies and SIA. Predicted values vary considerably. Nevertheless, all three methods predict that the activation energy for self-diffusion by vacancies is of similar magnitude as the SIA formation energy. Furthermore, the absolute magnitudes of relaxation volumes for vacancies and SIA are also similar, indicating that there exist no large bias for radiation-induced void swelling.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

Report on simulation of fission gas and fission product diffusion in UO 2

In UO 2 nuclear fuel, the retention and release of fission gas atoms such as xenon (Xe) are important for nuclear fuel performance by, for example, reducing the fuel thermal conductivity, causing fuel swelling that leads to mechanical interaction with the clad, increasing the plenum pressure and reducing the fuel–clad gap thermal conductivity. We use multi-­scale simulations to determine fission gas diffusion mechanisms as well as the corresponding rates in UO 2 under both intrinsic and irradiation conditions. In addition to Xe and Kr, the fission products Zr, Ru, Ce, Y, La, Sr and Ba have been investigated. Density functional theory (DFT) calculations are used to study formation, binding and migration energies of small clusters of Xe atoms and vacancies. Empirical potential calculations enable us to determine the corresponding entropies and attempt frequencies for migration as well as investigate the properties of large clusters or small fission gas bubbles. A continuum reaction-­diffusion model is developed for Xe and point defects based on the mechanisms and rates obtained from atomistic simulations. Effective fission gas diffusivities are then obtained by solving this set of equations for different chemical and irradiation conditions using the MARMOT phase field code. The predictions are compared to available experimental data. The importance of the large Xe U3O cluster (a Xe atom in a uranium + oxygen vacancy trap site with two bound uranium vacancies) is emphasized, which is a consequence of its high mobility and high binding energy. We find that the Xe U3O cluster gives Xe diffusion coefficients that are higher for intrinsic conditions than under irradiation over a wide range of temperatures. Under irradiation the fast-­moving Xe U3O cluster recombines quickly with irradiation-induced interstitial U ions, while this mechanism is less important for intrinsic conditions. The net result is higher concentration of the Xe U3O cluster for intrinsic conditions than under irradiation. We speculate that differences in the irradiation conditions and their impact on the Xe U3O cluster can explain the wide range of diffusivities reported in experimental studies. However, all vacancy-­mediated mechanisms underestimate the Xe diffusivity compared to the empirical radiation-­enhanced rate used in most fission gas release models. We investigate the possibility that diffusion of small fission gas bubbles or extended Xe-­vacancy clusters may give rise to the observed radiation-­enhanced diffusion coefficient. These studies highlight the importance of U divacancies and an octahedron coordination of uranium vacancies encompassing a Xe fission gas atom. The latter cluster can migrate via a multistep mechanism with a rather low effective barrier, which together with irradiation-induced clusters of uranium vacancies, gives rise to the irradiation-enhanced diffusion coefficient observed in experiments.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗