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At least 289 records · Page 16

Nucleation-mediated reshaping of facetted metallic nanocrystals: Breakdown of the classical free energy picture

Shape stability is key to avoiding degradation of performance for metallic nanocrystals synthesized with facetted non-equilibrium shapes to optimize properties for catalysis, plasmonics, and so on. Reshaping of facetted nanocrystals is controlled by the surface diffusion-mediated nucleation and growth of new outer layers of atoms. Here, Kinetic Monte Carlo (KMC) simulation of a realistic stochastic atomistic-level model is applied to precisely track the reshaping of Pd octahedra and nanocubes. Unexpectedly, separate constrained equilibrium Monte Carlo analysis of the free energy profile during reshaping reveals a fundamental failure of the classical nucleation theory (CNT) prediction for the reshaping barrier and rate. Why? Nucleation barriers can be relatively low for these processes, so the system is not locally equilibrated before crossing the barrier, as assumed in CNT. This claim is supported by an analysis of a first-passage problem for reshaping within a master equation framework for the model that reasonably captures the behavior in KMC simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Magnetic Field Vector Measurements Using Doppler-Free Saturation Spectroscopy

Experimentally measuring the magnetic-field vector topology in low-cost fusion-concept devices will provide critical information required to optimize and accelerate the development of those concepts for economical fusion energy. The magnetic-field measurement techniques most commonly used in modern tokamaks, i.e., beam-emission spectroscopy and optical emission spectroscopy, are not suitable below 5000 Gauss due to a lack of sensitivity. To diagnose magnetic field relevant to some of the ARPA-E-supported fusion concepts (50 to 1000 Gauss), a novel approach is required. Doppler-free saturation spectroscopy (DFSS) is a pump/probe laser-based technique and has been successfully demonstrated in the laboratory to provide a magnetic-field measurement accuracy of <10 Gauss. DFSS is implemented to obtain ultra-high-resolution spectra at a localized point in space. The spectral data is then fit to the Schrödinger equation for determination of the magnetic-field vector. To obtain the magnetic-field topology, the measurement spatial location is scanned over the desired region of space by steering the DFSS pump laser beam. The goal of this project is to assemble and commission a portable DFSS diagnostic capable of 2-D magnetic-field vector measurements utilizing the Hα spectral line profile.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Quantitative Evaluation of CO 2 Storage Potential in the Offshore Atlantic Lower Cretaceous Strata, Southeastern United States

The geological storage of CO 2 in the Earth’s subsurface has the potential to significantly offset greenhouse gas emissions for safe, economical, and acceptable public use. Due to legal advantages and vast resource capacity, offshore CO 2 storage provides an attractive alternative to onshore options. Although offshore Lower Cretaceous reservoirs have a vast expected storage capacity, there is a limited quantitative assessment of the offshore storage resource in the southeastern United States. This work is part of the Southeast Offshore Storage Resource Assessment (SOSRA) project, which presents a high-quality potential geological repository for CO 2 in the Mid- and South Atlantic Planning Areas. This is the first comprehensive investigation and quantitative assessment of CO 2 storage potential for the Lower Cretaceous section of the outer continental shelf that includes the Southeast Georgia Embayment and most of the Blake Plateau. An interpretation of 200,000 km of legacy industrial 2D seismic reflection profiles and geophysical well logs (i.e., TRANSCO 1005-1-1, COST GE-1, and EXXON 564-1) were utilized to create structure and thickness maps for the potential reservoirs and seals. We identified and assessed three target reservoirs isolated by seals based on their effective porosity values. The CO 2 storage capacity of these reservoirs was theoretically calculated using the DOE-NETL equation for saline formations. The prospective storage resources are estimated between 450 and 4700 Mt of CO 2 , with an offshore geological efficiency factor of dolomite between 2% and 3.6% at the formation scale.

03 NATURAL GAS↗

Sound velocities and thermal equation of state of fcc -iron-nickel alloys at high pressure and high temperature: Implications for the cores of Moon and several planets

Fcc-Fe-Ni alloy is believed to be the most dominant solid constitute of moderate-sized terrestrial planetary cores. Investigating the physical properties, especially the density and sound velocity of Fe-Ni alloys and comparing them with seismic observations is an indispensable approach to constructing compositional models for planetary interiors. In this study, we conducted sound velocity measurements on Fe-Ni alloys with 10 wt.% and 20 wt.% Ni up to ∼13.5 GPa and 1073 K, using the ultrasonic interferometry technique in a multi-anvil apparatus in conjunction with synchrotron radiation. By fitting the experimental data to finite strain equations, the bulk and shear moduli and their pressure and temperature derivatives are derived, yielding K S0 =145.8(14) GPa, G 0 = 73.2(7) GPa, K S0 ’ = 5.89(24), G 0 ’ = 2.89(8), (∂K S /∂T) P = -0.0181(12) GPa/K and (∂G/∂T) P = -0.0393(10) GPa/K for fcc-Fe 80 Ni 20 . An examination of the density-velocity relationship shows that compressional wave velocity is insensitive to temperature within the current pressure and temperature range, while shear wave velocity exhibits a large reduction with increasing temperature. Here, extrapolation of the sound velocities following the finite strain theories suggests that much slower Vs should be expected at pressure and temperature conditions corresponding to those of the lunar core. Possible core density and velocity profiles for other moderate planets and satellites, such as Mars, Mercury, and Ganymede are also calculated.

Equation of state↗

Computing molecular excited states on a D-Wave quantum annealer

Abstract The possibility of using quantum computers for electronic structure calculations has opened up a promising avenue for computational chemistry. Towards this direction, numerous algorithmic advances have been made in the last five years. The potential of quantum annealers, which are the prototypes of adiabatic quantum computers, is yet to be fully explored. In this work, we demonstrate the use of a D-Wave quantum annealer for the calculation of excited electronic states of molecular systems. These simulations play an important role in a number of areas, such as photovoltaics, semiconductor technology and nanoscience. The excited states are treated using two methods, time-dependent Hartree–Fock (TDHF) and time-dependent density-functional theory (TDDFT), both within a commonly used Tamm–Dancoff approximation (TDA). The resulting TDA eigenvalue equations are solved on a D-Wave quantum annealer using the Quantum Annealer Eigensolver (QAE), developed previously. The method is shown to reproduce a typical basis set convergence on the example $$\hbox {H}_2$$ H 2 molecule and is also applied to several other molecular species. Characteristic properties such as transition dipole moments and oscillator strengths are computed as well. Three potential energy profiles for excited states are computed for $$\hbox {NH}_3$$ NH 3 as a function of the molecular geometry. Similar to previous studies, the accuracy of the method is dependent on the accuracy of the intermediate meta-heuristic software called qbsolv.

74 ATOMIC AND MOLECULAR PHYSICS↗

Near-optimal combination of high performance and insensitivity in a shock compressed high explosive single crystal

Achieving the desired combination of superior detonation performance and insensitivity to shock initiation has been a long-standing goal in high explosive (HE) science and technology. Having previously established the shock insensitivity of 1,1-diamino-2,2-dinitroethene (also known as DADNE or FOX-7) single crystals to 20 GPa (extended to 25 GPa in this work), the FOX-7 detonation response was determined through wave profile measurements in ~250 μm thick single crystals shock compressed to 64 GPa. Quite unexpectedly, FOX-7 demonstrated the classic Chapman–Jouguet (C–J) detonation response—reaction completion in the detonation front (<0.7 ns) at pressures of 44 GPa and higher—not observed in other insensitive high explosives. Here, the experimentally determined C–J pressure (35 GPa), detonation wave velocities and the detonation products equation of state—together with shock insensitivity to 25 GPa—demonstrate that FOX-7 single crystals display a near-optimal combination of high performance and shock insensitivity, not observed in another HE crystal.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

SPRUCE Root Production Assessed with Manual Minirhizotrons Resolved to Plant Functional Type, 2015-2021

This dataset contains raw root length and diameter for individual roots and estimated root population production measurements from the Spruce and Peatland Responses Under Changing Environments (SPRUCE) experimental site within the Marcell Experimental Forest in northern Minnesota, USA. Measurements started at the beginning of whole ecosystem warming manipulations in 2015 through 2021 (2015-05-26 to 2021-09-01). Root morphology and estimated production were quantified throughout the peat profile with manual minirhizotrons deployed within SPRUCE plots. Images were processed using commercial software to quantify the length and diameter of individual roots. Roots were visually assigned to a plant functional type (PFT) of either (ericaceous) shrub, herb (sedges and Maianthemum trifolium), or tree (Larix laricina, Picea mariana) based on expert opinion. The biomass of individual roots was estimated using PFT-specific allometric equations (Iversen et al., 2018). Production per day was estimated as the length of new roots produced between imaging sessions, divided by the number of days between imaging sessions. These values were placed on a m2 aboveground area basis and scaled to a standard depth of 1m (roots are not evenly distributed with depth, do not interpret value as being on a m3 basis). Maximum and average (weighted by production length) depth of each PFT were also estimated within each minirhizotron tube. Annual production was interpolated as the average of four methods to scale these data (see Weber et al, 2026). Standing crop of roots was estimated for each tube as the maximum visible amount (both length and mass) of roots of that PFT for that year. These data expand the ability of researchers to accurately estimate the belowground dynamics of peatland vegetation, as well as the role that fine roots may play in impacting the fluxes of carbon within peatlands. This dataset contains three data files in comma-separate values (*.csv) format. This dataset contains one data file in comma-separate values (.csv) format. Additional metadata are provided: three data dictionaries and a file-level metadata file in comma-separate values (.csv) format and a user guide in PDF (*.pdf) format.

54 ENVIRONMENTAL SCIENCES↗

Soliton Generation in Negative Thermal Expansion Materials

Strain solitons have been observed statically in several 2D materials and dynamically in substrate materials using ultrafast laser pulses. The latter case relies on lattice relaxation in response to ultrafast heating in a light-absorbing transducer material, a process which is sensitive to the thermal expansion coefficient. Here we consider an unusual case where the sign of the thermal expansion coefficient is negative, a scenario which is experimentally feasible in light of rapid and recent advances in the discovery of negative thermal expansion materials. We present numerical solutions to a nonlinear differential equation which has been repeatedly demonstrated to quantitatively model experimental data and discuss the salient results using realistic parameters for material linear and nonlinear elasticity. The solitons that emerge from the initial value problem with negative and positive thermal expansion are qualitatively different in several ways. The new case of negative thermal expansion gives rise to a nearly-periodic soliton train with chirped profile and free of an isolated shock front. We suggest this unanticipated result may be realized experimentally and assess the potential for certain applications of this generic effect.

36 MATERIALS SCIENCE↗

Loss and Isotopic Fractionation of Alkali Elements during Diffusion-Limited Evaporation from Molten Silicate: Theory and Experiments

Moderately volatile elements (MVEs) are variably depleted in planetary bodies, reflecting the imprints of nebular and planetary processes. Among MVEs, Na, K, and Rb are excellent tracers for unraveling the history of MVE depletion in planetary bodies because they have similar geochemical behaviors but can be chemically fractionated by evaporation and condensation processes. Furthermore, K and Rb are amenable to high-precision isotopic analyses, which can help constrain the conditions of evaporation and condensation. To quantitatively understand why Na, K, and Rb are depleted in planetary bodies, we have carried out vacuum evaporation experiments from basaltic melt at 1200 and 1400 °C to study their evaporation kinetics and isotopic fractionations. We chose this composition because it is relevant to evaporation from small differentiated planetesimals. The Rb isotopic compositions of the evaporation residues were measured by multicollector inductively coupled plasma mass spectrometry (MC-ICPMS), and the K isotopic compositions were measured along profiles across the residues by secondary ion mass spectrometry (SIMS). In the 1400 °C run products, we found that the concentrations of both K and Rb in the run products decreased from core to rim, which was accompanied by a heavy K isotope enrichment near the surface. This indicates that, in this run, evaporation was limited by diffusion. To use those data quantitatively, we derive analytical equations that describe the evaporation rate and isotopic fractionation associated with diffusion-limited evaporation from a sphere, slab, and cylinder in transient and quasi-steady state regimes. This model is used to tease out the roles that diffusive transport in the melt and evaporation at the melt/gas interface play in setting the elemental depletion and isotopic composition of the residue. Under our experimental conditions, volatility decreases in the order of Na, Rb, and K. Using our experimental results in a thermodynamic model, we have estimated the product γΓ of activity coefficients × evaporation coefficients of Na, Rb, and K. The measured isotopic compositions of the residues are well explained using Rayleigh distillations, whereby the relative volatilities of K and Rb isotopes are given by the square root of their masses. We use our results and previously published data to predict how K and Rb could have been lost as a function of temperature, melt composition, oxygen fugacity, and saturation degree relevant to Vesta’s building blocks. We find that the K and Rb depletions, K/Rb elemental fractionation, and δ 41 K and δ 87 Rb isotopic fractionations of Vesta (as sampled by howardite-eucrite-diogenite (HED) meteorites) are best explained by evaporation of submillimeter size objects for 0.1-10 years at moderate temperatures (~1050 °C) in a medium ~98.8% saturated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Comparison of private flux region instability in conventional and super-X divertor configurations

Understanding turbulence in the divertor leg of tokamaks is essential to predicting the heat deposition profile on the divertor plate. This in turn is important for evaluating advanced divertor configurations, such as the super-X divertor. Within the divertor region, the private flux region is of interest because it is relatively unaffected by turbulence extending from the outboard midplane, so instabilities in this region could have a particularly pronounced effect on transport. These instabilities are modeled using the Arbitrary Topology Equation Reader (ArbiTER) eigenvalue code. Eigenmodes are examined further by comparing physics models to determine the fundamental mechanisms behind their formation, and quantifying the effect of individual terms. This analysis is conducted on both conventional and super-X divertors to compare these effects. Here, the resulting analysis reveals the presence of a geodesic curvature driven instability that is significantly more pronounced in the super-X configuration.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Sublimation temperature sensor for temperature locale

The sublimation temperature sensor (or “sublime sensor”) provides a continuum of measurement locations in which certain maximum temperatures are achieved during a heat up/cool down cycle. A predetermined material is encapsulated within a vacuum-sealed, non-volatile long tube (i.e., both ends capped and L$\gg$ D). This assembly is then inserted and centered into a heated zone, such as a furnace, exhaust pipe, or reactor. As the temperature increases, the material will sublimate (i.e., a process of having both the solid and gaseous states of matter simultaneously present) and will begin to fill the void - moving outward in both directions toward the ends of the tube. Once beyond the elevated temperatures, the gas will de-sublimate (i.e., deposition) onto the inner wall of the tube. The desired result of the sensor is the ring of material that develops over a relatively short period of time. This material deposit can be equated with temperature at an exact location. There is no need to interpolate and/or extrapolate for the desired measurement. Accuracy has been recorded for temperature locations on the range of ±2 mm over a 1 m span. Likewise, the precision of the measurement is ±0.2% the overall sensor domain. Furthermore, individual tubes with unique materials and pressures can be bundled together to provide a complete temperature profile of the heated zone.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Spatially resolved measurements of plasma ion velocity distributions in a dipole magnetic field

The equilibrium flows of a plasma discharge in a dipole magnetic field are a topic of interest in low temperature plasma physics. Experimentalists typically rely on probe-based and line-integrated diagnostic techniques in these environments to describe plasma behavior. Presented here are measurements of argon ion dynamics with laser induced fluorescence techniques to provide insight into plasma dynamics in dipole magnetic fields with nonperturbative, spatially localized measurements. Simulation results from a Lagrangian approach to track particle orbits are compared to measured density profiles and provide evidence to support the mechanism distinguishing experimental configurations is the initial approach of particles. Applying a negative DC bias to the magnet induces strong E×B flows around the magnet, even exceeding the ion acoustic speed as measured far from the magnet. A strong enough bias also produces two distinct ion populations and provides a method for controlling the density gradient on the equator.

McLaughlin, Jacob W. (ORCID:0000000152661888)↗

Analytic Sensitivity Coefficients for General Multigroup Infinite Medium k-Eigenvalue Problems

The general multigroup infinite medium k-eigenvalue neutron transport equation is used to derive analytic expressions for the infinite medium k-eigenvalue, the scalar neutron flux and adjoint, and the sensitivity of $k$ ∞ to perturbations in the multigroup nuclear data of a single species isotropic elastic scattering material. In the appendix, we present the multigroup nuclear data for U-235 and U-238 along with the corresponding k-eigenvalue, flux, adjoint, and sensitivity profiles, which include the sensitivity of $k$ ∞ to the total, fission, capture, and scattering macroscopic cross sections as well as to the group-to-group scattering cross section matrix, group neutron production, and the unconstrained and constrained fission neutron energy distribution.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Formation of Point Shocks for 3D Compressible Euler

We consider the 3D isentropic compressible Euler equations with the ideal gas law. We provide a constructive proof of the formation of the first point shock from smooth initial datum of finite energy, with no vacuum regions, with nontrivial vorticity present at the shock, and under no symmetry assumptions . We prove that for an open set of Sobolev‐class initial data that are a small L ∞ perturbation of a constant state, there exist smooth solutions to the Euler equations which form a generic stable shock in finite time. The blowup time and location can be explicitly computed, and solutions at the blowup time are smooth except for a single point , where they are of cusp‐type with Hölder C 1/3 regularity. Our proof is based on the use of modulated self‐similar variables that are used to enforce a number of constraints on the blowup profile, necessary to establish global existence and asymptotic stability in self‐similar variables. © 2022 Wiley Periodicals LLC.

Mathematics↗

BISON fuel performance modeling optimization for experiment X447 and X447A using axial swelling and cladding strain measurements

With the recent need to qualify new reactor designs such as the Versatile Test Reactor (VTR), fuel performance calculations need to be performed to determine safety criteria of the proposed designs. In order to validate the fuel performance results obtained by a fuel performance code, BISON, for new reactor designs, legacy fuel from EBR-II and FFTF MFF with Post -Irradiation Examination (PIE) data need to be used as validation cases to benchmark models. Here in this work, BISON has been paired with the Fuels Irradiation & Physics Database (FIPD) and IFR Materials Information System (IMIS) to supply PIE data for comparison with simulations of EBR-II experiments X447/X447A. X447/X447A were assessed by implementing models for Fuel Cladding Chemical Interaction (FCCI) within BISON and optimizing the friction coefficient between the fuel surface and the cladding, the anisotropic swelling factor, and the HT9 first thermal creep scalar (which scales the first term in the HT9 creep equation) to best match the PIE axial fuel swelling height and cladding profilometry for all pins in X447/X447A. The optimal values were found using a generic algorithm developed to select different values for the three parameters until end criteria was met and error couldn’t be reduced further. The BISON-simulated cladding profilometry was evaluated using Standard Error of the Estimate (SEE) to account for the profile shape of the cladding profilometry. Optimal values for the friction coefficient, anisotropic fuel swelling factor, and HT9 first thermal creep scalar were found to best fit the BISON simulation results to the PIE measurements found in IMIS and FIPD. Improvements to current models are suggested to account for the underprediction of fuel swelling at low burnups and the overprediction of fuel swelling at higher burnups observed for the axial fuel swelling height. Although two pins in EBR-II X447/X447A (DP70 and DP75) were known to fail due to FCCI, none of the pins simulated in BISON reached a cumulative damage fraction (CDF) above 0.008 with FCCI correlations coupled in the BISON simulations. The error estimate generated for all pins in X447/X447A using optimal values was 209 µm, which is deemed acceptable.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Analytic Sensitivity Coefficients for General Multigroup Infinite Medium k-Eigenvalue Problems

This work presents a general set of equations that can be used to rapidly generate new benchmarks to verify nuclear data sensitivity calculations. The general multigroup infinite medium k-eigenvalue neutron transport equation is used to derive analytic expressions for the infinite medium k-eigenvalue, the scalar neutron flux and adjoint flux, and the sensitivity of k∞ to perturbations in the multigroup nuclear data of a single species, isotropic and elastic scattering, material. The multigroup nuclear data for U-235 and U-238 is presented along with their corresponding k-eigenvalues, forward flux, adjoint flux, and sensitivity profiles, which include the sensitivity of k∞ to the total, fission, capture, and scattering macroscopic cross sections as well as to the group-to-group scattering cross section matrix, group-wise fission neutron production, and the unconstrained and constrained fission neutron energy distribution.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Radiation induced non-linear oscillations in ITER baseline scenario plasmas in DIII-D

Abstract This work shows how the radiation brought about by metals or metal-equivalent radiators such as Kr and Xe produces non-linear dynamics on otherwise stationary β N flattops of DIII-D ITER Baseline Scenario demonstration discharges. The Kr and Xe gases are used to reproduce the radiative loss rates of W in present machines that operate at core temperatures much lower than the expected ITER temperature. Experiments on DIII-D with injection of Kr and Xe, as well as with sources of intrinsic metals reach the range of radiated fraction values expected in the ITER core and experience slow oscillations in temperature and radiated power. In many cases of high radiated fraction, the core temperature decreases enough for the safety factor profile to rise above the 1/1 rational surface, naturally eliminating sawteeth and occasionally producing a persistent helical core. The oscillations can be reproduced by a modified Lotka–Volterra system for temperature and radiated fraction if diffusion and noise are included, which indicates that the interplay between temperature and radiation can be the main cause of the cyclic nature of the system. A new physics based model which includes equations for temperature, density and input power can also reproduce the oscillations observed in the experiments. The present results suggest that the non-linearity of the system can be increased by the inclusion of the inherently non-linear alpha heating term, which is proportional to ∼ n e 2 T i 2 , and obtains oscillations in the model when added to an otherwise more stationary system.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Characterization of Radiation Induced Defects Across Scales

The Whole Powder Pattern Modelling (WPPM) approach of diffraction line profile analysis (LPA) was applied for the first time on PuO 2 in order to understand the evolution of the microstructural properties as a function of process conditions. Crystallite size distributions and defect concentrations were determined by WPPM on three different PuO 2 samples - including one with a bimodal distribution and compared to the result of more common LPA analyses used in PuO 2 literature studies (e.g. Scherrer equation, double Voigt method). The conclusion was that a lognormal distribution of spherical crystallites with dislocations most closely represent the microstructure of PuO 2 produced by heating Pu 2 (C 2 O 4 ) 3 (H 2 O) 6 •3H 2 O between 650°C and 850°C. The volume-weighted mean column length (Lvol) parameter obtained from the double Voigt method for the monomodal samples were the same as the Lvol obtained from the WPPM within uncertainty. The two LPA methods did not agree on the Lvol parameters of the bimodal distribution sample with only the WPPM getting values that were consistent with the individual components. The WPPM can potentially provide more insight into future studies of the influences on the microstructure properties of PuO 2 .

36 MATERIALS SCIENCE↗