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At least 451 records · Page 25
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

LLNL Macroscopic Anisotropic Explosives Research at INL National Security Test Range - Test Results

A select team of 23 engineers, scientists, and explosives specialists from LLNL, LANL, INL, and Marine Raiders from Marine Special Operations Command (MARSOC) and U.S. Special Operations Command (SOCOM) assembled during the second week of November at the INL National Security Test Range near Idaho Falls to investigate and demonstrate fundamental principles of explosives anisotropy. Today's explosives are isotropic in their detonation performance. That is, no matter what direction a detonation runs through bulk explosive, the performance is the same; whereas, anisotropic explosives exhibit different performance, depending on which direction the detonation wave moves through the explosive. The ANISO Team worked in subfreezing temperatures on the Snake River Plain, carrying out 55 experimental explosives shots in four days that lead to a clear understanding of the performance and behavior of an assembly of small, linerless, C4 shaped charges. These shots clearly demonstrated, for the first time, on a macroscopic scale, the principle of anisotropy in measured progression of the detonation through the explosive assembly. The outputs of nine piezo timing pins in the explosive assembly clearly showed detonation progressing through the assembly faster than nominal detonation velocity and moving slower than nominal detonation velocity in the opposite direction. Basic data from these experiments will be used to design and construct explosives assemblies that will be shot in the LLNL High Explosives Applications Facility's (HEAF). These experimental tests will provide refined basic data that will then be used by modelers to develop high explosives models. Computer simulations using these models will then be run to predict performance and design inhomogeneous, anisotropic bulk explosive charges that will be tested at LLNL.

33 ADVANCED PROPULSION SYSTEMS↗
DOE OSTI2022

Variational approach to quantum state tomography based on maximal entropy formalism

Quantum state tomography is an integral part of quantum computation and offers the starting point for the validation of various quantum devices. One of the central tasks in the field of state tomography is to reconstruct, with high fidelity, the quantum states of a quantum system. From an experiment on a real quantum device, one can obtain the mean measurement values of different operators. With such data as input, in this report we employ the maximal entropy formalism to construct the least biased mixed quantum state that is consistent with the given set of expectation values. Even though, in principle, the reported formalism is quite general and should work for an arbitrary set of observables, in practice we shall demonstrate the efficacy of the algorithm on an informationally complete (IC) set of Hermitian operators. Such a set possesses the advantage of uniquely specifying a single quantum state from which the experimental measurements have been sampled and hence renders the rare opportunity not only to construct a least-biased quantum state but even replicate the exact state prepared experimentally within a preset tolerance. Here, the primary workhorse of the algorithm is reconstructing an energy function which we designate as the effective Hamiltonian of the system, and parameterizing it with Lagrange multipliers, according to the formalism of maximal entropy. These parameters are thereafter optimized variationally so that the reconstructed quantum state of the system converges to the true quantum state within an error threshold. To this end, we employ a parameterized quantum circuit and a hybrid quantum-classical variational algorithm to obtain such a target state, making our recipe easily implementable on a near-term quantum device.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Fast and Universal Kohn-Sham Density Functional Theory Algorithm for Warm Dense Matter to Hot Dense Plasma

Understanding many processes, e.g., fusion experiments, planetary interiors, and dwarf stars, depends strongly on microscopic physics modeling of warm dense matter and hot dense plasma. This complex state of matter consists of a transient mixture of degenerate and nearly free electrons, molecules, and ions. This regime challenges both experiment and analytical modeling, necessitating predictive ab initio atomistic computation, typically based on quantum mechanical Kohn-Sham density functional theory (KS-DFT). However, cubic computational scaling with temperature and system size prohibits the use of DFT through much of the warm dense matter regime. A recently developed stochastic approach to KS-DFT can be used at high temperatures, with the exact same accuracy as the deterministic approach, but the stochastic error can converge slowly and it remains expensive for intermediate temperatures (< 50 eV). Here we have developed a universal mixed stochastic-deterministic algorithm for DFT at any temperature. This approach leverages the physics of KS-DFT to seamlessly integrate the best aspects of these different approaches. We demonstrate that this method significantly accelerated self-consistent field calculations for temperatures from 3 to 50 eV, while producing stable molecular dynamics and accurate diffusion coefficients.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Pristine quantum criticality in a Kondo semimetal

The observation of quantum criticality in diverse classes of strongly correlated electron systems has been instrumental in establishing ordering principles, discovering new phases, and identifying the relevant degrees of freedom and interactions. At focus so far have been insulators and metals. Semimetals, which are of great current interest as candidate phases with nontrivial topology, are much less explored in experiments. Here, we study the Kondo semimetal CeRu 4 Sn 6 by magnetic susceptibility, specific heat, and inelastic neutron scattering experiments. The power-law divergence of the magnetic Grünesien ratio reveals that, unexpectedly, this compound is quantum critical without tuning. The dynamical energy over temperature scaling in the neutron response throughout the Brillouin zone and the temperature dependence of the static uniform susceptibility, indicate that temperature is the only energy scale in the criticality. Such behavior, which has been associated with Kondo destruction quantum criticality in metallic systems, could be generic in the semimetal setting.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Real-time gravitational replicas: formalism and a variational principle

This work is the first step in a two-part investigation of real-time replica wormholes. Here we study the associated real-time gravitational path integral and construct the variational principle that will define its saddle-points. We also describe the general structure of the resulting real-time replica wormhole saddles, setting the stage for construction of explicit examples. These saddles necessarily involve complex metrics, and thus are accessed by deforming the original real contour of integration. However, the construction of these saddles need not rely on analytic continuation, and our formulation can be used even in the presence of non-analytic boundary-sources. Furthermore, at least for replica- and CPT-symmetric saddles we show that the metrics may be taken to be real in regions spacelike separated from a so-called ‘splitting surface’. This feature is an important hallmark of unitarity in a field theory dual.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Investigating Electron Conductivity Regimes in the Bacterial Cytochrome Wire OmcS

The anaerobic bacterium Geobacter sulfurreducens produces extracellular, electronically conductive cytochrome polymer wires that are conductive over micron length scales. Structure models from cryo-electron microscopy data show OmcS wires form a linear chain of hemes along the protein wire axis, which is proposed as the structural basis supporting their electronic properties. However, the mechanism by which this heme arrangement supports long-range electronic conduction remains unknown. Structure models from cryo-electron microscopy data show these wires form a linear chain of hemes along the protein wire axis, which is proposed as the structural basis supporting their electronic properties. Existing computational models using static heme redox potentials and coupling energies fail to explain experimental observations, predicting conductances 10,000 to 100,000 times lower than measured values. Here, we investigate how dynamic disorder affects site energies, interheme coupling, and long-range electronic conductivity within these cytochrome wires. We introduce an approach to extract charge carrier site information directly from Kohn–Sham density functional theory, without employing projector schemes, and show that site and coupling energies are highly sensitive to changes in interheme geometry and the surrounding electrostatic environment. Unlike models that incorporate dynamic disorder as a thermally averaged quantity, our quantum charge carrier model incorporates proxies for dynamic disorder through decoherence corrections, yielding predicted diffusion coefficient closer to what is expected from experiment and comparable with other organic-based electronic materials. Based on these simulations, we propose that the instantaneous fluctuations of the local electrostatic environment can transiently lift energy degeneracies and delocalize charge carriers. Furthermore, these studies reveal how incorporating dynamic fluctuations associated with the environment resolves the discrepancy between theory and experiment in microbial cytochrome wires and highlight design principles for bioinspired, heme-based conductive materials.

Bioinorganic chemistry↗
DOE OSTI2022

Origin of the injection-dependent emission blueshift and linewidth broadening of III-nitride light-emitting diodes

III-nitride light-emitting diodes (LEDs) exhibit an injection-dependent emission blueshift and linewidth broadening that is severely detrimental to their color purity. By using first-principles multi-scale modeling that accurately captures the competition between polarization-charge screening, phase-space filling, and many-body plasma renormalization, we explain the current-dependent spectral characteristics of polar III-nitride LEDs fabricated with state-of-the-art quantum wells. Our analysis uncovers a fundamental connection between carrier dynamics and the injection-dependent spectral characteristics of light-emitting materials. For example, polar III-nitride LEDs offer poor control over their injection-dependent color purity due to their poor hole transport and slow carrier-recombination dynamics, which forces them to operate at or near degenerate carrier densities. Designs that accelerate carrier recombination and transport and reduce the carrier density required to operate LEDs at a given current density lessen their injection-dependent wavelength shift and linewidth broadening.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Computing the solubility of argon and xenon in molten sodium chloride and potassium chloride salts

Molten salt reactors (MSRs) offer significant advancements in nuclear reactor safety and efficiency by operating at higher temperatures and lower pressures compared to traditional reactors. A critical aspect of MSR operation involves understanding the solubility of fission byproducts, particularly noble gases, in the molten salts used. This study employs molecular dynamics (MD) simulations to compute Henry’s law constants and enthalpies of solvation for argon and xenon in molten sodium chloride (NaCl) and potassium chloride (KCl). We developed a new pairwise potential for the noble gas and salt interactions based on first principles calculations. We then used this potential to calculate Henry’s law constants of the two gases in the molten salts, which were modeled using both a rigid ion model (RIM) and a polarizable ion model (PIM). The solubility calculations, performed using the Widom insertion method, show qualitative agreement with limited experimental data, highlighting the temperature dependence and greater solubility of both gases in KCl compared to NaCl. Additionally, free volume analysis elucidated the role of available space within the molten salts in governing solubility trends. Our findings suggest that PIM trajectories provide more reliable predictions for noble gas solubility than RIM due to their accurate density representation. Furthermore, these results enhance understanding of gas solubility in MSR environments, and the methods can be readily extended to other systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Evidence for equilibrium exciton condensation in monolayer WTe 2

We present evidence that the two-dimensional bulk of monolayer WTe2 contains electrons and holes bound by Coulomb attraction—excitons—that spontaneously form in thermal equilibrium. On cooling from room temperature to 100 K, the conductivity develops a V-shaped dependence on electrostatic doping, while the chemical potential develops a step at the neutral point. These features are much sharper than is possible in an independent-electron picture, but they can be accounted for if electrons and holes interact strongly and are paired in equilibrium. Our calculations from first principles show that the exciton binding energy is larger than 100 meV and the radius as small as 4 nm, explaining their formation at high temperature and doping levels. Below 100 K, more strongly insulating behaviour is seen, suggesting that a charge-ordered state forms. The observed absence of charge density waves in this state is surprising within an excitonic insulator picture, but we show that it can be explained by the symmetries of the exciton wavefunction. Therefore, in addition to being a topological insulator, monolayer WTe2 exhibits strong correlations over a wide temperature range.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

High Accuracy Transition Metal Effective Cores for the Many-Body Diffusion Monte Carlo Method

Practical applications of the real-space diffusion Monte Carlo (DMC) method require the removal of core electrons, where currently localization approximations of semilocal potentials are generally used in the projector. Accurate calculations of complex solids and large molecules demand minimizing the impact of approximated atomic cores. Prior works have shown that the errors from such approximations can be sizable in both finite and periodic systems. In this work, we show that a class of differential pseudopotentials, known as pseudo-Hamiltonians, can be constructed for the 3d transition metal atoms, entirely removing the need for any localization scheme in the DMC projector. As a proof of principle, we demonstrate the approach for the case of Co. In order to minimize errors in the pseudo-Hamiltonian at the many-body level, we generalize the recently proposed correlation-consistent pseudopotential generation scheme to successively close semilocal representations of the differential potentials. Our generation scheme successfully produces potentials tailored specifically for real space projector quantum Monte Carlo methods with low error at the many-body level, i.e., with many-body scattering properties very close to relativistic all-electron results. In particular, we show that the agreement with respect to atomic and molecular quantities reach chemical accuracy in many cases-on par with the most accurate semilocal pseudopotentials available. Further, our pseudo-Hamiltonian generation scheme utilizes standard quantum chemistry codes designed only to work with semilocal pseudopotentials, enabling straightforward generation of pseudo-Hamiltonians for additional elements in future works.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Chiral Dirac Fermion in a Collinear Antiferromagnet

In a Dirac semimetal, the massless Dirac fermion has zero chirality, leading to surface states connected adiabatically to a topologically trivial surface state as well as vanishing anomalous Hall effect. Recently, it is predicted that in the nonrelativistic limit of certain collinear antiferromagnets, there exists a type of chiral "Dirac-like" fermion, whose dispersion manifests four-fold degenerate crossing points formed by spin-degenerate linear bands, with topologically protected Fermi arcs. Such an unconventional chiral fermion, protected by a hidden SU(2) symmetry in the hierarchy of an enhanced crystallographic group, namely spin space group, is not experimentally verified yet. Here, by angle-resolved photoemission spectroscopy measurements, we reveal the surface origin of the electron pocket at the Fermi surface in collinear antiferromagnet CoNb 3 S 6 . Combining with neutron diffraction and first-principles calculations, we suggest a multidomain collinear antiferromagnetic configuration, rendering the the existence of the Fermi-arc surface states induced by chiral Dirac-like fermions. Finally, our work provides spectral evidence of the chiral Dirac-like fermion caused by particular spin symmetry in CoNb 3 S 6 , paving an avenue for exploring new emergent phenomena in antiferromagnets with unconventional quasiparticle excitations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Nonequilibrium formulation of varying-temperature bit erasure

Landauer's principle states that erasing a bit of information at fixed temperature T costs at least $k$ B $T$ ln 2 units of work. Here we investigate erasure at varying temperature, to which Landauer's result does not apply. Here we formulate bit erasure as a stochastic nonequilibrium process involving a compression of configuration space, with physical and logical states associated in a symmetric way. Erasure starts and ends at temperature T, but temperature can otherwise vary with time in an arbitrary way. Defined in this way, erasure is governed by a set of nonequilibrium fluctuation relations that show that varying-temperature erasure can done with less work than $k$ B $T$ ln 2. As a result, erasure and the complementary process of bit randomization can be combined to form a work-producing engine cycle.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Using Hyperoptimized Tensor Networks and First-Principles Electronic Structure to Simulate the Experimental Properties of the Giant {Mn 84 } Torus

The single-molecule magnet {Mn 84 } is a challenge to theory because of its high nuclearity. Here, we directly compute two experimentally accessible observables, the field-dependent magnetization up to 75 T and the temperature-dependent heat capacity, using parameter-free theory. In particular, we use first-principles calculations to derive short- and long-range exchange interactions and compute the exact partition function of the resulting classical Potts and Ising spin models for all 84 Mn S = 2 spins to obtain observables. The latter computation is made possible by using hyperoptimized tensor network contractions, a technique developed to simulate quantum supremacy circuits. We also synthesize the magnet and measure its heat capacity and magnetization, observing qualitative agreement between theory and experiment and identifying an unusual bump in the heat capacity and a plateau in the magnetization. Our work also identifies some limitations of current theoretical modeling in large magnets, such as sensitivity to small, long-range exchange couplings.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Improved reference system for the corrected rigid spheres equation of state model

The Corrected Rigid Spheres (CRIS) EOS model, developed from fluid perturbation theory using a hard sphere reference system, has been successfully used to calculate the EOS of many materials, including gases and metals. The radial distribution function (RDF) plays a pivotal role in choosing the sphere diameter, through a variational principle, as well as the thermodynamic response. Despite its success, the CRIS model has some shortcomings in that it predicts too large a temperature for liquid-vapor critical points, can break down at large compression, and is computationally expensive. In this paper, we first demonstrate that an improved analytic representation of the hard sphere RDF does not alleviate these issues. Relaxing the strict adherence of the RDF to hard spheres allows an accurate fit to the isotherms and vapor dome of the Lennard-Jones fluid using an arbitrary reference system. Second order correction are eliminated, limiting the breakdown at large compression and significantly reducing the computation cost. The transferrability of the new model to real systems is demonstrated on argon, with an improved vapor dome compared to the original CRIS model.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Searching for ternary magnetic Zr–Fe–B compounds through deep machine learning

We use deep machine learning (ML) combined with first-principles calculations to search for energetically favorable ternary magnetic zirconium–iron borides. We show that an iterative ML approach enables efficient screening of vast structural libraries, effectively selecting promising candidates for subsequent first-principles investigations. Twenty-two new Fe-rich ternary compounds with formation energies within 60 meV atom −1 above the known ternary convex hull and with magnetic polarization larger than 0.6 T are identified, among which ten structures exhibit significant uniaxial anisotropy with magnetocrystalline anisotropy constant K 1 ⩾ 0.8 MJ m −3 , including a Zr 2 Fe 14 B phase. Such an ML-guided approach dramatically accelerates the discovery of rare-earth-free permanent magnetic materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Disorder-induced magnetoelastic behaviors of MnTexSbyBi1-x-y alloys

This dataset contains input and output files from density functional theory (DFT) simulations used to study the disorder-induced magnetoelastic behaviors of MnTexSbyBi1-x-y (0 ≤ x + y ≤ 1) alloys and their binary end members MnTe, MnSb, and MnBi. The alloys adopt the hexagonal NiAs-type (nickeline) structure and span ternary (MnTexSb1-x, MnTexBi1-x, MnBixSb1-x), and quaternary compositions across the full MnTe–MnSb–MnBi composition triangle. For each alloy composition, the dataset provides DFT calculations in three magnetic configurations: A-type antiferromagnetic (AFM), C-type AFM, and ferromagnetic (FM). Every magnetic configuration folder contains the fully relaxed crystal structure (CONTCAR), VASP input parameters (INCAR), and the main VASP output file (OUTCAR), from which total electronic energies, Mn magnetic moments, lattice parameters, and percent volume changes between magnetic states are extracted. These data are used to construct compositional phase diagrams, evaluate thermodynamic stability (formability), and map magnetoelastic responses across the alloy space. For A-type AFM and FM configurations, additional data are provided as follows: (i) FORCE_CONSTANTS and thermal_properties.yaml files at the top level of A-type_AFM/ and FM/ folders — present only for compositions marked with an asterisk (*) in Table I of the main text. These are derived from Phonopy finite-displacement calculations on full disordered 128-atom supercells and provide vibrational free energy, entropy (Svib)contribution from explicit disorder calculations. (Table I of the associated main manuscript) (ii) A VCA/ subfolder within A-type_AFM/ and FM/, containing FORCE_CONSTANTS and thermal_properties.yaml from Virtual Crystal Approximation phonon calculations (without spin-orbit coupling). VCA data are available for all compositions and are used to estimate vibrational contributions to the Gibbs free energy across the full composition space. (iii) A SOC/ subfolder containing CONTCAR, INCAR, and OUTCAR from spin-orbit coupling calculations, providing relativistic corrections to electronic energies and lattice parameters (Tables S2–S3 of the SM, and Table I of the main manuscript). (iv) A SOC/VCA/ subfolder containing FORCE_CONSTANTS and thermal_properties.yaml from VCA phonon calculations performed within the SOC framework, combining relativistic and vibrational thermodynamic corrections. The computed properties are used to map the AFM–FM magnetic crossover near MnTe0.75Sb0.25, demonstrate disorder- and spin-induced phonon broadening, identify a semiconductor-to-metal crossover, and quantify the pronounced magnetoelastic volume response near the magnetic phase boundary.

36 MATERIALS SCIENCE↗
DOE OSTI2025

The Impact of Carotenoid Energy Levels on the Exciton Dynamics and Singlet–Triplet Annihilation in Isolated Bacterial Light-Harvesting 2 Complexes

The light-harvesting 2 (LH2) complex of purple phototrophic bacteria plays a critical role in absorbing solar energy and distributing the excitation energy. Exciton dynamics within LH2 complexes are controlled by the structural arrangement and energy levels of the bacteriochlorophyll (BChl) and carotenoid (Car) pigments. However, there is still debate over the competing light-harvesting versus energy-dissipation pathways. In this work, we compared five variants of the LH2 complex from genetically modified strains of Rhodobacter sphaeroides, all containing the same BChls but different Cars with increasing conjugation: zeta-carotene (N = 7; LH2 Zeta ), neurosporene (N = 9; LH2 Neu ), spheroidene (N = 10; LH2 Spher ), lycopene (N = 11; LH2 Lyco ), and spirilloxanthin (N = 13; LH2 Spir ). Absorption measurements confirmed that the Car excited-state energy decreased with increasing conjugation. Similarly, fluorescence spectra showed that the B850 BChl emission peak had an increasing red shift from LH2 Zeta →(LH2 Neu /LH2 Spher )→LH2 Lyco →LH2 Spir . In contrast, time-resolved fluorescence and ultrafast transient absorption (fs-TA) revealed similar excited-state lifetimes (∼1 ns) for all complexes except LH2 Spir (∼0.7 ns). From fs-TA analysis, an additional ∼7 ps nonradiative dissipation step from B850 BChl was observed for LH2 Zeta . Further, singlet− singlet and singlet−triplet annihilation studies showed a ∼50% average fluorescence lifetime reduction in LH2Zeta at high laser power and high repetition rate, compared to ∼10−15% reductions in LH2 Neu /LH2 Spher /LH2 Lyco and minimal lifetime change in LH2 Spir . In LH2 Zeta , the fastest decay component (<50 ps) became prominent at high repetition rates, consistent with strong singlet−triplet annihilation. Nanosecond TA measurements revealed long-lived (>40 μs) BChl triplet states in LH2 Zeta and signs of damage caused by singlet oxygen, whereas other LH2s showed faster triplet quenching (∼18 ns) by Cars. These findings highlight a key design principle of LH2 complexes: the Car triplet energy must be significantly lower than the BChl triplet energy to efficiently quench BChl triplets that otherwise act as potent “trap states,” causing exciton annihilation in laser-based experiments or photodamage in native membranes.

Absorption↗
DOE OSTI2023

Understanding the Mechanism of Secondary Cation Release from the (001) Surface of Li(Ni 1/3 Mn 1/3 Co 1/3 )O 2 : Insights from First-Principles

The transformations of complex metal oxides in aqueous settings must be studied to form a chemical understanding of how technologically relevant nanomaterials impact the environment upon disposal. Owing to the inherent heterogeneity and structural complexity of the ternary intercalation material Li(Ni x Mn y Co 1-x-y )O 2 (NMC), the mechanisms of chemical processes at the solid–water interfac e are challenging to model. Here, density functional theory (DFT) + solvent ion methodology is used to study the energetics of stepwise release of two surface metals following unique pathways. Further, the study spans different combinations of metal removal and also considers unique patterns of defects formed by modeling the NMC surface in supercells. The approach here also considers the equilibration of the surface with the surroundings between successive metal removals. A key finding is that a second metal removal prefers to proceed at a metal lattice site adjacent to the initial defect, and this is attributed in part to how the resulting slab with two metal vacancies maintains the most antiferromagnetic couplings between the remaining Ni/Mn.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗