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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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At least 433 records · Page 24
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

A new computational framework for spinor-based relativistic exact two-component calculations using contracted basis functions

Here, a new computational framework for spinor-based relativistic exact two-component (X2C) calculations is developed using contracted basis sets with a spin–orbit contraction scheme. Generally contracted, j-adapted basis sets of p-block elements using primitive functions in the correlation-consistent basis sets are constructed for the X2C Hamiltonian with atomic mean-field spin–orbit integrals (the X2CAMF scheme). The contraction coefficients are taken from atomic X2CAMF Hartree–Fock spinors, thereby following the simple concept of a linear combination of atomic orbitals. Benchmark calculations of spin–orbit splittings, equilibrium bond lengths, and harmonic vibrational frequencies demonstrate the accuracy and efficacy of the j-adapted spin–orbit contraction scheme.

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

Calculation of spin–orbit couplings using RASCI spinless one-particle density matrices: Theory and applications

Here we present the formalism and implementation for calculations of spin–orbit couplings (SOCs) using the Breit–Pauli Hamiltonian and non-relativistic wave functions described by the restricted active space configuration interaction (RASCI) method with general excitation operators of spin-conserving spin-flipping, ionizing, and electron-attaching types. The implementation is based on the application of the Wigner–Eckart theorem within the spin space, which enables the calculation of the entire SOC matrix based on the explicit calculation of just one transition between the two spin multiplets. Numeric results for a diverse set of atoms and molecules highlight the importance of a balanced treatment of correlation and adequate basis sets and illustrate the overall robust performance of RASCI SOCs. The new implementation is a useful addition to the methodological toolkit for studying spin-forbidden processes and molecular magnetism.

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

Analysis of Fourth-, Fifth-, and Infinite-Order Triple Excitations in Unitary Coupled Cluster Theory

Here, in this work, we introduce a perturbative correction to the unitary coupled cluster method with single and double excitations (UCCSD) that incorporates the effects of missing triple excitations through fifth-order in many-body perturbation theory (MBPT). Referred to as UCCSD[T-5], this method is benchmarked alongside the previously developed UCCSD[T] to lend insight into the behavior of perturbative triples corrections relative to UCCSDT, which inherently provides an infinite-order treatment of triple excitations, as well as full configuration interaction (FCI). Two key findings emerge from this analysis. First, UCCSD[T] consistently yields ground-state energies in closest agreement with FCI, outperforming both UCCSD[T-5] and UCCSDT. Second, UCCSD[T-5] largely emulates the behavior of UCCSDT, suggesting a close relationship between fifth- and infinite-order triple-excitation contributions. Given the growing interest in UCC ansätze for quantum computing and the limitations of current quantum hardware, these results highlight the potential of classically computed perturbative corrections within UCC theory to capture triple-excitation effects without the additional quantum resources required by the UCCSDT ansatz.

Windom, Zachary W. [Oak Ridge National Laboratory ↗
DOE OSTI2016

Calculation of the neutron diffusion equation by using Homotopy Perturbation Method

The distribution of the neutrons in a nuclear fuel element in the nuclear reactor core can be calculated by the neutron diffusion theory. It is the basic and the simplest approximation for the neutron flux function in the reactor core. In this study, the neutron flux function is obtained by the Homotopy Perturbation Method (HPM) that is a new and convenient method in recent years. One-group time-independent neutron diffusion equation is examined for the most solved geometrical reactor core of spherical, cubic and cylindrical shapes, in the frame of the HPM. It is observed that the HPM produces excellent results consistent with the existing literature.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2011

Many-body physics in the classical-field description of a degenerate Bose gas

The classical-field formalism has been widely applied in the calculation of normal correlation functions, and the characterization of condensation, in finite-temperature Bose gases. Here we discuss the extension of this method to the calculation of more general correlations, including the so-called anomalous correlations of the field, without recourse to symmetry-breaking assumptions. Our method is based on the introduction of U(1)-symmetric classical-field variables analogous to the modified quantum ladder operators of number-conserving approaches to the degenerate Bose gas, and allows us to rigorously quantify the anomalous and non-Gaussian character of the field fluctuations. We compare our results for anomalous correlation functions with the predictions of mean-field theories, and demonstrate that the nonlinear classical-field dynamics incorporate a full description of many-body processes which modify the effective mean-field potentials experienced by condensate and noncondensate atoms. We discuss the role of these processes in shaping the condensate mode, and thereby demonstrate the consistency of the Penrose-Onsager definition of the condensate orbital in the classical-field equilibrium. We consider the contribution of various noncondensate-field correlations to the overall suppression of density fluctuations and interactions in the field, and demonstrate the distinct roles of phase and density fluctuations in the transition of the field to the normal phase.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Distinguishing erbium dopants in Y 2 O 3 by site symmetry: Ab initio theory of two spin-photon interfaces

Here, we present a first-principles study of the defect formation and electronic structure of erbium (Er)–doped yttria (Y 2 O 3 ). This is an emerging material for spin-photon interfaces in quantum information science due to the narrow-linewidth optical emission from Er dopants at standard telecommunication wavelengths and their potential for quantum memories and transducers. We calculate formation energies of neutral and negatively and positively charged Er dopants and find the charge-neutral configuration to be the most stable, consistent with experiment. Of the two substitutional sites of Er for Y, the C 2 (more relevant for quantum memories) and C 3i (more relevant for quantum transduction), we identify the former as possessing the lowest formation energy. The electronic properties are calculated using the Perdew-Burke-Ernzerhof functional along with the Hubbard U parameter and spin-orbit coupling, which yields a ~ 6 μ B orbital and a ~ 3 μ B spin magnetic moment, and 11 electrons in the Er 4 f shell, confirming the formation of charge-neutral Er 3+ . This standard density functional theory approach underestimates the band gap of the host and lacks a first-principles justification for U . To overcome these issues we performed screened hybrid functional calculations, including a negative U for the 4 f orbitals, with mixing (α) and screening (w) parameters. These produced robust electronic features with slight modifications in the band gap and the 4 f splittings depending on the choice of tuning parameters. We also computed the many-particle electronic excitation energies and compared them with experimental values from photoluminescence.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Computational insight into the capacitive performance of graphene edge planes

Recent experiments have shown that electric double-layer capacitors utilizing electrodes consisting of graphene edge plane exhibit higher capacitance than graphene basal plane. However, theoretical understanding of this capacitance enhancement is still limited. Here we applied a self-consistent joint density functional theory calculation on the electrode/electrolyte interface and found that the capacitance of graphene edge plane depends on the edge type: zigzag edge has higher capacitance than armchair edge due to the difference in their electronic structures. We further examined the quantum, dielectric, and electric double-layer (EDL) contributions to the total capacitance of the edge-plane electrodes. Classical molecular dynamics simulation found that the edge planes have higher EDL capacitance than the basal plane due to better adsorption of counter-ions and higher solvent accessible surface area. Finally, our work therefore has elucidated the capacitive energy storage in graphene edge planes that take into account both the electrode's electronic structure and the EDL structure.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Magnetic order driven ultrafast phase transition in NdNiO 3

Ultrashort x-ray pulses can be used to disentangle magnetic and structural dynamics and are accordingly utilized here to study the photoexcitation of NdNiO 3 (NNO), a model nickelate exhibiting structural and magnetic dynamics that conspire to induce an insulator-to-metal transition (IMT). Here, during the course of the photoinduced IMT with above-gap excitation, we observe an ultrafast (< 180 fs) quenching of magnetic order followed by a time delayed collapse of the insulating phase probed by x-ray absorption and THz transmission (450 fs) that correlates with the slowest optical phonon mode involved in the structural transition. A simultaneous order-disorder response at the Ni site and displacive response at the Nd site coexist in the ultrafast magnetic response. Crucially, we observe the optical phonon through its coherent coupling with Nd magnetic order, demonstrating that the magnetic and structural degrees of freedom both contribute in driving the IMT. Density functional theory calculations reveal a consistent scenario where optically driven intersite charge transfer drives a collapse of antiferromagnetic order that in turn destabilizes the charge-ordered phase resulting in an IMT. These experiments provide different modalities for the control of electronic phase transitions in quantum materials based on the ultrafast interplay between structural and magnetic orders created by femtosecond photoexcitation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

First-principles characterization of the magnetic properties of Cu 2 (OH) 3 Br

Low-dimensional spin-1/2 transition metal oxides and oxyhalides continue to be at the forefront of research investigating nonclassical phases such as quantum spin liquids. In this work, we examine the magnetic properties of the oxyhalide Cu 2 (OH) 3 Br in the botallackite structure using first-principles density functional theory, linear spin-wave theory, and exact diagonalization calculations. This quasi-two-dimensional system consists of Cu 2+ S = 1/2 moments arranged on a distorted triangular lattice. Our exact diagonalization calculations, which rely on a first-principles-based magnetic model, generate spectral functions consistent with inelastic neutron scattering data. By performing computational experiments to disentangle the chemical and steric effects of the halide ions, we find that the dominant effect of the halogen ions is steric in the Cu 2 (OH) 3 X series of compounds.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Pairing Dynamics in Low-energy Nuclear Collisions

Superfluidity is a generic feature of various quantum systems at low temperatures and it is in particular important for the description of dynam- ics of low energy nuclear reactions. The Time-Dependent Density Func- tional Theory (TDDFT) is, to date, the only microscopic method which takes into account in a consistent way far-from-equilibrium dynamics of pairing field and single-particle degrees of freedom. Here, the local version of TDDFT, so-called TDSLDA, is particularly useful for the description of nuclear reactions and is well-suited for leadership class computers of hybrid (CPU+GPU) architecture. The preliminary results obtained for collisions involving both medium-mass and heavy nuclei at the energies around the Coulomb barrier are presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2013

Functional Wigner representation of quantum dynamics of Bose-Einstein condensate

We develop a method of simulating the full quantum field dynamics of multi-mode multi-component Bose-Einstein condensates in a trap. We use the truncated Wigner representation to obtain a probabilistic theory that can be sampled. This method produces c-number stochastic equations which may be solved using conventional stochastic methods. The technique is valid for large mode occupation numbers. We give a detailed derivation of methods of functional Wigner representation appropriate for quantum fields. Our approach describes spatial evolution of spinor components and properly accounts for nonlinear losses. Such techniques are applicable to calculating the leading quantum corrections, including effects such as quantum squeezing, entanglement, EPR correlations, and interactions with engineered nonlinear reservoirs. By using a consistent expansion in the inverse density, we are able to explain an inconsistency in the nonlinear loss equations found by earlier authors.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2016

Determining polarizable force fields with electrostatic potentials from quantum mechanical linear response theory

We developed a new method to calculate the atomic polarizabilities by fitting to the electrostatic potentials (ESPs) obtained from quantum mechanical (QM) calculations within the linear response theory. This parallels the conventional approach of fitting atomic charges based on electrostatic potentials from the electron density. Our ESP fitting is combined with the induced dipole model under the perturbation of uniform external electric fields of all orientations. QM calculations for the linear response to the external electric fields are used as input, fully consistent with the induced dipole model, which itself is a linear response model. The orientation of the uniform external electric fields is integrated in all directions. The integration of orientation and QM linear response calculations together makes the fitting results independent of the orientations and magnitudes of the uniform external electric fields applied. Another advantage of our method is that QM calculation is only needed once, in contrast to the conventional approach, where many QM calculations are needed for many different applied electric fields. The molecular polarizabilities obtained from our method show comparable accuracy with those from fitting directly to the experimental or theoretical molecular polarizabilities. Since ESP is directly fitted, atomic polarizabilities obtained from our method are expected to reproduce the electrostatic interactions better. Our method was used to calculate both transferable atomic polarizabilities for polarizable molecular mechanics’ force fields and nontransferable molecule-specific atomic polarizabilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

Classical geometry to quantum behavior correspondence in a virtual extra dimension

In the Lorentz invariant formalism of compact space-time dimensions the assumption of periodic boundary conditions represents a consistent semi-classical quantization condition for relativistic fields. In Dolce (2011) we have shown, for instance, that the ordinary Feynman path integral is obtained from the interference between the classical paths with different winding numbers associated with the cyclic dynamics of the field solutions. By means of the boundary conditions, the kinematical information of interactions can be encoded on the relativistic geometrodynamics of the boundary, see Dolce (2012) . Furthermore, such a purely four-dimensional theory is manifestly dual to an extra-dimensional field theory. The resulting correspondence between extra-dimensional geometrodynamics and ordinary quantum behavior can be interpreted in terms of AdS/CFT correspondence. By applying this approach to a simple Quark-Gluon-Plasma freeze-out model we obtain fundamental analogies with basic aspects of AdS/QCD phenomenology. - Highlights: Black-Right-Pointing-Pointer Quantum behavior is related to the intrinsic periodicity of isolated systems. Black-Right-Pointing-Pointer A periodic phenomenon can be parameterized by a virtual extra dimension. Black-Right-Pointing-Pointer KK modes are used to describe the quantum excitations. Black-Right-Pointing-Pointer 5D classical geometry encodes 4D quantum behavior. Black-Right-Pointing-Pointer Geometrodynamical description of AdS/QCD as modulation of space-time periodicity.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2016

Skew-flavored dark matter

We explore a novel flavor structure in the interactions of dark matter with the Standard Model. We consider theories in which both the dark matter candidate, and the particles that mediate its interactions with the Standard Model fields, carry flavor quantum numbers. The interactions are skewed in flavor space, so that a dark matter particle does not directly couple to the Standard Model matter fields of the same flavor, but only to the other two flavors. This framework respects minimal flavor violation and is, therefore, naturally consistent with flavor constraints. We study the phenomenology of a benchmark model in which dark matter couples to right-handed charged leptons. In large regions of parameter space, the dark matter can emerge as a thermal relic, while remaining consistent with the constraints from direct and indirect detection. The collider signatures of this scenario include events with multiple leptons and missing energy. In conclusion, these events exhibit a characteristic flavor pattern that may allow this class of models to be distinguished from other theories of dark matter.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2026

Single-Particle Insights Into the Electronic Structure and Enhanced Stability of CsPbBr 3 /FAPbBr 3 Core/Crown Nanoplatelets at the Nanometer Scale

Colloidal perovskite nanoplatelets (NPLs), despite their exceptional optoelectronic properties, face significant challenges due to their intrinsic instability and trap-assisted non-radiative recombination. Although many studies employing surface engineering, such as selecting ligands or coating to passivate defects, have demonstrated improved optoelectronic properties, these enhancements are typically inferred from bulk-ensemble measurements; the effects at the single-particle level remain elusive. Here, we conduct single-particle-level studies using scanning tunneling spectroscopy (STS) on a unique core–crown system, CsPbBr 3 @FAPbBr 3 NPLs, where the lateral surfaces of the CsPbBr 3 core are coated with an FAPbBr 3 crown. Experimental density-of-states (DOS) analysis reveals a 47% reduction in deep-trap states in core-crown NPLs compared to core-only NPLs, consistent with nearly two-fold enhancements in photoluminescence quantum yields. Progressive I–V sweep measurements demonstrate superior electrical stability in core-crown NPLs, preserving band structure with minimal degradation, while core-only NPLs exhibit rapid bandgap shrinkage and trap formation. Density functional theory (DFT) calculations indicate that FA incorporation distorts Pb octahedral lattice, widening the bandgap. This study elucidates how surface engineering modulates charge localization, passivates defects, and enhances stability at the single-particle level. Moreover, by uncovering bias-induced trap states in single unpassivated NPLs, this study establishes a precise, robust approach for characterizing emerging perovskite nanocrystals.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2019

Crystal growth and quantum oscillations in the topological chiral semimetal CoSi

Here, we survey the electrical transport properties of single-crystalline, topological chiral semimetal CoSi grown via different methods. High-quality CoSi single crystals were found in the growth from a tellurium solution. The sample's high carrier mobility enables us to observe quantum oscillations (QOs) in its thermoelectrical signals. Our analysis of QOs reveals two spherical Fermi surfaces around the R point in its Brillouin zone corner. The extracted Berry phases of these electron orbits are consistent with the -2 chiral charge as reported in density functional theory (DFT) calculations. A detailed analysis of the QOs reveals that the spin-orbit-coupling-induced band splitting is less than 2 meV near the Fermi level, one order of magnitude smaller than our DFT calculation. We also report a large phonon-drag-induced Nernst effect in CoSi at intermediate temperatures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Low-temperature phonoemissive tunneling rates in single molecule magnets

Tunneling between the two lowest energy levels of single molecule magnets with Ising type anisotropy, accompanied by the emission or absorption of phonons, is considered. Quantitatively accurate calculations of the rates for such tunneling are performed for a model Hamiltonian especially relevant to the best studied example, Fe{sub 8}. Two different methods are used: high-order perturbation theory in the spin–phonon interaction and the non-Ising-symmetric parts of the spin Hamiltonian, and a novel semiclassical approach based on spin-coherent-state-path-integral instantons. The methods are found to be in good quantitative agreement with other, and consistent with previous approaches to the problem. The implications of these results for magnetization of molecular solids of these molecules are discussed briefly.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗