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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 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Resolution-of-identity stochastic time-dependent configuration interaction for dissipative electron dynamics in strong fields

In this contribution, we introduce a method for simulating dissipative, ultrafast many-electron dynamics in intense laser fields. The method is based on the norm-conserving stochastic unraveling of the dissipative Liouville-von Neumann equation in its Lindblad form. The N-electron wave functions sampling the density matrix are represented in the basis of singly excited configuration state functions. The interaction with an external laser field is treated variationally and the response of the electronic density is included to all orders in this basis. The coupling to an external environment is included via relaxation operators inducing transition between the configuration state functions. Single electron ionization is represented by irreversible transition operators from the ionizing states to an auxiliary continuum state. The method finds its efficiency in the representation of the operators in the interaction picture, where the resolution-of-identity is used to reduce the size of the Hamiltonian eigenstate basis. The zeroth-order eigenstates can be obtained either at the configuration interaction singles level or from a time-dependent density functional theory reference calculation. The latter offers an alternative to explicitly time-dependent density functional theory which has the advantage of remaining strictly valid for strong field excitations while improving the description of the correlation as compared to configuration interaction singles. The method is tested on a well-characterized toy system, the excitation of the low-lying charge transfer state in LiCN.

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

Charge-density-wave melting in the one-dimensional Holstein model

We study the Holstein model of spinless fermions, which at half filling exhibits a quantum phase transition from a metallic Tomonaga-Luttinger liquid phase to an insulating charge-density-wave (CDW) phase at a critical electron-phonon coupling strength. In our work, we focus on the real-time evolution starting from two different types of initial states that are CDW ordered: (i) ideal CDW states with and without additional phonons in the system and (ii) correlated ground states in the CDW phase. We identify the mechanism for CDW melting in the ensuing real-time dynamics and show that it strongly depends on the type of initial state. We focus on the far-from-equilibrium regime and emphasize the role of electron-phonon coupling rather than dominant electronic correlations, thus complementing a previous study of photoinduced CDW melting [H. Hashimoto and S. Ishihara, Phys. Rev. B 96, 035154 (2017)]. The numerical simulations are performed by means of matrix-product-state based methods with a local basis optimization (LBO). Within these techniques, one rotates the local (bosonic) Hilbert spaces adaptively into an optimized basis that can then be truncated while still maintaining a high precision. In this work, we extend the time-evolving block decimation (TEBD) algorithm with LBO, previously applied to single-polaron dynamics, to a half-filled system. We demonstrate that in some parameter regimes, a conventional TEBD method without LBO would fail. Furthermore, we introduce and use a ground-state density-matrix renormalization group method for electron-phonon systems using local basis optimization. In our examples, we account for up to M ph =40 bare phonons per site by working with O(10) optimal phonon modes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Synergy between pair coupled cluster doubles and pair density functional theory

Pair coupled cluster doubles (pCCD) has been recently studied as a method capable of accounting for static correlation with low polynomial cost. We present three combinations of pCCD with Kohn–Sham functionals of the density and on-top pair density (the probability of finding two electrons on top of each other) to add dynamic correlation to pCCD without double counting. With a negligible increase in computational cost, these pCCD+DFT blends greatly improve upon pCCD in the description of typical problems where static and dynamic correlations are both important. We argue that—as a black-box method with low scaling, size-extensivity, size-consistency, and a simple quasidiagonal two-particle density matrix—pCCD is an excellent match for pair density functionals in this type of fusion of multireference wavefunctions with DFT.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

ELSI — An open infrastructure for electronic structure solvers

Routine applications of electronic structure theory to molecules and periodic systems need to compute the electron density from given Hamiltonian and, in case of non-orthogonal basis sets, overlap matrices. System sizes can range from few to thousands or, in some examples, millions of atoms. Different discretization schemes (basis sets) and different system geometries (finite non-periodic vs. infinite periodic boundary conditions) yield matrices with different structures. The ELectronic Structure Infrastructure (ELSI) project provides an open-source software interface to facilitate the implementation and optimal use of high-performance solver libraries covering cubic scaling eigensolvers, linear scaling density-matrix-based algorithms, and other reduced scaling methods in between. In this paper, we present recent improvements and developments inside ELSI, mainly covering (1) new solvers connected to the interface, (2) matrix layout and communication adapted for parallel calculations of periodic and/or spin-polarized systems, (3) routines for density matrix extrapolation in geometry optimization and molecular dynamics calculations, and (4) general utilities such as parallel matrix I/O and JSON output. The ELSI interface has been integrated into four electronic structure code projects (DFTB+, DGDFT, FHI-aims, SIESTA), allowing us to rigorously benchmark the performance of the solvers on an equal footing. Based on results of a systematic set of large-scale benchmarks performed with Kohn–Sham density-functional theory and density-functional tight-binding theory, we identify factors that strongly affect the efficiency of the solvers, and propose a decision layer that assists with the solver selection process. As a result, we describe a reverse communication interface encoding matrix-free iterative solver strategies that are amenable, e.g., for use with planewave basis sets.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Assessment of DFT functionals for a minimal nitrogenase [Fe(SH) 4 H]- model employing state-of-the-art ab initio methods

We have designed a [Fe(SH)4H]- model with the fifth proton binding either to Fe or S. We show that the energy difference between these two isomers (ΔE) is hard to estimate with quantum-mechanical (QM) methods. For example, different density functional theory (DFT) methods give ΔE estimates that vary by almost 140 kJ/mol, mainly depending on the amount of exact Hartree–Fock included (0%–54%). The model is so small that it can be treated by many high-level QM methods, including coupled-cluster (CC) and multiconfigurational perturbation theory approaches. With extrapolated CC series (up to fully connected coupled-cluster calculations with singles, doubles, and triples) and semistochastic heat-bath configuration interaction methods, we obtain results that seem to be converged to full configuration interaction results within 5 kJ/mol. Our best result for ΔE is 101 kJ/mol. With this reference, we show that M06 and B3LYP-D3 give the best results among 35 DFT methods tested for this system. Brueckner doubles coupled cluster with perturbaitve triples seems to be the most accurate coupled-cluster approach with approximate triples. CCSD(T) with Kohn–Sham orbitals gives results within 4–11 kJ/mol of the extrapolated CC results, depending on the DFT method. Single-reference CC calculations seem to be reasonably accurate (giving an error of ~5 kJ/mol compared to multireference methods), even if the D1 diagnostic is quite high (0.25) for one of the two isomers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Hybrid programming-model strategies for GPU offloading of electronic structure calculation kernels

To address the challenge of performance portability and facilitate the implementation of electronic structure solvers, we developed the basic matrix library (BML) and Parallel, Rapid O(N), and Graph-based Recursive Electronic Structure Solver (PROGRESS) library. The BML implements linear algebra operations necessary for electronic structure kernels using a unified user interface for various matrix formats (dense and sparse) and architectures (CPUs and GPUs). Focusing on density functional theory and tight-binding models, PROGRESS implements several solvers for computing the single-particle density matrix and relies on BML. In this paper, we describe the general strategies used for these implementations on various computer architectures, using OpenMP target functionalities on GPUs, in conjunction with third-party libraries to handle performance critical numerical kernels. In this study, we demonstrate the portability of this approach and its performance in benchmark problems.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Interplay between fractional quantum Hall liquid and crystal phases at low filling

The nature of the state at low Landau-level filling factors has been a long-standing puzzle in the field of the fractional quantum Hall effect (FQHE). While theoretical calculations suggest that a crystal is favored at filling factors $\nu$≲1/6, experiments show, at somewhat elevated temperatures, minima in the longitudinal resistance that are associated with fractional quantum Hall effect at $\nu$ 1/7, 2/11, 2/13, 3/19, 1/9, 2/15, and 2/17, which belong to the standard sequences $\nu$ =n/(6n ± 1) and $\nu$=n/(8n ± 1). To address this paradox, we investigate the nature of some of the low-$\nu$ states, specifically $\nu$= 1/7, 2/13, and 1/9, by variational Monte Carlo, density matrix renormalization group, and exact diagonalization methods. We conclude that in the thermodynamic limit, these are likely to be incompressible fractional quantum Hall liquids, albeit with strong short-range crystalline correlations. Finally, this suggests a natural explanation for the experimentally observed behavior and a rich phase diagram that admits, in the low-disorder limit, a multitude of crystal-FQHE liquid transitions as the filling factor is reduced.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Search for a standard model Higgs boson produced in association with a top-quark pair and decaying to bottom quarks using a matrix element method

A search for a standard model Higgs boson produced in association with a top-quark pair and decaying to bottom quarks is presented. Events with hadronic jets and one or two oppositely charged leptons are selected from a data sample corresponding to an integrated luminosity of 19.5fb -1 collected by the CMS experiment at the LHC in pp collisions at a centre-of-mass energy of 8TeV. In order to separate the signal from the larger tt¯ + jets background, this analysis uses a matrix element method that assigns a probability density value to each reconstructed event under signal or background hypotheses. The ratio between the two values is used in a maximum likelihood fit to extract the signal yield. The results are presented in terms of the measured signal strength modifier, μ, relative to the standard model prediction for a Higgs boson mass of 125GeV. The observed (expected) exclusion limit at a 95 % confidence level is μ < 4.2 (3.3), corresponding to a best fit value μ^ = 1.2 +1.6 -1.5 .

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2017

The Impacts of Source Location in Tomographic Gamma Scanning - 17324

Canberra Industries has recently designed and built a Tomographic Gamma Scanning (TGS) system for the deployment in a nuclear facility. The TGS technique combines high-resolution gamma spectroscopy with low spatial resolution 3-dimensional image reconstruction to provide increased accuracy over traditional approaches for the assay of non-uniform source distributions in low-to medium-density containers. The TGS system has been optimized to measure 120 liter drums and has been equipped to use various collimators and attenuators to assay containers under a wide range of operational conditions. In this paper, we report on experimental work using TGS systems aimed at evaluating the effects of source locations at the limits of volume elements, or voxels, defined in the image reconstruction. These include sources placed at voxel boundaries within a single vertical layer and sources placed in the lowest and highest possible vertical positions within the containers. Building upon previous studies, the accuracy of the TGS system was also assessed by varying the radial position of a point source within a vertical segment. The robustness of the TGS image reconstruction algorithm to location of the sources location was also analyzed as a function of matrix density and gamma-ray energy. Methods to reduce the biases from source location at extreme positions within the container were implemented and tested. The results from this work have been used to better understand the total measurement uncertainty (TMU) and analysis methodology used in TGS systems currently deployed and under development. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

TU-F-18A-02: Iterative Image-Domain Decomposition for Dual-Energy CT

Purpose: Dual energy CT (DECT) imaging plays an important role in advanced imaging applications due to its material decomposition capability. Direct decomposition via matrix inversion suffers from significant degradation of image signal-to-noise ratios, which reduces clinical value. Existing de-noising algorithms achieve suboptimal performance since they suppress image noise either before or after the decomposition and do not fully explore the noise statistical properties of the decomposition process. We propose an iterative image-domain decomposition method for noise suppression in DECT, using the full variance-covariance matrix of the decomposed images. Methods: The proposed algorithm is formulated in the form of least-square estimation with smoothness regularization. It includes the inverse of the estimated variance-covariance matrix of the decomposed images as the penalty weight in the least-square term. Performance is evaluated using an evaluation phantom (Catphan 600) and an anthropomorphic head phantom. Results are compared to those generated using direct matrix inversion with no noise suppression, a de-noising method applied on the decomposed images, and an existing algorithm with similar formulation but with an edge-preserving regularization term. Results: On the Catphan phantom, our method retains the same spatial resolution as the CT images before decomposition while reducing the noise standard deviation of decomposed images by over 98%. The other methods either degrade spatial resolution or achieve less low-contrast detectability. Also, our method yields lower electron density measurement error than direct matrix inversion and reduces error variation by over 97%. On the head phantom, it reduces the noise standard deviation of decomposed images by over 97% without blurring the sinus structures. Conclusion: We propose an iterative image-domain decomposition method for DECT. The method combines noise suppression and material decomposition into an iterative process and achieves both goals simultaneously. The proposed algorithm shows superior performance on noise suppression with high image spatial resolution and low-contrast detectability. This work is supported by a Varian MRA grant.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Real-space formulation of the stress tensor for O (N) density functional theory: Application to high temperature calculations

We present an accurate and efficient real-space formulation of the Hellmann–Feynman stress tensor for O (N) Kohn–Sham density functional theory (DFT). While applicable at any temperature, the formulation is most efficient at high temperature where the Fermi–Dirac distribution becomes smoother and the density matrix becomes correspondingly more localized. We first rewrite the orbital-dependent stress tensor for real-space DFT in terms of the density matrix, thereby making it amenable to O (N) methods. We then describe its evaluation within the O (N) infinite-cell Clenshaw–Curtis Spectral Quadrature (SQ) method, a technique that is applicable to metallic and insulating systems, is highly parallelizable, becomes increasingly efficient with increasing temperature, and provides results corresponding to the infinite crystal without the need of Brillouin zone integration. We demonstrate systematic convergence of the resulting formulation with respect to SQ parameters to exact diagonalization results and show convergence with respect to mesh size to the established plane wave results. Here, we employ the new formulation to compute the viscosity of hydrogen at 10 6 K from Kohn–Sham quantum molecular dynamics, where we find agreement with previous more approximate orbital-free density functional methods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Analysis of band structure, transmission properties, and dispersion behavior of THz wave in one-dimensional parabolic plasma photonic crystal

The photonic band gap of obliquely incident terahertz electromagnetic waves in a one-dimensional plasma photonic crystal is studied. The periodic structure consists of lossless dielectric and inhomogeneous plasma with a parabolic density profile. The dispersion relation and the THz wave transmittance are analyzed based on the electromagnetic equations and transfer matrix method. The dependence of effective plasma frequency and photonic band gap characteristics on dielectric and plasma thickness, plasma density, and incident angle are discussed in detail. A theoretical calculation for effective plasma frequency is presented and compared with numerical results. Results of these two methods are in good agreement.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2014

Global solutions of restricted open-shell Hartree-Fock theory from semidefinite programming with applications to strongly correlated quantum systems

We present a density matrix approach for computing global solutions of restricted open-shell Hartree-Fock theory, based on semidefinite programming (SDP), that gives upper and lower bounds on the Hartree-Fock energy of quantum systems. While wave function approaches to Hartree-Fock theory yield an upper bound to the Hartree-Fock energy, we derive a semidefinite relaxation of Hartree-Fock theory that yields a rigorous lower bound on the Hartree-Fock energy. We also develop an upper-bound algorithm in which Hartree-Fock theory is cast as a SDP with a nonconvex constraint on the rank of the matrix variable. Equality of the upper- and lower-bound energies guarantees that the computed solution is the globally optimal solution of Hartree-Fock theory. The work extends a previously presented method for closed-shell systems [S. Veeraraghavan and D. A. Mazziotti, Phys. Rev. A 89, 010502–R (2014)]. For strongly correlated systems the SDP approach provides an alternative to the locally optimized Hartree-Fock energies and densities with a certificate of global optimality. Applications are made to the potential energy curves of C{sub 2}, CN, Cr {sub 2}, and NO {sub 2}.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Electronic Structure Theory and Novel Materials

This grant supported research on electronic structure and materials theory, with focus on three main issues: (i) novel techniques to deal with correlation in the electronic ground-state, (ii) topological materials, (iii) the phase diagram of lattice spin models. Regarding (i), we applied to the homogeneous electron liquid an approach that we previously developed in the context of molecular systems. In this scheme the electronic occupation probabilities and the natural spin orbitals are used to construct an approximate two-body density matrix for the electronic ground-state. Regarding (ii) we used standard electronic structure methods based on density functional theory to model topological materials and interpret experimental observations. Finally, regarding (iii) we further developed a numerical approach to compute the renormalized couplings within real space renormalization group theory in the context of lattice spin models. The main findings were the following. (i) We found that with our approximate two-body density matrix, which works well for small molecules, is not sufficiently accurate for condensed phase systems. Missing a systematic way of improving on the adopted approximations, we decided not to pursue this approach. (ii) We performed two studies. In one, we investigated the influence of Te defects on the topological properties of a WTe2 monolayer, finding that while Te vacancies, even in modest concentration, destroy the topological character, Te adatoms do not, consistent with a recent experiment. In another study, we predicted Weyl semimetal character and strong anomalous Hall effect in the Heusler compensated ferrimagnet Ti2MnAl. (iii) We developed a new Monte Carlo method to do real space renormalization group calculations for lattice spin models. We subsequently extended the scheme to deal with lattice spin models in presence of quenched disorder, finding that the approach can distinguish systems with finite and strong disorder. In the finite disorder case, the method allows one to find with good approximation the critical coupling distribution and the critical exponents.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Rigorous investigation of the reduced density matrix for the ideal Bose gas in harmonic traps by a loop-gas-like approach

In this paper, we rigorously investigate the reduced density matrix (RDM) associated to the ideal Bose gas in harmonic traps. We present a method based on a sum-decomposition of the RDM allowing to treat not only the isotropic trap, but also general anisotropic traps. When focusing on the isotropic trap, the method is analogous to the loop-gas approach developed by Mullin [“The loop-gas approach to Bose-Einstein condensation for trapped particles,” Am. J. Phys. 68(2), 120 (2000)]. Turning to the case of anisotropic traps, we examine the RDM for some anisotropic trap models corresponding to some quasi-1D and quasi-2D regimes. For such models, we bring out an additional contribution in the local density of particles which arises from the mesoscopic loops. The close connection with the occurrence of generalized-Bose-Einstein condensation is discussed. Our loop-gas-like approach provides relevant information which can help guide numerical investigations on highly anisotropic systems based on the Path Integral Monte Carlo method.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1973

On Digital Simulation of Multicorrelated Random Processes and Its Applications

Two methods are described to simulate, on a digital computer, a set of correlated, stationary, and Gaussian time series with zero mean from the given matrix of power spectral densities and cross spectral densities. The first method is based upon trigonometric series with random amplitudes and deterministic phase angles. The random amplitudes are generated by using a standard random number generator subroutine. An example is given which corresponds to three components of wind velocities at two different spatial locations for a total of six correlated time series. In the second method, the whole process is carried out using the Fast Fourier Transform approach. This method gives more accurate results and works about twenty times faster for a set of six correlated time series.

Sinha, A. K.↗
DOE OSTI2014

Energy density matrix formalism for interacting quantum systems: a quantum Monte Carlo study

We develop an energy density matrix that parallels the one-body reduced density matrix (1RDM) for many-body quantum systems. Just as the density matrix gives access to the number density and occupation numbers, the energy density matrix yields the energy density and orbital occupation energies. The eigenvectors of the matrix provide a natural orbital partitioning of the energy density while the eigenvalues comprise a single particle energy spectrum obeying a total energy sum rule. For mean-field systems the energy density matrix recovers the exact spectrum. When correlation becomes important, the occupation energies resemble quasiparticle energies in some respects. We explore the occupation energy spectrum for the finite 3D homogeneous electron gas in the metallic regime and an isolated oxygen atom with ground state quantum Monte Carlo techniques imple- mented in the QMCPACK simulation code. The occupation energy spectrum for the homogeneous electron gas can be described by an effective mass below the Fermi level. Above the Fermi level evanescent behavior in the occupation energies is observed in similar fashion to the occupation numbers of the 1RDM. A direct comparison with total energy differences demonstrates a quantita- tive connection between the occupation energies and electron addition and removal energies for the electron gas. For the oxygen atom, the association between the ground state occupation energies and particle addition and removal energies becomes only qualitative. The energy density matrix provides a new avenue for describing energetics with quantum Monte Carlo methods which have traditionally been limited to total energies.

density matrix↗
DOE OSTI2024

Site Suitability and Air Pollution Impacts of Composting Infrastructure for California’s Organic Waste Diversion Law

The emerging field of polaritonic chemistry explores the behavior of molecules under strong coupling with cavity modes. Despite recent developments in ab initio polaritonic methods for simulating polaritonic chemistry under electronic strong coupling, their capabilities are limited, especially in cases where the molecule also features strong electronic correlation. To bridge this gap, we have developed a novel method for cavity QED calculations utilizing the Density Matrix Renormalization Group (DMRG) algorithm in conjunction with the Pauli–Fierz Hamiltonian. Our approach is applied to investigate the effect of the cavity on the S0–S1 transition of n-oligoacenes, with n ranging from 2 to 5, encompassing 22 fully correlated π orbitals in the largest pentacene molecule. Our findings indicate that the influence of the cavity intensifies with larger acenes. Additionally, we demonstrate that, unlike the full determinantal representation, DMRG efficiently optimizes and eliminates excess photonic degrees of freedom, resulting in an asymptotically constant computational cost as the photonic basis increases.

54 ENVIRONMENTAL SCIENCES↗