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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 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Variational quantum state eigensolver

Extracting eigenvalues and eigenvectors of exponentially large matrices will be an important application of near-term quantum computers. The variational quantum eigensolver (VQE) treats the case when the matrix is a Hamiltonian. Here, we address the case when the matrix is a density matrix ρ. We introduce the variational quantum state eigensolver (VQSE), which is analogous to VQE in that it variationally learns the largest eigenvalues of ρ as well as a gate sequence V that prepares the corresponding eigenvectors. VQSE exploits the connection between diagonalization and majorization to define a cost function C=Tr(ρ~H) where H is a non-degenerate Hamiltonian. Due to Schur-concavity, C is minimized when ρ~=VρV† is diagonal in the eigenbasis of H. VQSE only requires a single copy of ρ (only n qubits) per iteration of the VQSE algorithm, making it amenable for near-term implementation. We heuristically demonstrate two applications of VQSE: (1) Principal component analysis, and (2) Error mitigation.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2016

Quantum decoherence during inflation from gravitational nonlinearities

We study the inflationary quantum-to-classical transition for the adiabatic curvature perturbation ζ due to quantum decoherence, focusing on the role played by squeezed-limit mode couplings. We evolve the quantum state Ψ in the Schrödinger picture, for a generic cubic coupling to additional environment degrees of freedom. Focusing on the case of minimal gravitational interactions, we find the evolution of the reduced density matrix for a given long-wavelength fluctuation by tracing out the other (mostly shorter-wavelength) modes of ζ as an environment. We show that inflation produces phase oscillations in the wave functional Ψ[ζ(x)], which suppress off-diagonal components of the reduced density matrix, leaving a diagonal mixture of different classical configurations. Gravitational nonlinearities thus provide a minimal mechanism for generating classical stochastic perturbations from inflation. We identify the time when decoherence occurs, which is delayed after horizon crossing due to the weak coupling, and find that Hubble-scale modes act as the decohering environment. We also comment on the observational relevance of decoherence and its relation to the squeezing of the quantum state.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Application of the theory of open quantum systems to nuclear physics problems

Quantum diffusion equations with transport coefficients explicitly depending on time are derived from the generalized non-Markovian Langevin equations. The asymptotic behavior of the friction and diffusion coefficients is investigated in the case of the FC and RWA couplings between the collective and internal subsystems. An asymptotic expression is obtained for the propagator of the density matrix of the open quantum system with the general quadratic Hamiltonian, linearly coupled (in coordinate and momentum) to internal degrees of freedom. The effect of different sets of transport coefficients on the decoherence and decay rate of the metastable state is investigated using the master equation for the reduced density matrix of open quantum systems. The developed approach is used to study the capture of the projectile nucleus by the target nucleus at energies near the Coulomb barrier. Capture cross sections in asymmetric reactions are well described with allowance for the calculated capture probabilities. Particular cases where dissipation favors penetration through the potential barrier are found. The generalized Kramers formula for the quasi-stationary decay rate of the quantum metastable systems is analytically derived.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2016

A well-scaling natural orbital theory

Here, we introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled approximations to the two-particle density matrix that yield algebraic scaling in general, and Hartree–Fock scaling in its seniority-zero version. Results from the latter version for small molecular systems are compared with those of highly accurate quantum-chemical computations. The energies lie above full configuration interaction calculations, close to doubly occupied configuration interaction calculations. Their accuracy is considerably greater than that obtained from current density-functional theory approximations and from current functionals of the oneparticle density matrix.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2017

Study of decoherence in a system of superconducting flux-qubits interacting with an ensemble of electrons

The degree of coherence in a hybrid system composed of superconducting flux-qubits and an electron ensemble is analysed. Both, the interactions among the electrons and among the superconducting flux-qubits are taken into account. The time evolution of the hybrid system is solved exactly, and discussed in terms of the reduced density matrix of each subsystem. It is seen that the inclusion of a line width, for the electrons and for the superconducting flux-qubits, influences the pattern of spin-squeezing and the coherence of the superconducting flux qubits. - Highlights: • The degree of coherence in a hybrid system, composed of superconducting flux qubits and an electron ensemble, is analysed. • The time evolution of the hybrid system is solved exactly and discussed in terms of the reduced density matrix of each subsystem. • It is shown that the initial state of the system evolves to a stationary squeezed state.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Photoconductivities from band states and a dissipative electron dynamics: Si(111) without and with adsorbed Ag clusters

A new general computational procedure is presented to obtain photoconductivities starting from atomic structures, combining ab initio electronic energy band states with populations from density matrix theory, and implemented for a specific set of materials based on Si crystalline slabs and their nanostructured surfaces without and with adsorbed Ag clusters. The procedure accounts for charge mobility in semiconductors in photoexcited states, and specifically electron and hole photomobilities at Si(111) surfaces with and without adsorbed Ag clusters using ab initio energy bands and orbitals generated from a generalized gradient functional, however with excited energy levels modified to provide correct bandgaps. Photoexcited state populations for each band and carrier type were generated using steady state solution of a reduced density matrix which includes dissipative medium effects. The present calculations provide photoexcited electronic populations and photoinduced mobilities resulting from applied electric fields and obtained from the change of driven electron energies with their electronic momentum. Extensive results for Si slabs with 8 layers, without and with adsorbed Ag clusters, show that the metal adsorbates lead to substantial increases in the photomobility and photoconductivity of electrons and holes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1999

What is the Best Alternative to Diagonalization of the Hamiltonian in Large Scale Semiempirical Calculations?

Recently, several linear scaling approaches have been introduced which replace the time dominating diagonalization step in semiempirical methods, enabling practical calculations to be performed, on very large molecules. This paper compares the accuracy and performance of pseudodiagonalization (PD), conjugate gradient density matrix search (CG-DMS), the Chebyshev polynomial expansion method (CEM), and purification of the density matrix (PDM) as linear scaling substitutions for diagonalization. The scaling, speed, and reliability of these methods are compared for AMI single point energy calculations on polyglycine chains (up to 20,000 atoms), water clusters (up to 12,300 atoms), and nucleic acids (up to 6300 atoms).

Daniels, Andrew D.↗
DOE OSTI2019

Carotenoid Nuclear Reorganization and Interplay of Bright and Dark Excited States

We report here quantum chemical calculations using multireference perturbation theory (MRPT) with the density matrix renormalization group (DMRG) plus photothermal deflection spectroscopy measurements to investigate the manifold of carotenoid excited states and establish their energies relative to the bright state (S 2 ) as a function of nuclear reorganization. We conclude that the primary photophysics and function of carotenoids are determined by interplay of only the bright (S 2 ) and lowest-energy dark (S 1 ) states. The lowest-lying dark state, far from being energetically distinguishable from the lowest-lying bright state along the entire excited-state nuclear reorganization pathway, is instead computed to be either the second or first excited state depending on what equilibrium geometry is considered. This finding suggests that, rather than there being a dark intermediate excited state bridging a non-negligible energy gap from the lowest-lying dark state to the lowest-lying bright state, there is in fact no appreciable energy gap to bridge following photoexcitation. Instead, excited-state nuclear reorganization constitutes the bridge from S 2 to S 1 , in the sense that these two states attain energetic degeneracy along this pathway.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
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 OSTI2016

Generalization of the Kohn-Sham system that can represent arbitrary one-electron density matrices

Density functional theory is currently the most widely applied method in electronic structure theory. The Kohn-Sham method, based on a fictitious system of noninteracting particles, is the workhorse of the theory. The particular form of the Kohn-Sham wave function admits only idempotent one-electron density matrices whereas wave functions of correlated electrons in post-Hartree-Fock methods invariably have fractional occupation numbers. Here we show that by generalizing the orbital concept and introducing a suitable dot product as well as a probability density, a noninteracting system can be chosen that can represent the one-electron density matrix of any system, even one with fractional occupation numbers. This fictitious system ensures that the exact electron density is accessible within density functional theory. It can also serve as the basis for reduced density matrix functional theory. Moreover, to aid the analysis of the results the orbitals may be assigned energies from a mean-field Hamiltonian. This produces energy levels that are akin to Hartree-Fock orbital energies such that conventional analyses based on Koopmans' theorem are available. Lastly, this system is convenient in formalisms that depend on creation and annihilation operators as they are trivially applied to single-determinant wave functions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2019

The HANDE-QMC Project: Open-Source Stochastic Quantum Chemistry from the Ground State Up

Building on the success of Quantum Monte Carlo techniques such as diffusion Monte Carlo, alternative stochastic approaches to solve electronic structure problems have emerged over the past decade. The full configuration interaction quantum Monte Carlo (FCIQMC) method allows one to systematically approach the exact solution of such problems, for cases where very high accuracy is desired. The introduction of FCIQMC has subsequently led to the development of coupled cluster Monte Carlo (CCMC) and density matrix quantum Monte Carlo (DMQMC), allowing stochastic sampling of the coupled cluster wave function and the exact thermal density matrix, respectively. In this Article, we describe the HANDE-QMC code, an open-source implementation of FCIQMC, CCMC and DMQMC, including initiator and semistochastic adaptations. We describe our code and demonstrate its use on three example systems; a molecule (nitric oxide), a model solid (the uniform electron gas), and a real solid (diamond). An illustrative tutorial is also included.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

On regularizing the MCTDH equations of motion

The Multiconfiguration Time-Dependent Hartree (MCTDH) approach leads to equations of motion (EOM) which become singular when there are unoccupied so-called single-particle functions (SPFs). Starting from a Hartree product, all SPFs, except the first one, are unoccupied initially. To solve the MCTDH-EOMs numerically, one therefore has to remove the singularity by a regularization procedure. Usually the inverse of a density matrix is regularized. Here we argue and show that regularizing the coefficient tensor, which in turn regularizes the density matrix as well, leads to an improved performance of the EOMs. The initially unoccupied SPFs are rotated faster into their “correct direction” in Hilbert space and the final results are less sensitive to the choice of the value of the regularization parameter. For a particular example (a spin-boson system studied with a transformed Hamiltonian), we could even show that only with the new regularization scheme could one obtain correct results. Lastly, in Appendix A, a new integration scheme for the MCTDH-EOMs developed by Lubich and co-workers is discussed. It is argued that this scheme does not solve the problem of the unoccupied natural orbitals because this scheme ignores the latter and does not propagate them at all.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2003

Intersubband Transitions in InAs/AlSb Quantum Wells

We have studied intersubband transitions in InAs/AlSb quantum wells experimentally and theoretically. Experimentally, we performed polarization-resolved infrared absorption spectroscopy to measure intersubband absorption peak frequencies and linewidths as functions of temperature (from 4 K to room temperature) and quantum well width (from a few nm to 10 nm). To understand experimental results, we performed a self-consistent 8-band k-p band-structure calculation including spatial charge separation. Based on the calculated band structure, we developed a set of density matrix equations to compute TE and TM optical transitions self-consistently, including both interband and intersubband channels. This density matrix formalism is also ideal for the inclusion of various many-body effects, which are known to be important for intersubband transitions. Detailed comparison between experimental data and theoretical simulations is presented.

Li, J.↗
DOE OSTI2021

Quantum information approach to high energy interactions

High energy hadron interactions are commonly described by using a probabilistic parton model that ignores quantum entanglement present in the light-cone wave functions. Here, we argue that since a high energy interaction samples an instant snapshot of the hadron wave function, the phases of different Fock state wave functions cannot be measured—therefore the light-cone density matrix has to be traced over these unobservable phases. Performing this trace with the corresponding U(1) Haar integration measure leads to ‘Haar scrambling’ of the density matrix, and to the emergence of entanglement entropy. This entanglement entropy is determined by the Fock state probability distribution, and is thus directly related to the parton structure functions. As proposed earlier, at large rapidity η the hadron state becomes maximally entangled, and the entanglement entropy is S E ~η according to QCD evolution equations. When the phases of Fock state components are controlled, for example in spin asymmetry measurements, the Haar average cannot be performed, and the probabilistic parton description breaks down.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1973

Quantum theory of an optical maser. VI - Transient behavior.

The transient behavior of a laser is discussed using the quantum theory as did Scully and Lamb. The formal solution of the density-matrix equation is expressed in terms of exponentially decaying eigenmodes. Some of the lower decay constants are obtained numerically. The equations for the moments of the density matrix are then derived and solved by a truncation method. The equations of motion are integrated numerically for the case where the average number of photons in a laser cavity has the realistically large value 1.3 x 100,000. An alternative Fokker-Planck-equation approach is discussed.

Wang, Y. K.↗
DOE OSTI2024

GPU-Accelerated Solution of the Bethe–Salpeter Equation for Large and Heterogeneous Systems

We present a massively parallel GPU-accelerated implementation of the Bethe–Salpeter equation (BSE) for the calculation of the vertical excitation energies (VEEs) and optical absorption spectra of condensed and molecular systems, starting from single-particle eigenvalues and eigenvectors obtained with density functional theory. The algorithms adopted here circumvent the slowly converging sums over empty and occupied states and the inversion of large dielectric matrices through a density matrix perturbation theory approach and a low-rank decomposition of the screened Coulomb interaction, respectively. Further computational savings are achieved by exploiting the nearsightedness of the density matrix of semiconductors and insulators to reduce the number of screened Coulomb integrals. We scale our calculations to thousands of GPUs with a hierarchical loop and data distribution strategy. The efficacy of our method is demonstrated by computing the VEEs of several spin defects in wide-band-gap materials, showing that supercells with up to 1000 atoms are necessary to obtain converged results. We discuss the validity of the common approximation that solves the BSE with truncated sums over empty and occupied states. In conclusion, we then apply our GW-BSE implementation to a diamond lattice with 1727 atoms to study the symmetry breaking of triplet states caused by the interaction of a point defect with an extended line defect.

Absorption spectra↗
DOE OSTI2019

Reconstructing Entanglement Hamiltonian via Entanglement Eigenstates

Entanglement Hamiltonian holds crucial clues in understanding quantum entanglement and its underlying phenomenon in strongly correlated systems. To date, however, a generic recipe to map out the operator form of entanglement Hamiltonian remains outstanding. In this work, we present a systematic framework which explicitly reconstructs entanglement Hamiltonian based on the information of one entangled mode of the reduced density matrix. Additionally, we demonstrate its successful application to quantum spin lattice models. The obtained entanglement Hamiltonians accurately recover the expectations from analytical theories and faithfully capture all features of the reduced density matrices, which are evidenced by the agreement between the original and reconstructed full entanglement spectra and the high density matrix fidelity.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Incorporating Brueckner-Hartree-Fock correlations in energy density functionals

Recently, a microscopically motivated nuclear energy density functional was derived by applying the density-matrix expansion to the Hartree-Fock (HF) energy obtained from long-range chiral effective-field theory two- and three-nucleon interactions. However, the HF approach cannot account for all many-body correlations. One class of correlations is included by Brueckner-Hartree-Fock (BHF) theory, which gives an improved definition of the one-body HF potential by replacing the interaction by a reaction matrix G. In this paper, we find that the difference between the G matrix and the similarity renormalization group evolved nucleon-nucleon potential V SRG can be well accounted for by a truncated series of contact terms. This is consistent with renormalization-group decoupling generating a series of counterterms as short-distance physics is integrated out. Here, the coefficients C n of the power series expansion Σ C n q n for the counterterms are examined for two potentials at different renormalization-group resolutions and at a range of densities. The success of this expansion for G–V SRG means we can apply the density-matrix expansion at the HF level with low-momentum interactions and density-dependent zero-range interactions to model BHF correlations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗