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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 1,729 records · Page 96
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Anomalous confined electron states in graphene superlattices

We show that periodic scalar potentials can induce the localization of some electronic states in graphene. Particularly, localized states are found at energies outside the potential variation range and embedded in the continuum spectrum of delocalized ones. The picture of the connection of wave functions with typical symmetries defined in relevant-edge nanoribbons is employed to explain the formation of the electronic structure and to characterize/classify eigen-states in graphene superlattices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Stochastic many-body perturbation theory for anharmonic molecular vibrations

A new quantum Monte Carlo (QMC) method for anharmonic vibrational zero-point energies and transition frequencies is developed, which combines the diagrammatic vibrational many-body perturbation theory based on the Dyson equation with Monte Carlo integration. The infinite sums of the diagrammatic and thus size-consistent first- and second-order anharmonic corrections to the energy and self-energy are expressed as sums of a few m- or 2m-dimensional integrals of wave functions and a potential energy surface (PES) (m is the vibrational degrees of freedom). Each of these integrals is computed as the integrand (including the value of the PES) divided by the value of a judiciously chosen weight function evaluated on demand at geometries distributed randomly but according to the weight function via the Metropolis algorithm. In this way, the method completely avoids cumbersome evaluation and storage of high-order force constants necessary in the original formulation of the vibrational perturbation theory; it furthermore allows even higher-order force constants essentially up to an infinite order to be taken into account in a scalable, memory-efficient algorithm. The diagrammatic contributions to the frequency-dependent self-energies that are stochastically evaluated at discrete frequencies can be reliably interpolated, allowing the self-consistent solutions to the Dyson equation to be obtained. This method, therefore, can compute directly and stochastically the transition frequencies of fundamentals and overtones as well as their relative intensities as pole strengths, without fixed-node errors that plague some QMC. It is shown that, for an identical PES, the new method reproduces the correct deterministic values of the energies and frequencies within a few cm{sup −1} and pole strengths within a few thousandths. With the values of a PES evaluated on the fly at random geometries, the new method captures a noticeably greater proportion of anharmonic effects.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Electronic and intraband optical properties of single quantum rings under intense laser field radiation

The influence of an intense laser field on one-electron states and intraband optical absorption coefficients is investigated in two-dimensional GaAs/Ga{sub 0.7}Al{sub 0.3}As quantum rings. An analytical expression of the effective lateral confining potential induced by the laser field is obtained. The one-electron energy spectrum and wave functions are found using the effective mass approximation and exact diagonalization technique. We have shown that changes in the incident light polarization lead to blue- or redshifts in the intraband optical absorption spectrum. Moreover, we found that only blueshift is obtained with increasing outer radius of the quantum ring.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Bound state solution of Dirac equation for 3D harmonics oscillator plus trigonometric scarf noncentral potential using SUSY QM approach

Dirac equation of 3D harmonics oscillator plus trigonometric Scarf non-central potential for spin symmetric case is solved using supersymmetric quantum mechanics approach. The Dirac equation for exact spin symmetry reduces to Schrodinger like equation. The relativistic energy and wave function for spin symmetric case are simply obtained using SUSY quantum mechanics method and idea of shape invariance.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Extended space expectation values in quantum dynamical system evolutions

The time variant power series expansion for the expectation value of a given quantum dynamical operator is well-known and well-investigated issue in quantum dynamics. However, depending on the operator and Hamiltonian singularities this expansion either may not exist or may not converge for all time instances except the beginning of the evolution. This work focuses on this issue and seeks certain cures for the negativities. We work in the extended space obtained by adding all images of the initial wave function under the system Hamiltonian’s positive integer powers. This requires the introduction of certain appropriately defined weight operators. The resulting better convergence in the temporal power series urges us to call the new defined entities “extended space expectation values” even though they are constructed over certain weight operators and are somehow pseudo expectation values.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Ab initio molecular dynamics with noisy forces: Validating the quantum Monte Carlo approach with benchmark calculations of molecular vibrational properties

We present a systematic study of a recently developed ab initio simulation scheme based on molecular dynamics and quantum Monte Carlo. In this approach, a damped Langevin molecular dynamics is employed by using a statistical evaluation of the forces acting on each atom by means of quantum Monte Carlo. This allows the use of an highly correlated wave function parametrized by several variational parameters and describing quite accurately the Born-Oppenheimer energy surface, as long as these parameters are determined at the minimum energy condition. However, in a statistical method both the minimization method and the evaluation of the atomic forces are affected by the statistical noise. In this work, we study systematically the accuracy and reliability of this scheme by targeting the vibrational frequencies of simple molecules such as the water monomer, hydrogen sulfide, sulfur dioxide, ammonia, and phosphine. We show that all sources of systematic errors can be controlled and reliable frequencies can be obtained with a reasonable computational effort. This work provides convincing evidence that this molecular dynamics scheme can be safely applied also to realistic systems containing several atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Vibrational frequency scaling factors for correlation consistent basis sets and the methods CC2 and MP2 and their spin-scaled SCS and SOS variants

We present scaling factors for vibrational frequencies calculated within the harmonic approximation and the correlated wave-function methods coupled cluster singles and doubles model (CC2) and Møller-Plesset perturbation theory (MP2) with and without a spin-component scaling (SCS or spin-opposite scaling (SOS)). Frequency scaling factors and the remaining deviations from the reference data are evaluated for several non-augmented basis sets of the cc-pVXZ family of generally contracted correlation-consistent basis sets as well as for the segmented contracted TZVPP basis. We find that the SCS and SOS variants of CC2 and MP2 lead to a slightly better accuracy for the scaled vibrational frequencies. The determined frequency scaling factors can also be used for vibrational frequencies calculated for excited states through response theory with CC2 and the algebraic diagrammatic construction through second order and their spin-component scaled variants.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Theoretical investigation of the relaxation of the bending mode of CH{sub 2}(X{sup ~}) by collisions with helium

We have earlier determined the dependence on the bending angle of the interaction of the methylene radical (CH{sub 2}) in its X{sup ~3}B{sub 1} state with He [L. Ma, P. J. Dagdigian, and M. H. Alexander, J. Chem. Phys. 136, 224306 (2012)]. By integration over products of the bending vibrational wave function, in a quantum close-coupled treatment we have calculated cross sections for the ro-vibrational relaxation of CH{sub 2}(X{sup ~}). Specifically, we find that cross sections for a loss of one vibrational quantum (v{sub b} = 2 → 1 and 1 → 0) are roughly two orders of magnitude smaller, and those for a loss of two vibrational quanta (v{sub b} = 2 → 0) four orders of magnitude smaller, than those for pure rotational relaxation. In addition, no clear cut dependence on the energy gap is seen.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Oscillation of electron mobility in parabolic double quantum well structure due to applied electric field

We show that oscillation of low temperature electron mobility μ can be obtained by applying an electric field F along the growth direction of the asymmetrically barrier delta doped Al{sub x}Ga{sub 1-x}As parabolic double quantum well structure. The drastic changes in the subband Fermi energies and distributions of subband wave functions as a function of F yield nonmonotonic intra- and intersubband scattering rate matrix elements mediated by intersubband effects. The oscillatory enhancement of μ, which is attributed to the subband mobilities governed by the ionized impurity scattering, magnifies with increase in well width and decrease in height of the parabolic structure potential. The results can be utilized for nanoscale low temperature device applications.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Time-dependent quantum chemistry of laser driven many-electron molecules

A Time-Dependent Configuration Interaction approach using multiple Feshbach partitionings, corresponding to multiple ionization stages of a laser-driven molecule, has recently been proposed [T.-T. Nguyen-Dang and J. Viau-Trudel, J. Chem. Phys. 139, 244102 (2013)]. To complete this development toward a fully ab-initio method for the calculation of time-dependent electronic wavefunctions of an N-electron molecule, we describe how tools of multiconfiguration quantum chemistry such as the management of the configuration expansion space using Graphical Unitary Group Approach concepts can be profitably adapted to the new context, that of time-resolved electronic dynamics, as opposed to stationary electronic structure. The method is applied to calculate the detailed, sub-cycle electronic dynamics of BeH{sub 2}, treated in a 3–21G bound-orbital basis augmented by a set of orthogonalized plane-waves representing continuum-type orbitals, including its ionization under an intense λ = 800 nm or λ = 80 nm continuous-wave laser field. The dynamics is strongly non-linear at the field-intensity considered (I ≃ 10{sup 15} W/cm{sup 2}), featuring important ionization of an inner-shell electron and strong post-ionization bound-electron dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2014

Seniority-based coupled cluster theory

Doubly occupied configuration interaction (DOCI) with optimized orbitals often accurately describes strong correlations while working in a Hilbert space much smaller than that needed for full configuration interaction. However, the scaling of such calculations remains combinatorial with system size. Pair coupled cluster doubles (pCCD) is very successful in reproducing DOCI energetically, but can do so with low polynomial scaling (N{sup 3}, disregarding the two-electron integral transformation from atomic to molecular orbitals). We show here several examples illustrating the success of pCCD in reproducing both the DOCI energy and wave function and show how this success frequently comes about. What DOCI and pCCD lack are an effective treatment of dynamic correlations, which we here add by including higher-seniority cluster amplitudes which are excluded from pCCD. This frozen pair coupled cluster approach is comparable in cost to traditional closed-shell coupled cluster methods with results that are competitive for weakly correlated systems and often superior for the description of strongly correlated systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Sub-band transport mechanism and switching properties for resistive switching nonvolatile memories with structure of silver/aluminum oxide/p-type silicon

In this paper, we discuss a model of sub-band in resistive switching nonvolatile memories with a structure of silver/aluminum oxide/p-type silicon (Ag/Al{sub x}O{sub y}/p-Si), in which the sub-band is formed by overlapping of wave functions of electron-occupied oxygen vacancies in Al{sub x}O{sub y} layer deposited by atomic layer deposition technology. The switching processes exhibit the characteristics of the bipolarity, discreteness, and no need of forming process, all of which are discussed deeply based on the model of sub-band. The relationships between the SET voltages and distribution of trap levels are analyzed qualitatively. The semiconductor-like behaviors of ON-state resistance affirm the sub-band transport mechanism instead of the metal filament mechanism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Free-complement local-Schrödinger-equation method for solving the Schrödinger equation of atoms and molecules: Basic theories and features

The free-complement (FC) method is a general method for solving the Schrödinger equation (SE): The produced wave function has the potentially exact structure as the solution of the Schrödinger equation. The variables included are determined either by using the variational principle (FC-VP) or by imposing the local Schrödinger equations (FC-LSE) at the chosen set of the sampling points. The latter method, referred to as the local Schrödinger equation (LSE) method, is integral-free and therefore applicable to any atom and molecule. The purpose of this paper is to formulate the basic theories of the LSE method and explain their basic features. First, we formulate three variants of the LSE method, the AB, HS, and H{sup T}Q methods, and explain their properties. Then, the natures of the LSE methods are clarified in some detail using the simple examples of the hydrogen atom and the Hooke’s atom. Finally, the ideas obtained in this study are applied to solving the SE of the helium atom highly accurately with the FC-LSE method. The results are very encouraging: we could get the world’s most accurate energy of the helium atom within the sampling-type methodologies, which is comparable to those obtained with the FC-VP method. Thus, the FC-LSE method is an easy and yet a powerful integral-free method for solving the Schrödinger equation of general atoms and molecules.

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

5D quantum dynamics of the H{sub 2}@SWNT system: Quantitative study of the rotational-translational coupling

The dynamics of the dihydrogen molecule when confined in carbon nanotubes with different chiralities and diameters are studied by using a 5 dimensional model considering the most relevant degrees of freedom of the system. The nuclear eigenstates are calculated for an (8,0) and a (5,0) carbon nanotubes by the State-Average Multiconfigurational Time-dependent Hartree, and then studied using qualitative tools (mapping of the total wave functions onto given subspaces) and more rigorous analysis (different kinds of overlaps with reference functions). The qualitative analysis is seen to fail due to a strong coupling between the internal and translational degrees of freedom. Using more accurate tools allows us to gain a deeper insight into the behaviour of confined species.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Time-dependent projected Hartree-Fock

Projected Hartree-Fock (PHF) has recently emerged as an alternative approach to describing degenerate systems where static correlation is abundant, when the spin-symmetry is projected. Here, we derive a set of linearized time-dependent equations for PHF in order to be able to access excited states. The close connection of such linear-response time-dependent PHF (TDPHF) to the stability condition of a PHF wave function is discussed. Expanding this analysis also makes it possible to give analytical expressions for the projected coupling terms of Hamiltonian and overlaps between excited Slater determinants. TDPHF with spin-projection (TDSUHF) and its Tamm-Dancoff approximation are benchmarked for several electronically degenerate molecules including the dissociating H{sub 2}, F{sub 2} and O{sub 3} at equilibrium, and the distorted ethylene. It is shown that they give consistently better descriptions of excited states than does time-dependent HF (TDHF). Furthermore, we demonstrate that they offer not only singly but also doubly excited states, which naturally arise upon spin-projection. We also address the thermodynamic limit of TDSUHF, using non-interacting He gas. While TDPHF singly excited states tend to converge to those of HF with the size of the system due to the lack of size-extensivity of PHF, doubly excited states remain reasonable even at the thermodynamic limit. We find that the overall performance of our method is systematically better than the regular TDHF in many cases at the same computational scaling.

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

The same number of optimized parameters scheme for determining intermolecular interaction energies

We introduce the Same Number Of Optimized Parameters (SNOOP) scheme as an alternative to the counterpoise method for treating basis set superposition errors in calculations of intermolecular interaction energies. The key point of the SNOOP scheme is to enforce that the number of optimized wave function parameters for the noninteracting system is the same as for the interacting system. This ensures a delicate balance between the quality of the monomer and dimer finite basis set calculations. We compare the SNOOP scheme to the uncorrected and counterpoise schemes theoretically as well as numerically. Numerical results for second-order Møller-Plesset perturbation theory (MP2) and coupled-cluster with single, double, and approximate triple excitations (CCSD(T)) show that the SNOOP scheme in general outperforms the uncorrected and counterpoise approaches. Moreover, we iterate that SNOOP interaction energies calculated using a given basis set are of similar quality as those determined by basis set extrapolation of counterpoise-corrected results obtained at a similar computational cost.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

Linear and nonlinear optical absorption coefficients and refractive index changes in GaN/Al{sub x}Ga{sub (1−x)}N double quantum wells operating at 1.55 μm

In the present paper, the linear and nonlinear optical absorption coefficients and refractive index changes between the ground and the first excited states in double GaN/Al{sub x}Ga{sub (1−x)}N quantum wells are studied theoretically. The electronic energy levels and their corresponding wave functions are obtained by solving Schrödinger-Poisson equations self-consistently within the effective mass approximation. The obtained results show that the optical absorption coefficients and refractive index changes can be red- and blue-shifted through varying the left quantum well width and the aluminum concentration x{sub b2} of the central barrier, respectively. These structural parameters are found to present optimum values for carrying out the transition of 0.8 eV (1.55 μm). Furthermore, we show that the desired transition can also be achieved by replacing the GaN in the left quantum well with Al{sub y}Ga{sub (1−y)}N and by varying the aluminum concentration y{sub Al}. The obtained results give a new degree of freedom in optoelectronic device applications such as optical fiber telecommunications operating at (1.55 μm)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Enhancement of electrical conductivity in CoO-SiO{sub 2} nanoglasses and large magnetodielectric effect in ZnO-nanoglass composites

Nanoglasses of compositions xCoO·(100-x)SiO{sub 2} (mol. %) with x having values 10, 15, and 20, respectively, were grown within the nanopores of a pellet comprising of ZnO nanoparticles by soaking the latter in a suitable sol followed by necessary heat treatment. Both Co{sup 2+} and Co{sup 3+} ions were present and confirmed by X-ray photoelectron spectroscopy, the fraction of Co{sup 2+} species being ∼ 0.70. Small polaron hopping conduction was found to be present in the nanoglasses. The activation energy in the latter was observed to be smaller (range of 0.32–0.44 eV) than that in the corresponding bulk glass (0.70–0.77 eV). This was caused by the higher free volume in the nanoglass as compared to that of the bulk glass. This was confirmed by the extracted values of intersite separation between cobalt ions, which were higher in the nanoglass. Weak ferromagnetism was exhibited by the nanocomposites. This was ascribed to super exchange interaction between spin moments associated with Co{sup 2+} and Co{sup 3+} ions, respectively, leading to an antiferromagnetic spin alignment. The nanocomposites showed magnetodielectric effect with the magnetodielectric parameter having values in the range of 5.5% to 10%. The experimental data were fitted to equations derived from Catalan's model by invoking a negative and a positive magnetoresistance for nanoglasses of compositions having x = 20 and x = 10, respectively. A weak spin-orbit coupling and wave function shrinkage in a magnetic field for strongly localized states, respectively, are believed to cause such behaviour in the nanoglass systems concerned. Direct magnetoresistance measurements were carried out on the nanocomposites containing nanoglasses having 10CoO and 20CoO, respectively. The trend of results obtained indeed confirmed the presence of positive and negative magnetoresistance in the two nanoglasses, respectively. The materials would be suitable for magnetic sensor applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗