Enhanced Constraints for Accurate Lower Bounds on Many-Electron Quantum Energies from Variational Two-Electron Reduced Density Matrix Theory

NASA Astrophysics Data System (ADS)

Mazziotti, David A.

2016-10-01

A central challenge of physics is the computation of strongly correlated quantum systems. The past ten years have witnessed the development and application of the variational calculation of the two-electron reduced density matrix (2-RDM) without the wave function. In this Letter we present an orders-of-magnitude improvement in the accuracy of 2-RDM calculations without an increase in their computational cost. The advance is based on a low-rank, dual formulation of an important constraint on the 2-RDM, the T 2 condition. Calculations are presented for metallic chains and a cadmium-selenide dimer. The low-scaling T 2 condition will have significant applications in atomic and molecular, condensed-matter, and nuclear physics.

Detection of density dependence requires density manipulations and calculation of lambda.

PubMed

Fowler, N L; Overath, R Deborah; Pease, Craig M

2006-03-01

To investigate density-dependent population regulation in the perennial bunchgrass Bouteloua rigidiseta, we experimentally manipulated density by removing adults or adding seeds to replicate quadrats in a natural population for three annual intervals. We monitored the adjacent control quadrats for 14 annual intervals. We constructed a population projection matrix for each quadrat in each interval, calculated lambda, and did a life table response experiment (LTRE) analysis. We tested the effects of density upon lambda by comparing experimental and control quadrats, and by an analysis of the 15-year observational data set. As measured by effects on lambda and on N(t+1/Nt in the experimental treatments, negative density dependence was strong: the population was being effectively regulated. The relative contributions of different matrix elements to treatment effect on lambda differed among years and treatments; overall the pattern was one of small contributions by many different life cycle stages. In contrast, density dependence could not be detected using only the observational (control quadrats) data, even though this data set covered a much longer time span. Nor did experimental effects on separate matrix elements reach statistical significance. These results suggest that ecologists may fail to detect density dependence when it is present if they have only descriptive, not experimental, data, do not have data for the entire life cycle, or analyze life cycle components separately.

Linear-scaling density-functional simulations of charged point defects in Al2O3 using hierarchical sparse matrix algebra.

PubMed

Hine, N D M; Haynes, P D; Mostofi, A A; Payne, M C

2010-09-21

We present calculations of formation energies of defects in an ionic solid (Al(2)O(3)) extrapolated to the dilute limit, corresponding to a simulation cell of infinite size. The large-scale calculations required for this extrapolation are enabled by developments in the approach to parallel sparse matrix algebra operations, which are central to linear-scaling density-functional theory calculations. The computational cost of manipulating sparse matrices, whose sizes are determined by the large number of basis functions present, is greatly improved with this new approach. We present details of the sparse algebra scheme implemented in the ONETEP code using hierarchical sparsity patterns, and demonstrate its use in calculations on a wide range of systems, involving thousands of atoms on hundreds to thousands of parallel processes.

Modified Hartree-Fock-Bogoliubov theory at finite temperature

NASA Astrophysics Data System (ADS)

Dinh Dang, Nguyen; Arima, Akito

2003-07-01

The modified Hartree-Fock-Bogoliubov (MHFB) theory at finite temperature is derived, which conserves the unitarity relation of the particle-density matrix. This is achieved by constructing a modified-quasiparticle-density matrix, where the fluctuation of the quasiparticle number is microscopically built in. This matrix can be directly obtained from the usual quasiparticle-density matrix by applying the secondary Bogoliubov transformation, which includes the quasiparticle-occupation number. It is shown that, in the limit of constant pairing parameter, the MHFB theory yields the previously obtained modified BCS (MBCS) equations. It is also proved that the modified quasiparticle-random-phase approximation, which is based on the MBCS quasiparticle excitations, conserves the Ikeda sum rule. The numerical calculations of the pairing gap, heat capacity, level density, and level-density parameter within the MBCS theory are carried out for 120Sn. The results show that the superfluid-normal phase transition is completely washed out. The applicability of the MBCS up to a temperature as high as T˜5 MeV is analyzed in detail.

Low-memory iterative density fitting.

PubMed

Grajciar, Lukáš

2015-07-30

A new low-memory modification of the density fitting approximation based on a combination of a continuous fast multipole method (CFMM) and a preconditioned conjugate gradient solver is presented. Iterative conjugate gradient solver uses preconditioners formed from blocks of the Coulomb metric matrix that decrease the number of iterations needed for convergence by up to one order of magnitude. The matrix-vector products needed within the iterative algorithm are calculated using CFMM, which evaluates them with the linear scaling memory requirements only. Compared with the standard density fitting implementation, up to 15-fold reduction of the memory requirements is achieved for the most efficient preconditioner at a cost of only 25% increase in computational time. The potential of the method is demonstrated by performing density functional theory calculations for zeolite fragment with 2592 atoms and 121,248 auxiliary basis functions on a single 12-core CPU workstation. © 2015 Wiley Periodicals, Inc.

Spectral function from Reduced Density Matrix Functional Theory

NASA Astrophysics Data System (ADS)

Romaniello, Pina; di Sabatino, Stefano; Berger, Jan A.; Reining, Lucia

2015-03-01

In this work we focus on the calculation of the spectral function, which determines, for example, photoemission spectra, from reduced density matrix functional theory. Starting from its definition in terms of the one-body Green's function we derive an expression for the spectral function that depends on the natural occupation numbers and on an effective energy which accounts for all the charged excitations. This effective energy depends on the two-body as well as higher-order density matrices. Various approximations to this expression are explored by using the exactly solvable Hubbard chains.

Computer simulation of the matrix-inclusion interphase in bulk metallic glass based nanocomposites

NASA Astrophysics Data System (ADS)

Kokotin, V.; Hermann, H.; Eckert, J.

2011-10-01

Atomistic models for matrix-inclusion systems are generated. Analyses of the systems show that interphase layers of finite thickness appear interlinking the surface of the nanocrystalline inclusion and the embedding amorphous matrix. In a first approximation, the interphase is characterized as an amorphous structure with a density slightly reduced compared to that of the matrix. This result holds for both monatomic hard sphere systems and a Cu47.5Zr47.5Al5 alloy simulated by molecular dynamics (MD). The elastic shear and bulk modulus of the interphase are calculated by simulated deformation of the MD systems. Both moduli diminish with decreasing density but the shear modulus is more sensitive against density reduction by one order of magnitude. This result explains recent observations of shear band initiation at the amorphous-crystalline interface during plastic deformation.

Multivariate Granger causality: an estimation framework based on factorization of the spectral density matrix

PubMed Central

Wen, Xiaotong; Rangarajan, Govindan; Ding, Mingzhou

2013-01-01

Granger causality is increasingly being applied to multi-electrode neurophysiological and functional imaging data to characterize directional interactions between neurons and brain regions. For a multivariate dataset, one might be interested in different subsets of the recorded neurons or brain regions. According to the current estimation framework, for each subset, one conducts a separate autoregressive model fitting process, introducing the potential for unwanted variability and uncertainty. In this paper, we propose a multivariate framework for estimating Granger causality. It is based on spectral density matrix factorization and offers the advantage that the estimation of such a matrix needs to be done only once for the entire multivariate dataset. For any subset of recorded data, Granger causality can be calculated through factorizing the appropriate submatrix of the overall spectral density matrix. PMID:23858479

Watching excitons move: the time-dependent transition density matrix

NASA Astrophysics Data System (ADS)

Ullrich, Carsten

2012-02-01

Time-dependent density-functional theory allows one to calculate excitation energies and the associated transition densities in principle exactly. The transition density matrix (TDM) provides additional information on electron-hole localization and coherence of specific excitations of the many-body system. We have extended the TDM concept into the real-time domain in order to visualize the excited-state dynamics in conjugated molecules. The time-dependent TDM is defined as an implicit density functional, and can be approximately obtained from the time-dependent Kohn-Sham orbitals. The quality of this approximation is assessed in simple model systems. A computational scheme for real molecular systems is presented: the time-dependent Kohn-Sham equations are solved with the OCTOPUS code and the time-dependent Kohn-Sham TDM is calculated using a spatial partitioning scheme. The method is applied to show in real time how locally created electron-hole pairs spread out over neighboring conjugated molecular chains. The coupling mechanism, electron-hole coherence, and the possibility of charge separation are discussed.

Variational Optimization of the Second-Order Density Matrix Corresponding to a Seniority-Zero Configuration Interaction Wave Function.

PubMed

Poelmans, Ward; Van Raemdonck, Mario; Verstichel, Brecht; De Baerdemacker, Stijn; Torre, Alicia; Lain, Luis; Massaccesi, Gustavo E; Alcoba, Diego R; Bultinck, Patrick; Van Neck, Dimitri

2015-09-08

We perform a direct variational determination of the second-order (two-particle) density matrix corresponding to a many-electron system, under a restricted set of the two-index N-representability P-, Q-, and G-conditions. In addition, we impose a set of necessary constraints that the two-particle density matrix must be derivable from a doubly occupied many-electron wave function, i.e., a singlet wave function for which the Slater determinant decomposition only contains determinants in which spatial orbitals are doubly occupied. We rederive the two-index N-representability conditions first found by Weinhold and Wilson and apply them to various benchmark systems (linear hydrogen chains, He, N2, and CN(-)). This work is motivated by the fact that a doubly occupied many-electron wave function captures in many cases the bulk of the static correlation. Compared to the general case, the structure of doubly occupied two-particle density matrices causes the associate semidefinite program to have a very favorable scaling as L(3), where L is the number of spatial orbitals. Since the doubly occupied Hilbert space depends on the choice of the orbitals, variational calculation steps of the two-particle density matrix are interspersed with orbital-optimization steps (based on Jacobi rotations in the space of the spatial orbitals). We also point to the importance of symmetry breaking of the orbitals when performing calculations in a doubly occupied framework.

Direct calculation of liquid-vapor phase equilibria from transition matrix Monte Carlo simulation

NASA Astrophysics Data System (ADS)

Errington, Jeffrey R.

2003-06-01

An approach for directly determining the liquid-vapor phase equilibrium of a model system at any temperature along the coexistence line is described. The method relies on transition matrix Monte Carlo ideas developed by Fitzgerald, Picard, and Silver [Europhys. Lett. 46, 282 (1999)]. During a Monte Carlo simulation attempted transitions between states along the Markov chain are monitored as opposed to tracking the number of times the chain visits a given state as is done in conventional simulations. Data collection is highly efficient and very precise results are obtained. The method is implemented in both the grand canonical and isothermal-isobaric ensemble. The main result from a simulation conducted at a given temperature is a density probability distribution for a range of densities that includes both liquid and vapor states. Vapor pressures and coexisting densities are calculated in a straightforward manner from the probability distribution. The approach is demonstrated with the Lennard-Jones fluid. Coexistence properties are directly calculated at temperatures spanning from the triple point to the critical point.

Density-matrix based determination of low-energy model Hamiltonians from ab initio wavefunctions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Changlani, Hitesh J.; Zheng, Huihuo; Wagner, Lucas K.

2015-09-14

We propose a way of obtaining effective low energy Hubbard-like model Hamiltonians from ab initio quantum Monte Carlo calculations for molecular and extended systems. The Hamiltonian parameters are fit to best match the ab initio two-body density matrices and energies of the ground and excited states, and thus we refer to the method as ab initio density matrix based downfolding. For benzene (a finite system), we find good agreement with experimentally available energy gaps without using any experimental inputs. For graphene, a two dimensional solid (extended system) with periodic boundary conditions, we find the effective on-site Hubbard U{sup ∗}/t tomore » be 1.3 ± 0.2, comparable to a recent estimate based on the constrained random phase approximation. For molecules, such parameterizations enable calculation of excited states that are usually not accessible within ground state approaches. For solids, the effective Hamiltonian enables large-scale calculations using techniques designed for lattice models.« less

Propagation of Circularly Polarized Light Through a Two-Dimensional Random Medium

NASA Astrophysics Data System (ADS)

Gorodnichev, E. E.

2017-12-01

The problem of small-angle multiple-scattering of circularly polarized light in a two-dimensional medium with large fiberlike inhomogeneities is studied. The attenuation lengths for elements the density matrix are calculated. It is found that with increasing the sample thickness the intensity of waves polarized along the fibers decays faster than the other density matrix elements. With further increase in the thickness, the off-diagonal element which is responsible for correlation between the cross-polarized waves dissapears. In the case of very thick samples the scattered field proves to be polarized perpendicular to the fibers. It is shown that the difference in the attenuation lengths of the density matrix elements results in a non-monotonic depth dependence of the degree of polarization.

Electron momentum densities in disordered muffin-tin alloys

NASA Astrophysics Data System (ADS)

Bansil, A.; Rao, R. S.; Mijnarends, P. E.; Schwartz, L.

1981-04-01

The application of average t-matrix (ATA) and coherent potential (CPA) approximations to the calculation of average electron momentum density ρ(p-->) in random muffin-tin alloys AxB1-x is considered. The necessary equations for the general matrix elements of the operators describing scattering by the CPA atom and also by an A or B atom embedded in the effective medium are derived. Various versions of the ATA for ρ(p-->) are discussed. Several ρ(p-->) curves calculated on the basis of the CPA and ATA in CuxNi1-x are presented. These results are used to delineate the effects on ρ(p-->) of self-consistency in the treatment of disorder.

Decay of correlations between cross-polarized electromagnetic waves in a two-dimensional random medium.

PubMed

Gorodnichev, E E

2018-04-01

The problem of multiple scattering of polarized light in a two-dimensional medium composed of fiberlike inhomogeneities is studied. The attenuation lengths for the density matrix elements are calculated. For a highly absorbing medium it is found that, as the sample thickness increases, the intensity of waves polarized along the fibers decays faster than the other density matrix elements. With further increase in the sample thickness, the off-diagonal elements which are responsible for correlations between the cross-polarized waves disappear. In the asymptotic limit of very thick samples the scattered light proves to be polarized perpendicular to the fibers. The difference in the attenuation lengths between the density matrix elements results in a nonmonotonic depth dependence of the degree of polarization. In the opposite case of a weakly absorbing medium, the off-diagonal element of the density matrix and, correspondingly, the correlations between the cross-polarized fields are shown to decay faster than the intensity of waves polarized along and perpendicular to the fibers.

Electronic Absorption Spectra of Neutral Perylene (C20H12), Terrylene (C30H16), and Quaterrylene (C40H20) and their Positive and Negative Ions: Ne Matrix-Isolation Spectroscopy and Time Dependent Density Functional Theory Calculations

NASA Technical Reports Server (NTRS)

Halasinski, Thomas M.; Weisman, Jennifer L.; Lee, Timothy J.; Salama, Farid; Head-Gordon, Martin; Kwak, Dochan (Technical Monitor)

2002-01-01

We present a full experimental and theoretical study of an interesting series of polycyclic aromatic hydrocarbons, the oligorylenes. The absorption spectra of perylene, terrylene and quaterrylene in neutral, cationic and anionic charge states are obtained by matrix-isolation spectroscopy in Ne. The experimental spectra are dominated by a bright state that red shifts with growing molecular size. Excitation energies and state symmetry assignments are supported by calculations using time dependent density functional theory methods. These calculations also provide new insight into the observed trends in oscillator strength and excitation energy for the bright states: the oscillator strength per unit mass of carbon increases along the series.

Minkowski Tensors in Two Dimensions: Probing the Morphology and Isotropy of the Matter and Galaxy Density Fields

NASA Astrophysics Data System (ADS)

Appleby, Stephen; Chingangbam, Pravabati; Park, Changbom; Hong, Sungwook E.; Kim, Juhan; Ganesan, Vidhya

2018-05-01

We apply the Minkowski tensor statistics to two-dimensional slices of the three-dimensional matter density field. The Minkowski tensors are a set of functions that are sensitive to directionally dependent signals in the data and, furthermore, can be used to quantify the mean shape of density fields. We begin by reviewing the definition of Minkowski tensors and introducing a method of calculating them from a discretely sampled field. Focusing on the statistic {W}21,1—a 2 × 2 matrix—we calculate its value for both the entire excursion set and individual connected regions and holes within the set. To study the morphology of structures within the excursion set, we calculate the eigenvalues λ 1, λ 2 for the matrix {W}21,1 of each distinct connected region and hole and measure their mean shape using the ratio β \\equiv < {λ }2/{λ }1> . We compare both {W}21,1 and β for a Gaussian field and a smoothed density field generated from the latest Horizon Run 4 cosmological simulation to study the effect of gravitational collapse on these functions. The global statistic {W}21,1 is essentially independent of gravitational collapse, as the process maintains statistical isotropy. However, β is modified significantly, with overdensities becoming relatively more circular compared to underdensities at low redshifts. When applying the statistics to a redshift-space distorted density field, the matrix {W}21,1 is no longer proportional to the identity matrix, and measurements of its diagonal elements can be used to probe the large-scale velocity field.

The Feynman-Vernon Influence Functional Approach in QED

NASA Astrophysics Data System (ADS)

Biryukov, Alexander; Shleenkov, Mark

2016-10-01

In the path integral approach we describe evolution of interacting electromagnetic and fermionic fields by the use of density matrix formalism. The equation for density matrix and transitions probability for fermionic field is obtained as average of electromagnetic field influence functional. We obtain a formula for electromagnetic field influence functional calculating for its various initial and final state. We derive electromagnetic field influence functional when its initial and final states are vacuum. We present Lagrangian for relativistic fermionic field under influence of electromagnetic field vacuum.

Density-matrix-based algorithm for solving eigenvalue problems

NASA Astrophysics Data System (ADS)

Polizzi, Eric

2009-03-01

A fast and stable numerical algorithm for solving the symmetric eigenvalue problem is presented. The technique deviates fundamentally from the traditional Krylov subspace iteration based techniques (Arnoldi and Lanczos algorithms) or other Davidson-Jacobi techniques and takes its inspiration from the contour integration and density-matrix representation in quantum mechanics. It will be shown that this algorithm—named FEAST—exhibits high efficiency, robustness, accuracy, and scalability on parallel architectures. Examples from electronic structure calculations of carbon nanotubes are presented, and numerical performances and capabilities are discussed.

Stockholder projector analysis: A Hilbert-space partitioning of the molecular one-electron density matrix with orthogonal projectors

NASA Astrophysics Data System (ADS)

Vanfleteren, Diederik; Van Neck, Dimitri; Bultinck, Patrick; Ayers, Paul W.; Waroquier, Michel

2012-01-01

A previously introduced partitioning of the molecular one-electron density matrix over atoms and bonds [D. Vanfleteren et al., J. Chem. Phys. 133, 231103 (2010)] is investigated in detail. Orthogonal projection operators are used to define atomic subspaces, as in Natural Population Analysis. The orthogonal projection operators are constructed with a recursive scheme. These operators are chemically relevant and obey a stockholder principle, familiar from the Hirshfeld-I partitioning of the electron density. The stockholder principle is extended to density matrices, where the orthogonal projectors are considered to be atomic fractions of the summed contributions. All calculations are performed as matrix manipulations in one-electron Hilbert space. Mathematical proofs and numerical evidence concerning this recursive scheme are provided in the present paper. The advantages associated with the use of these stockholder projection operators are examined with respect to covalent bond orders, bond polarization, and transferability.

Efficient parallel linear scaling construction of the density matrix for Born-Oppenheimer molecular dynamics.

PubMed

Mniszewski, S M; Cawkwell, M J; Wall, M E; Mohd-Yusof, J; Bock, N; Germann, T C; Niklasson, A M N

2015-10-13

We present an algorithm for the calculation of the density matrix that for insulators scales linearly with system size and parallelizes efficiently on multicore, shared memory platforms with small and controllable numerical errors. The algorithm is based on an implementation of the second-order spectral projection (SP2) algorithm [ Niklasson, A. M. N. Phys. Rev. B 2002 , 66 , 155115 ] in sparse matrix algebra with the ELLPACK-R data format. We illustrate the performance of the algorithm within self-consistent tight binding theory by total energy calculations of gas phase poly(ethylene) molecules and periodic liquid water systems containing up to 15,000 atoms on up to 16 CPU cores. We consider algorithm-specific performance aspects, such as local vs nonlocal memory access and the degree of matrix sparsity. Comparisons to sparse matrix algebra implementations using off-the-shelf libraries on multicore CPUs, graphics processing units (GPUs), and the Intel many integrated core (MIC) architecture are also presented. The accuracy and stability of the algorithm are illustrated with long duration Born-Oppenheimer molecular dynamics simulations of 1000 water molecules and a 303 atom Trp cage protein solvated by 2682 water molecules.

Linear-scaling method for calculating nuclear magnetic resonance chemical shifts using gauge-including atomic orbitals within Hartree-Fock and density-functional theory.

PubMed

Kussmann, Jörg; Ochsenfeld, Christian

2007-08-07

Details of a new density matrix-based formulation for calculating nuclear magnetic resonance chemical shifts at both Hartree-Fock and density functional theory levels are presented. For systems with a nonvanishing highest occupied molecular orbital-lowest unoccupied molecular orbital gap, the method allows us to reduce the asymptotic scaling order of the computational effort from cubic to linear, so that molecular systems with 1000 and more atoms can be tackled with today's computers. The key feature is a reformulation of the coupled-perturbed self-consistent field (CPSCF) theory in terms of the one-particle density matrix (D-CPSCF), which avoids entirely the use of canonical MOs. By means of a direct solution for the required perturbed density matrices and the adaptation of linear-scaling integral contraction schemes, the overall scaling of the computational effort is reduced to linear. A particular focus of our formulation is to ensure numerical stability when sparse-algebra routines are used to obtain an overall linear-scaling behavior.

Efficient Computation of Sparse Matrix Functions for Large-Scale Electronic Structure Calculations: The CheSS Library.

PubMed

Mohr, Stephan; Dawson, William; Wagner, Michael; Caliste, Damien; Nakajima, Takahito; Genovese, Luigi

2017-10-10

We present CheSS, the "Chebyshev Sparse Solvers" library, which has been designed to solve typical problems arising in large-scale electronic structure calculations using localized basis sets. The library is based on a flexible and efficient expansion in terms of Chebyshev polynomials and presently features the calculation of the density matrix, the calculation of matrix powers for arbitrary powers, and the extraction of eigenvalues in a selected interval. CheSS is able to exploit the sparsity of the matrices and scales linearly with respect to the number of nonzero entries, making it well-suited for large-scale calculations. The approach is particularly adapted for setups leading to small spectral widths of the involved matrices and outperforms alternative methods in this regime. By coupling CheSS to the DFT code BigDFT, we show that such a favorable setup is indeed possible in practice. In addition, the approach based on Chebyshev polynomials can be massively parallelized, and CheSS exhibits excellent scaling up to thousands of cores even for relatively small matrix sizes.

Micromechanics effects in creep of metal-matrix composites

NASA Astrophysics Data System (ADS)

Davis, L. C.; Allison, J. E.

1995-12-01

The creep of metal-matrix composites is analyzed by finite element techniques. An axisymmetric unit-cell model with spherical reinforcing particles is used. Parameters appropriate to TiC particles in a precipitation-hardened (2219) Al matrix are chosen. The effects of matrix plasticity and residual stresses on the creep of the composite are calculated. We confirm (1) that the steady-state rate is independent of the particle elastic moduli and the matrix elastic and plastic properties, (2) that the ratio of composite to matrix steady-state rates depends only on the volume fraction and geometry of the reinforcing phase, and (3) that this ratio can be determined from a calculation of the stress-strain relation for the geometrically identical composite (same phase volume and geometry) with rigid particles in the appropriate power-law hardening matrix. The values of steady-state creep are compared to experimental ones (Krajewski et al.). Continuum mechanics predictions give a larger reduction of the composite creep relative to the unreinforced material than measured, suggesting that the effective creep rate of the matrix is larger than in unreinforced precipitation-hardened Al due to changes in microstructure, dislocation density, or creep mechanism. Changes in matrix creep properties are also suggested by the comparison of calculated and measured creep strain rates in the primary creep regime, where significantly different time dependencies are found. It is found that creep calculations performed for a timeindependent matrix creep law can be transformed to obtain the creep for a time-dependent creep law.

Optoelectronics of inverted type-I CdS/CdSe core/crown quantum ring

NASA Astrophysics Data System (ADS)

Bose, Sumanta; Fan, Weijun; Zhang, Dao Hua

2017-10-01

Inverted type-I heterostructure core/crown quantum rings (QRs) are quantum-efficient luminophores, whose spectral characteristics are highly tunable. Here, we study the optoelectronic properties of type-I core/crown CdS/CdSe QRs in the zincblende phase—over contrasting lateral size and crown width. For this, we inspect their strain profiles, transition energies, transition matrix elements, spatial charge densities, electronic bandstructures, band-mixing probabilities, optical gain spectra, maximum optical gains, and differential optical gains. Our framework uses an effective-mass envelope function theory based on the 8-band k ṡ p method employing the valence force field model for calculating the atomic strain distributions. The gain calculations are based on the density-matrix equation and take into consideration the excitonic effects with intraband scattering. Variations in the QR lateral size and relative widths of core and crown (ergo the composition) affect their energy levels, band-mixing probabilities, optical transition matrix elements, emission wavelengths/intensities, etc. The optical gain of QRs is also strongly dimension and composition dependent with further dependency on the injection carrier density causing the band-filling effect. They also affect the maximum and differential gain at varying dimensions and compositions.

Alternative dimensional reduction via the density matrix

NASA Astrophysics Data System (ADS)

de Carvalho, C. A.; Cornwall, J. M.; da Silva, A. J.

2001-07-01

We give graphical rules, based on earlier work for the functional Schrödinger equation, for constructing the density matrix for scalar and gauge fields in equilibrium at finite temperature T. More useful is a dimensionally reduced effective action (DREA) constructed from the density matrix by further functional integration over the arguments of the density matrix coupled to a source. The DREA is an effective action in one less dimension which may be computed order by order in perturbation theory or by dressed-loop expansions; it encodes all thermal matrix elements. We term the DREA procedure alternative dimensional reduction, to distinguish it from the conventional dimensionally reduced field theory (DRFT) which applies at infinite T. The DREA is useful because it gives a dimensionally reduced theory usable at any T including infinity, where it yields the DRFT, and because it does not and cannot have certain spurious infinities which sometimes occur in the density matrix itself or the conventional DRFT; these come from ln T factors at infinite temperature. The DREA can be constructed to all orders (in principle) and the only regularizations needed are those which control the ultraviolet behavior of the zero-T theory. An example of spurious divergences in the DRFT occurs in d=2+1φ4 theory dimensionally reduced to d=2. We study this theory and show that the rules for the DREA replace these ``wrong'' divergences in physical parameters by calculable powers of ln T; we also compute the phase transition temperature of this φ4 theory in one-loop order. Our density-matrix construction is equivalent to a construction of the Landau-Ginzburg ``coarse-grained free energy'' from a microscopic Hamiltonian.

Continuum Level Density of a Coupled-Channel System in the Complex Scaling Method

NASA Astrophysics Data System (ADS)

Suzuki, R.; Kruppa, A. T.; Giraud, B. G.; Katō, K.

2008-06-01

We study the continuum level density (CLD) in the formalism of the complex scaling method (CSM) for coupled-channel systems. We apply the formalism to the ^{4}He = [^{3}H + p] + [^3{He} + n] coupled-channel cluster model where there are resonances at low energy. Numerical calculations of the CLD in the CSM with a finite number of L^{2} basis functions are consistent with the exact result calculated from the S-matrix by solving coupled-channel equations. We also study channel densities. In this framework, the extended completeness relation (ECR) plays an important role.

Forecasts of non-Gaussian parameter spaces using Box-Cox transformations

NASA Astrophysics Data System (ADS)

Joachimi, B.; Taylor, A. N.

2011-09-01

Forecasts of statistical constraints on model parameters using the Fisher matrix abound in many fields of astrophysics. The Fisher matrix formalism involves the assumption of Gaussianity in parameter space and hence fails to predict complex features of posterior probability distributions. Combining the standard Fisher matrix with Box-Cox transformations, we propose a novel method that accurately predicts arbitrary posterior shapes. The Box-Cox transformations are applied to parameter space to render it approximately multivariate Gaussian, performing the Fisher matrix calculation on the transformed parameters. We demonstrate that, after the Box-Cox parameters have been determined from an initial likelihood evaluation, the method correctly predicts changes in the posterior when varying various parameters of the experimental setup and the data analysis, with marginally higher computational cost than a standard Fisher matrix calculation. We apply the Box-Cox-Fisher formalism to forecast cosmological parameter constraints by future weak gravitational lensing surveys. The characteristic non-linear degeneracy between matter density parameter and normalization of matter density fluctuations is reproduced for several cases, and the capabilities of breaking this degeneracy by weak-lensing three-point statistics is investigated. Possible applications of Box-Cox transformations of posterior distributions are discussed, including the prospects for performing statistical data analysis steps in the transformed Gaussianized parameter space.

US Army Research Laboratory Power-Line UAV Modeling and Simulation (ARL-PLUMS Ver 2.x) Software Tool: User Manual and Technical Report

DTIC Science & Technology

2015-09-01

shown have units of pF/m. This is the capacitance matrix for the 115-kV 3-phase circuit seen in Fig. 24.....................................24 Fig. 29...The window that appears when one clicks “Calculate Lambdas ”. These are the linear charge densities for the 115-kV 3-phase circuit seen in Fig. 24...calculate the capacitance matrix (Fig. 28). The diagonal entries are called the coefficients of capacitance, and the non-diagonal entries are called

A state interaction spin-orbit coupling density matrix renormalization group method

NASA Astrophysics Data System (ADS)

Sayfutyarova, Elvira R.; Chan, Garnet Kin-Lic

2016-06-01

We describe a state interaction spin-orbit (SISO) coupling method using density matrix renormalization group (DMRG) wavefunctions and the spin-orbit mean-field (SOMF) operator. We implement our DMRG-SISO scheme using a spin-adapted algorithm that computes transition density matrices between arbitrary matrix product states. To demonstrate the potential of the DMRG-SISO scheme we present accurate benchmark calculations for the zero-field splitting of the copper and gold atoms, comparing to earlier complete active space self-consistent-field and second-order complete active space perturbation theory results in the same basis. We also compute the effects of spin-orbit coupling on the spin-ladder of the iron-sulfur dimer complex [Fe2S2(SCH3)4]3-, determining the splitting of the lowest quartet and sextet states. We find that the magnitude of the zero-field splitting for the higher quartet and sextet states approaches a significant fraction of the Heisenberg exchange parameter.

Generalized Pauli constraints in reduced density matrix functional theory.

PubMed

Theophilou, Iris; Lathiotakis, Nektarios N; Marques, Miguel A L; Helbig, Nicole

2015-04-21

Functionals of the one-body reduced density matrix (1-RDM) are routinely minimized under Coleman's ensemble N-representability conditions. Recently, the topic of pure-state N-representability conditions, also known as generalized Pauli constraints, received increased attention following the discovery of a systematic way to derive them for any number of electrons and any finite dimensionality of the Hilbert space. The target of this work is to assess the potential impact of the enforcement of the pure-state conditions on the results of reduced density-matrix functional theory calculations. In particular, we examine whether the standard minimization of typical 1-RDM functionals under the ensemble N-representability conditions violates the pure-state conditions for prototype 3-electron systems. We also enforce the pure-state conditions, in addition to the ensemble ones, for the same systems and functionals and compare the correlation energies and optimal occupation numbers with those obtained by the enforcement of the ensemble conditions alone.

Quantum Entanglement and Reduced Density Matrices

NASA Astrophysics Data System (ADS)

Purwanto, Agus; Sukamto, Heru; Yuwana, Lila

2018-05-01

We investigate entanglement and separability criteria of multipartite (n-partite) state by examining ranks of its reduced density matrices. Firstly, we construct the general formula to determine the criterion. A rank of origin density matrix always equals one, meanwhile ranks of reduced matrices have various ranks. Next, separability and entanglement criterion of multipartite is determined by calculating ranks of reduced density matrices. In this article we diversify multipartite state criteria into completely entangled state, completely separable state, and compound state, i.e. sub-entangled state and sub-entangledseparable state. Furthermore, we also shorten the calculation proposed by the previous research to determine separability of multipartite state and expand the methods to be able to differ multipartite state based on criteria above.

Wavelets in electronic structure calculations

NASA Astrophysics Data System (ADS)

Modisette, Jason Perry

1997-09-01

Ab initio calculations of the electronic structure of bulk materials and large clusters are not possible on today's computers using current techniques. The storage and diagonalization of the Hamiltonian matrix are the limiting factors in both memory and execution time. The scaling of both quantities with problem size can be reduced by using approximate diagonalization or direct minimization of the total energy with respect to the density matrix in conjunction with a localized basis. Wavelet basis members are much more localized than conventional bases such as Gaussians or numerical atomic orbitals. This localization leads to sparse matrices of the operators that arise in SCF multi-electron calculations. We have investigated the construction of the one-electron Hamiltonian, and also the effective one- electron Hamiltonians that appear in density-functional and Hartree-Fock theories. We develop efficient methods for the generation of the kinetic energy and potential matrices, the Hartree and exchange potentials, and the local exchange-correlation potential of the LDA. Test calculations are performed on one-electron problems with a variety of potentials in one and three dimensions.

Thermal and active fluctuations of a compressible bilayer vesicle

NASA Astrophysics Data System (ADS)

Sachin Krishnan, T. V.; Yasuda, Kento; Okamoto, Ryuichi; Komura, Shigeyuki

2018-05-01

We discuss thermal and active fluctuations of a compressible bilayer vesicle by using the results of hydrodynamic theory for vesicles. Coupled Langevin equations for the membrane deformation and the density fields are employed to calculate the power spectral density matrix of membrane fluctuations. Thermal contribution is obtained by means of the fluctuation dissipation theorem, whereas active contribution is calculated from exponentially decaying time correlation functions of active random forces. We obtain the total power spectral density as a sum of thermal and active contributions. An apparent response function is further calculated in order to compare with the recent microrheology experiment on red blood cells. An enhanced response is predicted in the low-frequency regime for non-thermal active fluctuations.

Disorder and superfluid density in overdoped cuprate superconductors

NASA Astrophysics Data System (ADS)

Lee-Hone, N. R.; Dodge, J. S.; Broun, D. M.

2017-07-01

We calculate superfluid density for a dirty d -wave superconductor. The effects of impurity scattering are treated within the self-consistent t -matrix approximation, in weak-coupling BCS theory. Working from a realistic tight-binding parametrization of the Fermi surface, we find a superfluid density that is both correlated with Tc and linear in temperature, in good correspondence with recent experiments on overdoped La2 -xSrxCuO4 .

Intersubband Transitions in InAs/AlSb Quantum Wells

NASA Technical Reports Server (NTRS)

Li, J.; Koloklov, K.; Ning, C. Z.; Larraber, D. C.; Khodaparast, G. A.; Kono, J.; Ueda, K.; Nakajima, Y.; Sasa, S.; Inoue, M.

2003-01-01

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.

Dynamical simulation of electron transfer processes in self-assembled monolayers at metal surfaces using a density matrix approach.

PubMed

Prucker, V; Bockstedte, M; Thoss, M; Coto, P B

2018-03-28

A single-particle density matrix approach is introduced to simulate the dynamics of heterogeneous electron transfer (ET) processes at interfaces. The characterization of the systems is based on a model Hamiltonian parametrized by electronic structure calculations and a partitioning method. The method is applied to investigate ET in a series of nitrile-substituted (poly)(p-phenylene)thiolate self-assembled monolayers adsorbed at the Au(111) surface. The results show a significant dependence of the ET on the orbital symmetry of the donor state and on the molecular and electronic structure of the spacer.

Effective representation of amide III, II, I, and A modes on local vibrational modes: Analysis of ab initio quantum calculation results.

PubMed

Hahn, Seungsoo

2016-10-28

The Hamiltonian matrix for the first excited vibrational states of a protein can be effectively represented by local vibrational modes constituting amide III, II, I, and A modes to simulate various vibrational spectra. Methods for obtaining the Hamiltonian matrix from ab initio quantum calculation results are discussed, where the methods consist of three steps: selection of local vibrational mode coordinates, calculation of a reduced Hessian matrix, and extraction of the Hamiltonian matrix from the Hessian matrix. We introduce several methods for each step. The methods were assessed based on the density functional theory calculation results of 24 oligopeptides with four different peptide lengths and six different secondary structures. The completeness of a Hamiltonian matrix represented in the reduced local mode space is improved by adopting a specific atom group for each amide mode and reducing the effect of ignored local modes. The calculation results are also compared to previous models using C=O stretching vibration and transition dipole couplings. We found that local electric transition dipole moments of the amide modes are mainly bound on the local peptide planes. Their direction and magnitude are well conserved except amide A modes, which show large variation. Contrary to amide I modes, the vibrational coupling constants of amide III, II, and A modes obtained by analysis of a dipeptide are not transferable to oligopeptides with the same secondary conformation because coupling constants are affected by the surrounding atomic environment.

Communication: Hilbert-space partitioning of the molecular one-electron density matrix with orthogonal projectors

NASA Astrophysics Data System (ADS)

Vanfleteren, Diederik; Van Neck, Dimitri; Bultinck, Patrick; Ayers, Paul W.; Waroquier, Michel

2010-12-01

A double-atom partitioning of the molecular one-electron density matrix is used to describe atoms and bonds. All calculations are performed in Hilbert space. The concept of atomic weight functions (familiar from Hirshfeld analysis of the electron density) is extended to atomic weight matrices. These are constructed to be orthogonal projection operators on atomic subspaces, which has significant advantages in the interpretation of the bond contributions. In close analogy to the iterative Hirshfeld procedure, self-consistency is built in at the level of atomic charges and occupancies. The method is applied to a test set of about 67 molecules, representing various types of chemical binding. A close correlation is observed between the atomic charges and the Hirshfeld-I atomic charges.

Validation and application of auxiliary density perturbation theory and non-iterative approximation to coupled-perturbed Kohn-Sham approach for calculation of dipole-quadrupole polarizability

NASA Astrophysics Data System (ADS)

Shedge, Sapana V.; Pal, Sourav; Köster, Andreas M.

2011-07-01

Recently, two non-iterative approaches have been proposed to calculate response properties within density functional theory (DFT). These approaches are auxiliary density perturbation theory (ADPT) and the non-iterative approach to the coupled-perturbed Kohn-Sham (NIA-CPKS) method. Though both methods are non-iterative, they use different techniques to obtain the perturbed Kohn-Sham matrix. In this Letter, for the first time, both of these two independent methods have been used for the calculation of dipole-quadrupole polarizabilities. To validate these methods, three tetrahedral molecules viz., P4,CH4 and adamantane (C10H16) have been used as examples. The comparison with MP2 and CCSD proves the reliability of the methodology.

Linear scaling computation of the Fock matrix. II. Rigorous bounds on exchange integrals and incremental Fock build

NASA Astrophysics Data System (ADS)

Schwegler, Eric; Challacombe, Matt; Head-Gordon, Martin

1997-06-01

A new linear scaling method for computation of the Cartesian Gaussian-based Hartree-Fock exchange matrix is described, which employs a method numerically equivalent to standard direct SCF, and which does not enforce locality of the density matrix. With a previously described method for computing the Coulomb matrix [J. Chem. Phys. 106, 5526 (1997)], linear scaling incremental Fock builds are demonstrated for the first time. Microhartree accuracy and linear scaling are achieved for restricted Hartree-Fock calculations on sequences of water clusters and polyglycine α-helices with the 3-21G and 6-31G basis sets. Eightfold speedups are found relative to our previous method. For systems with a small ionization potential, such as graphitic sheets, the method naturally reverts to the expected quadratic behavior. Also, benchmark 3-21G calculations attaining microhartree accuracy are reported for the P53 tetramerization monomer involving 698 atoms and 3836 basis functions.

Spectral functions with the density matrix renormalization group: Krylov-space approach for correction vectors

DOE Office of Scientific and Technical Information (OSTI.GOV)

None, None

Frequency-dependent correlations, such as the spectral function and the dynamical structure factor, help illustrate condensed matter experiments. Within the density matrix renormalization group (DMRG) framework, an accurate method for calculating spectral functions directly in frequency is the correction-vector method. The correction vector can be computed by solving a linear equation or by minimizing a functional. Our paper proposes an alternative to calculate the correction vector: to use the Krylov-space approach. This paper also studies the accuracy and performance of the Krylov-space approach, when applied to the Heisenberg, the t-J, and the Hubbard models. The cases we studied indicate that themore » Krylov-space approach can be more accurate and efficient than the conjugate gradient, and that the error of the former integrates best when a Krylov-space decomposition is also used for ground state DMRG.« less

On the stability of the electronic system in transition metal dichalcogenides.

PubMed

Faraggi, M N; Zubizarreta, X; Arnau, A; Silkin, V M

2016-05-11

Based on first-principles calculations, we prove that the origin of charge-density wave formation in metallic layered transition metal dichalcogenides (TMDC) is not due to an electronic effect, like the Fermi surface (FS) nesting, as it had been proposed. In particular, we consider NbSe2, NbS2, TaSe2, and TaS2 as representative examples of 2H-TMDC polytypes. Our main result consists that explicit inclusion of the matrix elements in first-principles calculations of the electron susceptibility [Formula: see text] removes, due to strong momentum dependence of the matrix elements, almost all the information about the FS topologies in the resulting [Formula: see text]. This finding strongly supports an interpretation in which the momentum dependence of the electron-phonon interaction is the only reason why the phenomenon of charge-density waves appears in this class of materials.

Spectral functions with the density matrix renormalization group: Krylov-space approach for correction vectors

DOE PAGES

None, None

2016-11-21

Frequency-dependent correlations, such as the spectral function and the dynamical structure factor, help illustrate condensed matter experiments. Within the density matrix renormalization group (DMRG) framework, an accurate method for calculating spectral functions directly in frequency is the correction-vector method. The correction vector can be computed by solving a linear equation or by minimizing a functional. Our paper proposes an alternative to calculate the correction vector: to use the Krylov-space approach. This paper also studies the accuracy and performance of the Krylov-space approach, when applied to the Heisenberg, the t-J, and the Hubbard models. The cases we studied indicate that themore » Krylov-space approach can be more accurate and efficient than the conjugate gradient, and that the error of the former integrates best when a Krylov-space decomposition is also used for ground state DMRG.« less

Quadratic canonical transformation theory and higher order density matrices.

PubMed

Neuscamman, Eric; Yanai, Takeshi; Chan, Garnet Kin-Lic

2009-03-28

Canonical transformation (CT) theory provides a rigorously size-extensive description of dynamic correlation in multireference systems, with an accuracy superior to and cost scaling lower than complete active space second order perturbation theory. Here we expand our previous theory by investigating (i) a commutator approximation that is applied at quadratic, as opposed to linear, order in the effective Hamiltonian, and (ii) incorporation of the three-body reduced density matrix in the operator and density matrix decompositions. The quadratic commutator approximation improves CT's accuracy when used with a single-determinant reference, repairing the previous formal disadvantage of the single-reference linear CT theory relative to singles and doubles coupled cluster theory. Calculations on the BH and HF binding curves confirm this improvement. In multireference systems, the three-body reduced density matrix increases the overall accuracy of the CT theory. Tests on the H(2)O and N(2) binding curves yield results highly competitive with expensive state-of-the-art multireference methods, such as the multireference Davidson-corrected configuration interaction (MRCI+Q), averaged coupled pair functional, and averaged quadratic coupled cluster theories.

Systematic sparse matrix error control for linear scaling electronic structure calculations.

PubMed

Rubensson, Emanuel H; Sałek, Paweł

2005-11-30

Efficient truncation criteria used in multiatom blocked sparse matrix operations for ab initio calculations are proposed. As system size increases, so does the need to stay on top of errors and still achieve high performance. A variant of a blocked sparse matrix algebra to achieve strict error control with good performance is proposed. The presented idea is that the condition to drop a certain submatrix should depend not only on the magnitude of that particular submatrix, but also on which other submatrices that are dropped. The decision to remove a certain submatrix is based on the contribution the removal would cause to the error in the chosen norm. We study the effect of an accumulated truncation error in iterative algorithms like trace correcting density matrix purification. One way to reduce the initial exponential growth of this error is presented. The presented error control for a sparse blocked matrix toolbox allows for achieving optimal performance by performing only necessary operations needed to maintain the requested level of accuracy. Copyright 2005 Wiley Periodicals, Inc.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Malone, Fionn D., E-mail: f.malone13@imperial.ac.uk; Lee, D. K. K.; Foulkes, W. M. C.

The recently developed density matrix quantum Monte Carlo (DMQMC) algorithm stochastically samples the N-body thermal density matrix and hence provides access to exact properties of many-particle quantum systems at arbitrary temperatures. We demonstrate that moving to the interaction picture provides substantial benefits when applying DMQMC to interacting fermions. In this first study, we focus on a system of much recent interest: the uniform electron gas in the warm dense regime. The basis set incompleteness error at finite temperature is investigated and extrapolated via a simple Monte Carlo sampling procedure. Finally, we provide benchmark calculations for a four-electron system, comparing ourmore » results to previous work where possible.« less

Low complexity Reed-Solomon-based low-density parity-check design for software defined optical transmission system based on adaptive puncturing decoding algorithm

NASA Astrophysics Data System (ADS)

Pan, Xiaolong; Liu, Bo; Zheng, Jianglong; Tian, Qinghua

2016-08-01

We propose and demonstrate a low complexity Reed-Solomon-based low-density parity-check (RS-LDPC) code with adaptive puncturing decoding algorithm for elastic optical transmission system. Partial received codes and the relevant column in parity-check matrix can be punctured to reduce the calculation complexity by adaptive parity-check matrix during decoding process. The results show that the complexity of the proposed decoding algorithm is reduced by 30% compared with the regular RS-LDPC system. The optimized code rate of the RS-LDPC code can be obtained after five times iteration.

Variational calculation of second-order reduced density matrices by strong N-representability conditions and an accurate semidefinite programming solver.

PubMed

Nakata, Maho; Braams, Bastiaan J; Fujisawa, Katsuki; Fukuda, Mituhiro; Percus, Jerome K; Yamashita, Makoto; Zhao, Zhengji

2008-04-28

The reduced density matrix (RDM) method, which is a variational calculation based on the second-order reduced density matrix, is applied to the ground state energies and the dipole moments for 57 different states of atoms, molecules, and to the ground state energies and the elements of 2-RDM for the Hubbard model. We explore the well-known N-representability conditions (P, Q, and G) together with the more recent and much stronger T1 and T2(') conditions. T2(') condition was recently rederived and it implies T2 condition. Using these N-representability conditions, we can usually calculate correlation energies in percentage ranging from 100% to 101%, whose accuracy is similar to CCSD(T) and even better for high spin states or anion systems where CCSD(T) fails. Highly accurate calculations are carried out by handling equality constraints and/or developing multiple precision arithmetic in the semidefinite programming (SDP) solver. Results show that handling equality constraints correctly improves the accuracy from 0.1 to 0.6 mhartree. Additionally, improvements by replacing T2 condition with T2(') condition are typically of 0.1-0.5 mhartree. The newly developed multiple precision arithmetic version of SDP solver calculates extraordinary accurate energies for the one dimensional Hubbard model and Be atom. It gives at least 16 significant digits for energies, where double precision calculations gives only two to eight digits. It also provides physically meaningful results for the Hubbard model in the high correlation limit.

Density matrix embedding in an antisymmetrized geminal power bath

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tsuchimochi, Takashi; Welborn, Matthew; Van Voorhis, Troy, E-mail: tvan@mit.edu

2015-07-14

Density matrix embedding theory (DMET) has emerged as a powerful tool for performing wave function-in-wave function embedding for strongly correlated systems. In traditional DMET, an accurate calculation is performed on a small impurity embedded in a mean field bath. Here, we extend the original DMET equations to account for correlation in the bath via an antisymmetrized geminal power (AGP) wave function. The resulting formalism has a number of advantages. First, it allows one to properly treat the weak correlation limit of independent pairs, which DMET is unable to do with a mean-field bath. Second, it associates a size extensive correlationmore » energy with a given density matrix (for the models tested), which AGP by itself is incapable of providing. Third, it provides a reasonable description of charge redistribution in strongly correlated but non-periodic systems. Thus, AGP-DMET appears to be a good starting point for describing electron correlation in molecules, which are aperiodic and possess both strong and weak electron correlation.« less

A state interaction spin-orbit coupling density matrix renormalization group method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sayfutyarova, Elvira R.; Chan, Garnet Kin-Lic

We describe a state interaction spin-orbit (SISO) coupling method using density matrix renormalization group (DMRG) wavefunctions and the spin-orbit mean-field (SOMF) operator. We implement our DMRG-SISO scheme using a spin-adapted algorithm that computes transition density matrices between arbitrary matrix product states. To demonstrate the potential of the DMRG-SISO scheme we present accurate benchmark calculations for the zero-field splitting of the copper and gold atoms, comparing to earlier complete active space self-consistent-field and second-order complete active space perturbation theory results in the same basis. We also compute the effects of spin-orbit coupling on the spin-ladder of the iron-sulfur dimer complex [Fe{submore » 2}S{sub 2}(SCH{sub 3}){sub 4}]{sup 3−}, determining the splitting of the lowest quartet and sextet states. We find that the magnitude of the zero-field splitting for the higher quartet and sextet states approaches a significant fraction of the Heisenberg exchange parameter.« less

Regenerator filled with a matrix of polycrystalline iron whiskers

NASA Astrophysics Data System (ADS)

Eder, F. X.; Appel, H.

1982-08-01

In thermal regenerators, parameters were optimized: convection coefficient, surface of heat accumulating matrix, matrix density and heat capacity, and frequency of cycle inversions. The variation of heat capacity with working temperature was also computed. Polycrystalline iron whiskers prove a good compromise as matrix for heat regenerators at working temperatures ranging from 300 to 80 K. They were compared with wire mesh screens and microspheres of bronze and stainless steel. For theses structures and materials, thermal conductivity, pressure drop, heat transfer and yield were calculated and related to the experimental values. As transport heat gas, helium, argon, and dry nitrogen were applied at pressures up to 20 bar. Experimental and theoretical studies result in a set of formulas for calculating pressure drop, heat capacity, and heat transfer rate for a given thermal regenerator in function of mass flow. It is proved that a whisker matrix has an efficiency that depends strongly on gas pressure and composition. Iron whiskers make a good matrix with heat capacities of kW/cu cm per K, but their relative high pressure drop may, at low pressures, be a limitation. A regenerator expansion machine is described.

Multiple-scattering model for inclusive proton production in heavy ion collisions

NASA Technical Reports Server (NTRS)

Cucinotta, Francis A.

1994-01-01

A formalism is developed for evaluating the momentum distribution for proton production in nuclear abrasion during heavy ion collisions using the Glauber multiple-scattering series. Several models for the one-body density matrix of nuclei are considered for performing numerical calculations. Calculations for the momentum distribution of protons in abrasion are compared with experimental data for inclusive proton production.

The supersymmetric method in random matrix theory and applications to QCD

NASA Astrophysics Data System (ADS)

Verbaarschot, Jacobus

2004-12-01

The supersymmetric method is a powerful method for the nonperturbative evaluation of quenched averages in disordered systems. Among others, this method has been applied to the statistical theory of S-matrix fluctuations, the theory of universal conductance fluctuations and the microscopic spectral density of the QCD Dirac operator. We start this series of lectures with a general review of Random Matrix Theory and the statistical theory of spectra. An elementary introduction of the supersymmetric method in Random Matrix Theory is given in the second and third lecture. We will show that a Random Matrix Theory can be rewritten as an integral over a supermanifold. This integral will be worked out in detail for the Gaussian Unitary Ensemble that describes level correlations in systems with broken time-reversal invariance. We especially emphasize the role of symmetries. As a second example of the application of the supersymmetric method we discuss the calculation of the microscopic spectral density of the QCD Dirac operator. This is the eigenvalue density near zero on the scale of the average level spacing which is known to be given by chiral Random Matrix Theory. Also in this case we use symmetry considerations to rewrite the generating function for the resolvent as an integral over a supermanifold. The main topic of the second last lecture is the recent developments on the relation between the supersymmetric partition function and integrable hierarchies (in our case the Toda lattice hierarchy). We will show that this relation is an efficient way to calculate superintegrals. Several examples that were given in previous lectures will be worked out by means of this new method. Finally, we will discuss the quenched QCD Dirac spectrum at nonzero chemical potential. Because of the nonhermiticity of the Dirac operator the usual supersymmetric method has not been successful in this case. However, we will show that the supersymmetric partition function can be evaluated by means of the replica limit of the Toda lattice equation.

Improved hybrid algorithm with Gaussian basis sets and plane waves: First-principles calculations of ethylene adsorption on β-SiC(001)-(3×2)

NASA Astrophysics Data System (ADS)

Wieferink, Jürgen; Krüger, Peter; Pollmann, Johannes

2006-11-01

We present an algorithm for DFT calculations employing Gaussian basis sets for the wave function and a Fourier basis for the potential representation. In particular, a numerically very efficient calculation of the local potential matrix elements and the charge density is described. Special emphasis is placed on the consequences of periodicity and explicit k -vector dependence. The algorithm is tested by comparison with more straightforward ones for the case of adsorption of ethylene on the silicon-rich SiC(001)-(3×2) surface clearly revealing its substantial advantages. A complete self-consistency cycle is speeded up by roughly one order of magnitude since the calculation of matrix elements and of the charge density are accelerated by factors of 10 and 80, respectively, as compared to their straightforward calculation. Our results for C2H4:SiC(001)-(3×2) show that ethylene molecules preferentially adsorb in on-top positions above Si dimers on the substrate surface saturating both dimer dangling bonds per unit cell. In addition, a twist of the molecules around a surface-perpendicular axis is slightly favored energetically similar to the case of a complete monolayer of ethylene adsorbed on the Si(001)-(2×1) surface.

Quantum calculations for one-dimensional cooling of helium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vredenbregt, E.; Doery, M.; Bergeman, T.

1993-05-01

We report theoretical velocity distributions for sub-Doppler laser cooling of metastable He*(2{sup 3}S), calculated with the Density Matrix and Monte Carlo Wavefunction approaches. For low-field (B = 50 mG) magnetic-field induced laser cooling on the 2{sup 3}S {yields} (2{sup 3}P, J = 2) transition ({lambda} = 1083 nm), we get a narrow, sub-Doppler structure, consisting of three, {approximately}1 photon recoil wide peaks, spaced {approximately}1 recoil apart. With increasing field, this three-peak structure develops into two velocity-selective resonance (VSR) peaks, each {approximately}2 recoils wide. For the 2{sup 3}S {yields} (3{sup 3}P, J = 2) transition ({lambda} 389 nm), VSR peaks aremore » predicted to appear at low field without the third, central peak, which only develops at higher field (B = 200 mG). Additional computations deal with polarization-gradient cooling. In general, we find that for one-dimensional cooling calculations, the Density Matrix method is more efficient than the Monte Carlo Wavefunction approach. Experiments are currently under way to test the results.« less

Matrix isolation infrared spectroscopic studies and density functional theory calculations of the MNN, (MN)2 (M = Y and La), and Y3NN molecules.

PubMed

Teng, Yun-Lei; Xu, Qiang

2008-04-24

The reactions of yttrium and lanthanum with dinitrogen were reinvestigated. Laser-ablated yttrium and lanthanum atoms were co-deposited at 4 K with dinitrogen in excess argon, and the low-temperature reactions of Y and La with N2 in solid argon were studied using infrared spectroscopy. The reaction products YNN, (YN)2, LaNN, and (LaN)2 were formed in the present experiments and characterized on the basis of 14N/15N isotopic shifts, mixed isotope splitting patterns, stepwise annealing, change of reagent concentration and laser energy, and comparison with theoretical predictions. Some assignments were made based on a previous report. Density functional theory calculations were performed on these systems to identify possible reaction products. The agreement between experimental and calculated vibrational frequencies, relative absorption intensities, and isotopic shifts of the MNN and (MN)2 (M = Y and La) molecules supports the identification of these molecules from the matrix infrared spectra. Plausible reaction mechanisms were proposed for the formation of these molecules along with tentative identification of the Y3NN molecule.

Quantum Crystallography: Density Matrix-Density Functional Theory and the X-Ray Diffraction Experiment

NASA Astrophysics Data System (ADS)

Soirat, Arnaud J. A.

Density Matrix Theory is a Quantum Mechanical formalism in which the wavefunction is eliminated and its role taken over by reduced density matrices. The interest of this is that, it allows one, in principle, to calculate any electronic property of a physical system, without having to solve the Schrodinger equation, using only two entities much simpler than an N-body wavefunction: first and second -order reduced density matrices. In practice, though, this very promising possibility faces the tremendous theoretical problem of N-representability, which has been solved for the former, but, until now, voids any hope of theoretically determining the latter. However, it has been shown that single determinant reduced density matrices of any order may be recovered from coherent X-ray diffraction data, if one provides a proper Quantum Mechanical description of the Crystallography experiment. A deeper investigation of this method is the purpose of this work, where we, first, further study the calculation of X-ray reduced density matrices N-representable by a single Slater determinant. In this context, we independently derive necessary and sufficient conditions for the uniqueness of the method. We then show how to account for electron correlation in this model. For the first time, indeed, we derive highly accurate, yet practical, density matrices approximately N-representable by correlated-determinant wavefunctions. The interest of such a result lies in the Quantum Mechanical validity of these density matrices, their property of being entirely obtainable from X-ray coherent diffraction data, their very high accuracy conferred by this known property of the N-representing wavefunction, as well as their definition as explicit functionals of the density. All of these properties are finally used in both a theoretical and a numerical application: in the former, we show that these density matrices may be used in the context of Density Functional Theory to highly accurately determine the unknown HK functional, associated with the theorem of Hohenberg and Kohn. The latter is provided by the calculation of helium correlation energy, where we test approximating the second-order density function by the leading term of its McLaurin's series expansion.

Open-Ended Recursive Approach for the Calculation of Multiphoton Absorption Matrix Elements

PubMed Central

2015-01-01

We present an implementation of single residues for response functions to arbitrary order using a recursive approach. Explicit expressions in terms of density-matrix-based response theory for the single residues of the linear, quadratic, cubic, and quartic response functions are also presented. These residues correspond to one-, two-, three- and four-photon transition matrix elements. The newly developed code is used to calculate the one-, two-, three- and four-photon absorption cross sections of para-nitroaniline and para-nitroaminostilbene, making this the first treatment of four-photon absorption in the framework of response theory. We find that the calculated multiphoton absorption cross sections are not very sensitive to the size of the basis set as long as a reasonably large basis set with diffuse functions is used. The choice of exchange–correlation functional, however, significantly affects the calculated cross sections of both charge-transfer transitions and other transitions, in particular, for the larger para-nitroaminostilbene molecule. We therefore recommend the use of a range-separated exchange–correlation functional in combination with the augmented correlation-consistent double-ζ basis set aug-cc-pVDZ for the calculation of multiphoton absorption properties. PMID:25821415

Pulsed field gradients in simulations of one- and two-dimensional NMR spectra.

PubMed

Meresi, G H; Cuperlovic, M; Palke, W E; Gerig, J T

1999-03-01

A method for the inclusion of the effects of z-axis pulsed field gradients in computer simulations of an arbitrary pulsed NMR experiment with spin (1/2) nuclei is described. Recognizing that the phase acquired by a coherence following the application of a z-axis pulsed field gradient bears a fixed relation to its order and the spatial position of the spins in the sample tube, the sample is regarded as a collection of volume elements, each phase-encoded by a characteristic, spatially dependent precession frequency. The evolution of the sample's density matrix is thus obtained by computing the evolution of the density matrix for each volume element. Following the last gradient pulse, these density matrices are combined to form a composite density matrix which evolves through the rest of the experiment to yield the observable signal. This approach is implemented in a program which includes capabilities for rigorous inclusion of spin relaxation by dipole-dipole, chemical shift anisotropy, and random field mechanisms, plus the effects of arbitrary RF fields. Mathematical procedures for accelerating these calculations are described. The approach is illustrated by simulations of representative one- and two-dimensional NMR experiments. Copyright 1999 Academic Press.

I-V characterization of a quantum well infrared photodetector with stepped and graded barriers

NASA Astrophysics Data System (ADS)

Nutku, F.; Erol, A.; Gunes, M.; Buklu, L. B.; Ergun, Y.; Arikan, M. C.

2012-09-01

I-V characterization of an n-type quantum well infrared photodetector which consists of stepped and graded barriers has been done under dark at temperatures between 20-300 K. Different current transport mechanisms and transition between them have been observed at temperature around 47 K. Activation energies of the electrons at various bias voltages have been obtained from the temperature dependent I-V measurements. Activation energy at zero bias has been calculated by extrapolating the bias dependence of the activation energies. Ground state energies and barrier heights of the four different quantum wells have been calculated by using an iterative technique, which depends on experimentally obtained activation energy. Ground state energies also have been calculated with transfer matrix technique and compared with iteration results. Incorporating the effect of high electron density induced electron exchange interaction on ground state energies; more consistent results with theoretical transfer matrix calculations have been obtained.

Neutrinoless ββ decay mediated by the exchange of light and heavy neutrinos: the role of nuclear structure correlations

NASA Astrophysics Data System (ADS)

Menéndez, J.

2018-01-01

Neutrinoless β β decay nuclear matrix elements calculated with the shell model and energy-density functional theory typically disagree by more than a factor of two in the standard scenario of light-neutrino exchange. In contrast, for a decay mediated by sterile heavy neutrinos the deviations are reduced to about 50%, an uncertainty similar to the one due to short-range effects. We compare matrix elements in the light- and heavy-neutrino-exchange channels, exploring the radial, momentum transfer and angular momentum-parity matrix element distributions, and considering transitions that involve correlated and uncorrelated nuclear states. We argue that the shorter-range heavy-neutrino exchange is less sensitive to collective nuclear correlations, and that discrepancies in matrix elements are mostly due to the treatment of long-range correlations in many-body calculations. Our analysis supports previous studies suggesting that isoscalar pairing correlations, which affect mostly the longer-range part of the neutrinoless β β decay operator, are partially responsible for the differences between nuclear matrix elements in the standard light-neutrino-exchange mechanism.

Inner Space Perturbation Theory in Matrix Product States: Replacing Expensive Iterative Diagonalization.

PubMed

Ren, Jiajun; Yi, Yuanping; Shuai, Zhigang

2016-10-11

We propose an inner space perturbation theory (isPT) to replace the expensive iterative diagonalization in the standard density matrix renormalization group theory (DMRG). The retained reduced density matrix eigenstates are partitioned into the active and secondary space. The first-order wave function and the second- and third-order energies are easily computed by using one step Davidson iteration. Our formulation has several advantages including (i) keeping a balance between the efficiency and accuracy, (ii) capturing more entanglement with the same amount of computational time, (iii) recovery of the standard DMRG when all the basis states belong to the active space. Numerical examples for the polyacenes and periacene show that the efficiency gain is considerable and the accuracy loss due to the perturbation treatment is very small, when half of the total basis states belong to the active space. Moreover, the perturbation calculations converge in all our numerical examples.

An efficient method for quantum transport simulations in the time domain

NASA Astrophysics Data System (ADS)

Wang, Y.; Yam, C.-Y.; Frauenheim, Th.; Chen, G. H.; Niehaus, T. A.

2011-11-01

An approximate method based on adiabatic time dependent density functional theory (TDDFT) is presented, that allows for the description of the electron dynamics in nanoscale junctions under arbitrary time dependent external potentials. The density matrix of the device region is propagated according to the Liouville-von Neumann equation. The semi-infinite leads give rise to dissipative terms in the equation of motion which are calculated from first principles in the wide band limit. In contrast to earlier ab initio implementations of this formalism, the Hamiltonian is here approximated in the spirit of the density functional based tight-binding (DFTB) method. Results are presented for two prototypical molecular devices and compared to full TDDFT calculations. The temporal profile of the current traces is qualitatively well captured by the DFTB scheme. Steady state currents show considerable variations, both in comparison of approximate and full TDDFT, but also among TDDFT calculations with different basis sets.

Revisit of Rotational Dynamics of Asteroid 4179 Toutatis from Chang'e-2's flyby

NASA Astrophysics Data System (ADS)

Zhao, Yuhui; Hu, Shoucun; Ji, Jianghui

2015-08-01

In this work we investigate the rotational dynamics of Toutatis based on the derived results from Chang'e-2's close flyby to the asteroid (Huang et al. 2013). Toutatis' non-principal axis rotation (NPA) was revealed by radar observations captured from its Earth approaches in the past two decades. Matrix of inertia calculated from radar derived shape model are inconsistent with observations, which may indicate an uneven density distribution of the asteroid. We perform numerical simulations of rotational evolution of Toutatis and figure out the relative rotational parameters of Euler angles, rotational velocities and matrix of inertia. According to the major morphological feature of the ginger-shaped asteroid, we suggest a density ratio of the two lobes. On the basis of these results, we will evaluate the magnitude of the bias of mass center and figure center, which may have slight effects in the momentum variation calculation. These results are in good agreements with the previous radar observation derived results (Takahashi et al. 2013).

Microscopically based energy density functionals for nuclei using the density matrix expansion: Implementation and pre-optimization

NASA Astrophysics Data System (ADS)

Stoitsov, M.; Kortelainen, M.; Bogner, S. K.; Duguet, T.; Furnstahl, R. J.; Gebremariam, B.; Schunck, N.

2010-11-01

In a recent series of articles, Gebremariam, Bogner, and Duguet derived a microscopically based nuclear energy density functional by applying the density matrix expansion (DME) to the Hartree-Fock energy obtained from chiral effective field theory two- and three-nucleon interactions. Owing to the structure of the chiral interactions, each coupling in the DME functional is given as the sum of a coupling constant arising from zero-range contact interactions and a coupling function of the density arising from the finite-range pion exchanges. Because the contact contributions have essentially the same structure as those entering empirical Skyrme functionals, a microscopically guided Skyrme phenomenology has been suggested in which the contact terms in the DME functional are released for optimization to finite-density observables to capture short-range correlation energy contributions from beyond Hartree-Fock. The present article is the first attempt to assess the ability of the newly suggested DME functional, which has a much richer set of density dependencies than traditional Skyrme functionals, to generate sensible and stable results for nuclear applications. The results of the first proof-of-principle calculations are given, and numerous practical issues related to the implementation of the new functional in existing Skyrme codes are discussed. Using a restricted singular value decomposition optimization procedure, it is found that the new DME functional gives numerically stable results and exhibits a small but systematic reduction of our test χ2 function compared to standard Skyrme functionals, thus justifying its suitability for future global optimizations and large-scale calculations.

Fast Time-Dependent Density Functional Theory Calculations of the X-ray Absorption Spectroscopy of Large Systems.

PubMed

Besley, Nicholas A

2016-10-11

The computational cost of calculations of K-edge X-ray absorption spectra using time-dependent density functional (TDDFT) within the Tamm-Dancoff approximation is significantly reduced through the introduction of a severe integral screening procedure that includes only integrals that involve the core s basis function of the absorbing atom(s) coupled with a reduced quality numerical quadrature for integrals associated with the exchange and correlation functionals. The memory required for the calculations is reduced through construction of the TDDFT matrix within the absorbing core orbitals excitation space and exploiting further truncation of the virtual orbital space. The resulting method, denoted fTDDFTs, leads to much faster calculations and makes the study of large systems tractable. The capability of the method is demonstrated through calculations of the X-ray absorption spectra at the carbon K-edge of chlorophyll a, C 60 and C 70 .

Unconventional field induced phases in a quantum magnet formed by free radical tetramers

NASA Astrophysics Data System (ADS)

Saúl, Andrés; Gauthier, Nicolas; Askari, Reza Moosavi; Côté, Michel; Maris, Thierry; Reber, Christian; Lannes, Anthony; Luneau, Dominique; Nicklas, Michael; Law, Joseph M.; Green, Elizabeth Lauren; Wosnitza, Jochen; Bianchi, Andrea Daniele; Feiguin, Adrian

2018-02-01

We report experimental and theoretical studies on the magnetic and thermodynamic properties of NIT-2Py, a free radical based organic magnet. From magnetization and specific-heat measurements we establish the temperature versus magnetic field phase diagram which includes two Bose-Einstein condensates (BEC) and an infrequent half-magnetization plateau. Calculations based on density functional theory demonstrate that magnetically this system can be mapped to a quasi-two-dimensional structure of weakly coupled tetramers. Density matrix renormalization group calculations show the unusual characteristics of the BECs where the spins forming the low-field condensate are different than those participating in the high-field one.

Energy-free machine learning force field for aluminum.

PubMed

Kruglov, Ivan; Sergeev, Oleg; Yanilkin, Alexey; Oganov, Artem R

2017-08-17

We used the machine learning technique of Li et al. (PRL 114, 2015) for molecular dynamics simulations. Atomic configurations were described by feature matrix based on internal vectors, and linear regression was used as a learning technique. We implemented this approach in the LAMMPS code. The method was applied to crystalline and liquid aluminum and uranium at different temperatures and densities, and showed the highest accuracy among different published potentials. Phonon density of states, entropy and melting temperature of aluminum were calculated using this machine learning potential. The results are in excellent agreement with experimental data and results of full ab initio calculations.

Investigation of the effect of scattering centers on low dimensional nanowire channel

NASA Astrophysics Data System (ADS)

Cariappa, K. S.; Shukla, Raja; Sarkar, Niladri

2018-05-01

In this work, we studied the effect of scattering centers on the electron density profiles of a one dimensional Nanowire channel. Density Matrix Formalism is used for calculating the local electron densities at room temperature. Various scattering centers have been simulated in the channel. The nearest neighbor tight binding method is applied to construct the Hamiltonian of nanoscale devices. We invoke scattering centers by adding local scattering potentials to the Hamiltonian. This analysis could give an insight into the understanding and utilization of defects for device engineering.

Excitation energies of dissociating H2: A problematic case for the adiabatic approximation of time-dependent density functional theory

NASA Astrophysics Data System (ADS)

Gritsenko, O. V.; van Gisbergen, S. J. A.; Görling, A.; Baerends, E. J.

2000-11-01

Time-dependent density functional theory (TDDFT) is applied for calculation of the excitation energies of the dissociating H2 molecule. The standard TDDFT method of adiabatic local density approximation (ALDA) totally fails to reproduce the potential curve for the lowest excited singlet 1Σu+ state of H2. Analysis of the eigenvalue problem for the excitation energies as well as direct derivation of the exchange-correlation (xc) kernel fxc(r,r',ω) shows that ALDA fails due to breakdown of its simple spatially local approximation for the kernel. The analysis indicates a complex structure of the function fxc(r,r',ω), which is revealed in a different behavior of the various matrix elements K1c,1cxc (between the highest occupied Kohn-Sham molecular orbital ψ1 and virtual MOs ψc) as a function of the bond distance R(H-H). The effect of nonlocality of fxc(r,r') is modeled by using different expressions for the corresponding matrix elements of different orbitals. Asymptotically corrected ALDA (ALDA-AC) expressions for the matrix elements K12,12xc(στ) are proposed, while for other matrix elements the standard ALDA expressions are retained. This approach provides substantial improvement over the standard ALDA. In particular, the ALDA-AC curve for the lowest singlet excitation qualitatively reproduces the shape of the exact curve. It displays a minimum and approaches a relatively large positive energy at large R(H-H). ALDA-AC also produces a substantial improvement for the calculated lowest triplet excitation, which is known to suffer from the triplet instability problem of the restricted KS ground state. Failure of the ALDA for the excitation energies is related to the failure of the local density as well as generalized gradient approximations to reproduce correctly the polarizability of dissociating H2. The expression for the response function χ is derived to show the origin of the field-counteracting term in the xc potential, which is lacking in the local density and generalized gradient approximations and which is required to obtain a correct polarizability.

Real time evolution at finite temperatures with operator space matrix product states

NASA Astrophysics Data System (ADS)

Pižorn, Iztok; Eisler, Viktor; Andergassen, Sabine; Troyer, Matthias

2014-07-01

We propose a method to simulate the real time evolution of one-dimensional quantum many-body systems at finite temperature by expressing both the density matrices and the observables as matrix product states. This allows the calculation of expectation values and correlation functions as scalar products in operator space. The simulations of density matrices in inverse temperature and the local operators in the Heisenberg picture are independent and result in a grid of expectation values for all intermediate temperatures and times. Simulations can be performed using real arithmetics with only polynomial growth of computational resources in inverse temperature and time for integrable systems. The method is illustrated for the XXZ model and the single impurity Anderson model.

Gravitational collapse and Hawking-like radiation of a shell in AdS spacetime

NASA Astrophysics Data System (ADS)

Saini, Anshul; Stojkovic, Dejan

2018-01-01

In this paper, we study the collapse of a massive shell in 2 +1 and 3 +1 dimensional gravity with anti-de Sitter asymptotics. Using the Gauss-Codazzi method, we derive gravitational equations of motion of the shell. We then use the functional Schrödinger formalism to calculate the spectrum of particles produced during the collapse. At the late time, radiation agrees very well with the standard Hawking results. In 3 +1 dimensions, we reproduce the Hawking-Page transition. We then construct the density matrix of this collapsing system and analyze the information content in the emitted radiation. We find that the off-diagonal elements of the density matrix are very important in preserving the unitarity of the system.

Density-matrix approach for the electroluminescence of molecules in a scanning tunneling microscope.

PubMed

Tian, Guangjun; Liu, Ji-Cai; Luo, Yi

2011-04-29

The electroluminescence (EL) of molecules confined inside a nanocavity in the scanning tunneling microscope possesses many intriguing but unexplained features. We present here a general theoretical approach based on the density-matrix formalism to describe the EL from molecules near a metal surface induced by both electron tunneling and localized surface plasmon excitations simultaneously. It reveals the underlying physical mechanism for the external bias dependent EL. The important role played by the localized surface plasmon on the EL is highlighted. Calculations for porphyrin derivatives have reproduced corresponding experimental spectra and nicely explained the observed unusual large variation of emission spectral profiles. This general theoretical approach can find many applications in the design of molecular electronic and photonic devices.

Enhanced superconductivity in the high pressure phase of SnAs studied from first principles

NASA Astrophysics Data System (ADS)

Sreenivasa Reddy, P. V.; Kanchana, V.; Millichamp, T. E.; Vaitheeswaran, G.; Dugdale, S. B.

2017-01-01

First principles calculations are performed using density functional theory and density functional perturbation theory for SnAs. Total energy calculations show the first order phase transition from an NaCl structure to a CsCl one at around 37 GPa, which is also confirmed from enthalpy calculations and agrees well with experimental work. Calculations of the phonon structure and hence the electron-phonon coupling, λep, and superconducting transition temperature, Tc, across the phase diagram are performed. These calculations give an ambient pressure Tc, in the NaCl structure, of 3.08 K, in good agreement with experiment whilst at the transition pressure, in the CsCl structure, a drastically increased value of Tc = 12.2 K is found. Calculations also show a dramatic increase in the electronic density of states at this pressure. The lowest energy acoustic phonon branch in each structure also demonstrates some softening effects. Electronic structure calculations of the Fermi surface in both phases are presented for the first time as well as further calculations of the generalised susceptibility with the inclusion of matrix elements. These calculations indicate that the softening is not derived from Fermi surface nesting and it is concluded to be due to a wavevector-dependent enhancement of the electron-phonon coupling.

The multifacet graphically contracted function method. I. Formulation and implementation

NASA Astrophysics Data System (ADS)

Shepard, Ron; Gidofalvi, Gergely; Brozell, Scott R.

2014-08-01

The basic formulation for the multifacet generalization of the graphically contracted function (MFGCF) electronic structure method is presented. The analysis includes the discussion of linear dependency and redundancy of the arc factor parameters, the computation of reduced density matrices, Hamiltonian matrix construction, spin-density matrix construction, the computation of optimization gradients for single-state and state-averaged calculations, graphical wave function analysis, and the efficient computation of configuration state function and Slater determinant expansion coefficients. Timings are given for Hamiltonian matrix element and analytic optimization gradient computations for a range of model problems for full-CI Shavitt graphs, and it is observed that both the energy and the gradient computation scale as O(N2n4) for N electrons and n orbitals. The important arithmetic operations are within dense matrix-matrix product computational kernels, resulting in a computationally efficient procedure. An initial implementation of the method is used to present applications to several challenging chemical systems, including N2 dissociation, cubic H8 dissociation, the symmetric dissociation of H2O, and the insertion of Be into H2. The results are compared to the exact full-CI values and also to those of the previous single-facet GCF expansion form.

The multifacet graphically contracted function method. I. Formulation and implementation.

PubMed

Shepard, Ron; Gidofalvi, Gergely; Brozell, Scott R

2014-08-14

The basic formulation for the multifacet generalization of the graphically contracted function (MFGCF) electronic structure method is presented. The analysis includes the discussion of linear dependency and redundancy of the arc factor parameters, the computation of reduced density matrices, Hamiltonian matrix construction, spin-density matrix construction, the computation of optimization gradients for single-state and state-averaged calculations, graphical wave function analysis, and the efficient computation of configuration state function and Slater determinant expansion coefficients. Timings are given for Hamiltonian matrix element and analytic optimization gradient computations for a range of model problems for full-CI Shavitt graphs, and it is observed that both the energy and the gradient computation scale as O(N(2)n(4)) for N electrons and n orbitals. The important arithmetic operations are within dense matrix-matrix product computational kernels, resulting in a computationally efficient procedure. An initial implementation of the method is used to present applications to several challenging chemical systems, including N2 dissociation, cubic H8 dissociation, the symmetric dissociation of H2O, and the insertion of Be into H2. The results are compared to the exact full-CI values and also to those of the previous single-facet GCF expansion form.

A molecular dynamics study on Young's modulus and tribology of carbon nanotube reinforced styrene-butadiene rubber.

PubMed

Chawla, Raj; Sharma, Sumit

2018-03-18

Styrene-butadiene rubber is a copolymer widely used in making car tires and has excellent abrasion resistance. The Young's modulus and tribology of pure styrene butadiene rubber (SBR) polymer and carbon nanotube reinforced polymer composites have been investigated using molecular dynamics simulations. The mechanism of enhanced tribology properties using carbon nanotube has been studied and discussed. The obtained Young's modulus shows the enhancement in mechanical properties of SBR polymer when carbon nanotubes are used as reinforcement. The concentration, temperature and velocity profiles, radial distribution function, frictional stresses, and cohesive energy density are calculated and analyzed in detail. The Young's modulus of SBR matrix increases about 29.16% in the presence of the 5% CNT. The atom movement velocity and average cohesive energy density in the friction area of pure SBR matrix was found to be more than that of the CNT/SBR composite. Graphical abstract Initial and final conditions of (a) pure SBR matrix and (b) CNT/SBR matrix subjected toshear loading and frictional stresses of top Fe layers of both pure SBR and CNT/SBR composite.

Random acoustic metamaterial with a subwavelength dipolar resonance.

PubMed

Duranteau, Mickaël; Valier-Brasier, Tony; Conoir, Jean-Marc; Wunenburger, Régis

2016-06-01

The effective velocity and attenuation of longitudinal waves through random dispersions of rigid, tungsten-carbide beads in an elastic matrix made of epoxy resin in the range of beads volume fraction 2%-10% are determined experimentally. The multiple scattering model proposed by Luppé, Conoir, and Norris [J. Acoust. Soc. Am. 131(2), 1113-1120 (2012)], which fully takes into account the elastic nature of the matrix and the associated mode conversions, accurately describes the measurements. Theoretical calculations show that the rigid particles display a local, dipolar resonance which shares several features with Minnaert resonance of bubbly liquids and with the dipolar resonance of core-shell particles. Moreover, for the samples under study, the main cause of smoothing of the dipolar resonance of the scatterers and the associated variations of the effective mass density of the dispersions is elastic relaxation, i.e., the finite time required for the shear stresses associated to the translational motion of the scatterers to propagate through the matrix. It is shown that its influence is governed solely by the value of the particle to matrix mass density contrast.

Effect of bidispersity in grafted chain length on grafted chain conformations and potential of mean force between polymer grafted nanoparticles in a homopolymer matrix.

PubMed

Nair, Nitish; Wentzel, Nathaniel; Jayaraman, Arthi

2011-05-21

In efforts to produce polymeric materials with tailored physical properties, significant interest has grown around the ability to control the spatial organization of nanoparticles in polymer nanocomposites. One way to achieve controlled particle arrangement is by grafting the nanoparticle surface with polymers that are compatible with the matrix, thus manipulating the interfacial interactions between the nanoparticles and the polymer matrix. Previous work has shown that the molecular weight of the grafted polymer, both at high grafting density and low grafting density, plays a key role in dictating the effective inter-particle interactions in a polymer matrix. At high grafting density nanoparticles disperse (aggregate) if the graft molecular weight is higher (lower) than the matrix molecular weight. At low grafting density the longer grafts can better shield the nanoparticle surface from direct particle-particle contacts than the shorter grafts and lead to the dispersion of the grafted particles in the matrix. Despite the importance of graft molecular weight, and evidence of non-trivial effects of polydispersity of chains grafted on flat surfaces, most theoretical work on polymer grafted nanoparticles has only focused on monodisperse grafted chains. In this paper, we focus on how bidispersity in grafted chain lengths affects the grafted chain conformations and inter-particle interactions in an implicit solvent and in a dense homopolymer polymer matrix. We first present the effects of bidispersity on grafted chain conformations in a single polymer grafted particle using purely Monte Carlo (MC) simulations. This is followed by calculations of the potential of mean force (PMF) between two grafted particles in a polymer matrix using a self-consistent Polymer Reference Interaction Site Model theory-Monte Carlo simulation approach. Monte Carlo simulations of a single polymer grafted particle in an implicit solvent show that in the bidisperse polymer grafted particles with an equal number of short and long grafts at low to medium grafting density, the short grafts are in a more coiled up conformation (lower radius of gyration) than their monodisperse counterparts to provide a larger free volume to the longer grafts so they can gain conformational entropy. The longer grafts do not show much difference in conformation from their monodisperse counterparts at low grafting density, but at medium grafting density the longer grafts exhibit less stretched conformations (lower radius of gyration) as compared to their monodisperse counterparts. In the presence of an explicit homopolymer matrix, the longer grafts are more compressed by the matrix homopolymer chains than the short grafts. We observe that the potential of mean force between bidisperse grafted particles has features of the PMF of monodisperse grafted particles with short grafts and monodisperse grafted particles with long grafts. The value of the PMF at contact is governed by the short grafts and values at large inter-particle distances are governed by the longer grafts. Further comparison of the PMF for bidisperse and monodisperse polymer grafted particles in a homopolymer matrix at varying parameters shows that the effects of matrix chain length, matrix packing fraction, grafting density, and particle curvature on the PMF between bidisperse polymer grafted particles are similar to those seen between monodisperse polymer grafted particles. © 2011 American Institute of Physics.

GPU acceleration of the Locally Selfconsistent Multiple Scattering code for first principles calculation of the ground state and statistical physics of materials

NASA Astrophysics Data System (ADS)

Eisenbach, Markus; Larkin, Jeff; Lutjens, Justin; Rennich, Steven; Rogers, James H.

2017-02-01

The Locally Self-consistent Multiple Scattering (LSMS) code solves the first principles Density Functional theory Kohn-Sham equation for a wide range of materials with a special focus on metals, alloys and metallic nano-structures. It has traditionally exhibited near perfect scalability on massively parallel high performance computer architectures. We present our efforts to exploit GPUs to accelerate the LSMS code to enable first principles calculations of O(100,000) atoms and statistical physics sampling of finite temperature properties. We reimplement the scattering matrix calculation for GPUs with a block matrix inversion algorithm that only uses accelerator memory. Using the Cray XK7 system Titan at the Oak Ridge Leadership Computing Facility we achieve a sustained performance of 14.5PFlop/s and a speedup of 8.6 compared to the CPU only code.

GPU acceleration of the Locally Selfconsistent Multiple Scattering code for first principles calculation of the ground state and statistical physics of materials

DOE PAGES

Eisenbach, Markus; Larkin, Jeff; Lutjens, Justin; ...

2016-07-12

The Locally Self-consistent Multiple Scattering (LSMS) code solves the first principles Density Functional theory Kohn–Sham equation for a wide range of materials with a special focus on metals, alloys and metallic nano-structures. It has traditionally exhibited near perfect scalability on massively parallel high performance computer architectures. In this paper, we present our efforts to exploit GPUs to accelerate the LSMS code to enable first principles calculations of O(100,000) atoms and statistical physics sampling of finite temperature properties. We reimplement the scattering matrix calculation for GPUs with a block matrix inversion algorithm that only uses accelerator memory. Finally, using the Craymore » XK7 system Titan at the Oak Ridge Leadership Computing Facility we achieve a sustained performance of 14.5PFlop/s and a speedup of 8.6 compared to the CPU only code.« less

Universality of quantum information in chaotic CFTs

NASA Astrophysics Data System (ADS)

Lashkari, Nima; Dymarsky, Anatoly; Liu, Hong

2018-03-01

We study the Eigenstate Thermalization Hypothesis (ETH) in chaotic conformal field theories (CFTs) of arbitrary dimensions. Assuming local ETH, we compute the reduced density matrix of a ball-shaped subsystem of finite size in the infinite volume limit when the full system is an energy eigenstate. This reduced density matrix is close in trace distance to a density matrix, to which we refer as the ETH density matrix, that is independent of all the details of an eigenstate except its energy and charges under global symmetries. In two dimensions, the ETH density matrix is universal for all theories with the same value of central charge. We argue that the ETH density matrix is close in trace distance to the reduced density matrix of the (micro)canonical ensemble. We support the argument in higher dimensions by comparing the Von Neumann entropy of the ETH density matrix with the entropy of a black hole in holographic systems in the low temperature limit. Finally, we generalize our analysis to the coherent states with energy density that varies slowly in space, and show that locally such states are well described by the ETH density matrix.

Quantum Chemical Calculations Using Accelerators: Migrating Matrix Operations to the NVIDIA Kepler GPU and the Intel Xeon Phi.

PubMed

Leang, Sarom S; Rendell, Alistair P; Gordon, Mark S

2014-03-11

Increasingly, modern computer systems comprise a multicore general-purpose processor augmented with a number of special purpose devices or accelerators connected via an external interface such as a PCI bus. The NVIDIA Kepler Graphical Processing Unit (GPU) and the Intel Phi are two examples of such accelerators. Accelerators offer peak performances that can be well above those of the host processor. How to exploit this heterogeneous environment for legacy application codes is not, however, straightforward. This paper considers how matrix operations in typical quantum chemical calculations can be migrated to the GPU and Phi systems. Double precision general matrix multiply operations are endemic in electronic structure calculations, especially methods that include electron correlation, such as density functional theory, second order perturbation theory, and coupled cluster theory. The use of approaches that automatically determine whether to use the host or an accelerator, based on problem size, is explored, with computations that are occurring on the accelerator and/or the host. For data-transfers over PCI-e, the GPU provides the best overall performance for data sizes up to 4096 MB with consistent upload and download rates between 5-5.6 GB/s and 5.4-6.3 GB/s, respectively. The GPU outperforms the Phi for both square and nonsquare matrix multiplications.

Double and Triple Si-H-M Bridge Bonds: Matrix Infrared Spectra and Theoretical Calculations for Reaction Products of Silane with Ti, Zr, and Hf Atoms.

PubMed

Xu, Bing; Shi, Peipei; Huang, Tengfei; Wang, Xuefeng; Andrews, Lester

2017-05-25

Infrared spectra of matrix isolated dibridged Si(μ-H) 2 MH 2 and tribridged Si(μ-H) 3 MH molecules (M = Zr and Hf) were observed following the laser-ablated metal atom reactions with SiH 4 during condensation in excess argon and neon, but only the latter species was observed with titanium. Assignments of the major vibrational modes, which included terminal MH, MH 2 and hydrogen bridge Si-H-M stretching modes, were confirmed by the appropriate SiD 4 isotopic shifts and density functional vibrational frequency calculations (B3LYP and BPW91). The Si-H-M hydrogen bridge bond is calculated as weak covalent interaction and compared with the C-H···M agostic interaction in terms of electron localization function (ELF) analysis and noncovalent interaction index (NCI) calculations. Furthermore, the different products of Ti, Zr, and Hf reactions with SiH 4 are discussed in detail.

T-matrix modeling of linear depolarization by morphologically complex soot and soot-containing aerosols

NASA Astrophysics Data System (ADS)

Mishchenko, Michael I.; Liu, Li; Mackowski, Daniel W.

2013-07-01

We use state-of-the-art public-domain Fortran codes based on the T-matrix method to calculate orientation and ensemble averaged scattering matrix elements for a variety of morphologically complex black carbon (BC) and BC-containing aerosol particles, with a special emphasis on the linear depolarization ratio (LDR). We explain theoretically the quasi-Rayleigh LDR peak at side-scattering angles typical of low-density soot fractals and conclude that the measurement of this feature enables one to evaluate the compactness state of BC clusters and trace the evolution of low-density fluffy fractals into densely packed aggregates. We show that small backscattering LDRs measured with ground-based, airborne, and spaceborne lidars for fresh smoke generally agree with the values predicted theoretically for fluffy BC fractals and densely packed near-spheroidal BC aggregates. To reproduce higher lidar LDRs observed for aged smoke, one needs alternative particle models such as shape mixtures of BC spheroids or cylinders.

T-Matrix Modeling of Linear Depolarization by Morphologically Complex Soot and Soot-Containing Aerosols

NASA Technical Reports Server (NTRS)

Mishchenko, Michael I.; Liu, Li; Mackowski, Daniel W.

2013-01-01

We use state-of-the-art public-domain Fortran codes based on the T-matrix method to calculate orientation and ensemble averaged scattering matrix elements for a variety of morphologically complex black carbon (BC) and BC-containing aerosol particles, with a special emphasis on the linear depolarization ratio (LDR). We explain theoretically the quasi-Rayleigh LDR peak at side-scattering angles typical of low-density soot fractals and conclude that the measurement of this feature enables one to evaluate the compactness state of BC clusters and trace the evolution of low-density fluffy fractals into densely packed aggregates. We show that small backscattering LDRs measured with groundbased, airborne, and spaceborne lidars for fresh smoke generally agree with the values predicted theoretically for fluffy BC fractals and densely packed near-spheroidal BC aggregates. To reproduce higher lidar LDRs observed for aged smoke, one needs alternative particle models such as shape mixtures of BC spheroids or cylinders.

Extended Bose-Hubbard model with dipolar and contact interactions

NASA Astrophysics Data System (ADS)

Biedroń, Krzysztof; Łącki, Mateusz; Zakrzewski, Jakub

2018-06-01

We study the phase diagram of the one-dimensional boson gas trapped inside an optical lattice with contact and dipolar interaction, taking into account next-nearest terms for both tunneling and interaction. Using the density-matrix renormalization group, we calculate how the locations of phase transitions change with increasing dipolar interaction strength for average density ρ =1 . Furthermore, we show the emergence of pair-correlated phases for a large dipolar interaction strength and ρ ≥2 , including a supersolid phase with an incommensurate density wave ordering manifesting the corresponding spontaneous breaking of the translational symmetry.

Collision cross sections of N2 by H+ impact at keV energies within time-dependent density-functional theory

NASA Astrophysics Data System (ADS)

Yu, W.; Gao, C.-Z.; Zhang, Y.; Zhang, F. S.; Hutton, R.; Zou, Y.; Wei, B.

2018-03-01

We calculate electron capture and ionization cross sections of N2 impacted by the H+ projectile at keV energies. To this end, we employ the time-dependent density-functional theory coupled nonadiabatically to molecular dynamics. To avoid the explicit treatment of the complex density matrix in the calculation of cross sections, we propose an approximate method based on the assumption of constant ionization rate over the period of the projectile passing the absorbing boundary. Our results agree reasonably well with experimental data and semi-empirical results within the measurement uncertainties in the considered energy range. The discrepancies are mainly attributed to the inadequate description of exchange-correlation functional and the crude approximation for constant ionization rate. Although the present approach does not predict the experiments quantitatively for collision energies below 10 keV, it is still helpful to calculate total cross sections of ion-molecule collisions within a certain energy range.

Experiment and density functional theory analyses of GdTaO4 single crystal

NASA Astrophysics Data System (ADS)

Ding, Shoujun; Kinross, Ashlie; Wang, Xiaofei; Yang, Huajun; Zhang, Qingli; Liu, Wenpeng; Sun, Dunlu

2018-05-01

GdTaO4 is a type of excellent materials that can be used as scintillation, laser matrix as well as self-activated phosphor has generated significant interest. Whereas its band structure, electronic structure and optical properties are still need elucidation. To solve this intriguing problem, high-quality GdTaO4 single crystal (M-type) was grown successfully using Czochralski method. Its structure as well as optical properties was determined in experiment. Moreover, a systematic theoretical calculation based on the density function theory methods were performed on M-type and M‧-type GdTaO4 and their band structure, density of state as well as optical properties were obtained. Combine with the performed experiment results, the calculated results were proved with high reliability. Hence, the calculated results obtained in this work could provide a deep understanding of GdTaO4 material, which also useful for the further investigation on GdTaO4 material.

Entanglement classification in the noninteracting Fermi gas

NASA Astrophysics Data System (ADS)

Jafarizadeh, M. A.; Eghbalifam, F.; Nami, S.; Yahyavi, M.

In this paper, entanglement classification shared among the spins of localized fermions in the noninteracting Fermi gas is studied. It is proven that the Fermi gas density matrix is block diagonal on the basis of the projection operators to the irreducible representations of symmetric group Sn. Every block of density matrix is in the form of the direct product of a matrix and identity matrix. Then it is useful to study entanglement in every block of density matrix separately. The basis of corresponding Hilbert space are identified from the Schur-Weyl duality theorem. Also, it can be shown that the symmetric part of the density matrix is fully separable. Then it has been shown that the entanglement measure which is introduced in Eltschka et al. [New J. Phys. 10, 043104 (2008)] and Guhne et al. [New J. Phys. 7, 229 (2005)], is zero for the even n qubit Fermi gas density matrix. Then by focusing on three spin reduced density matrix, the entanglement classes have been investigated. In three qubit states there is an entanglement measure which is called 3-tangle. It can be shown that 3-tangle is zero for three qubit density matrix, but the density matrix is not biseparable for all possible values of its parameters and its eigenvectors are in the form of W-states. Then an entanglement witness for detecting non-separable state and an entanglement witness for detecting nonbiseparable states, have been introduced for three qubit density matrix by using convex optimization problem. Finally, the four spin reduced density matrix has been investigated by restricting the density matrix to the irreducible representations of Sn. The restricted density matrix to the subspaces of the irreducible representations: Ssym, S3,1 and S2,2 are denoted by ρsym, ρ3,1 and ρ2,2, respectively. It has been shown that some highly entangled classes (by using the results of Miyake [Phys. Rev. A 67, 012108 (2003)] for entanglement classification) do not exist in the blocks of density matrix ρ3,1 and ρ2,2, so these classes do not exist in the total Fermi gas density matrix.

SevenOperators, a Mathematica script for harmonic oscillator nuclear matrix elements arising in semileptonic electroweak interactions

NASA Astrophysics Data System (ADS)

Haxton, Wick; Lunardini, Cecilia

2008-09-01

Semi-leptonic electroweak interactions in nuclei—such as β decay, μ capture, charged- and neutral-current neutrino reactions, and electron scattering—are described by a set of multipole operators carrying definite parity and angular momentum, obtained by projection from the underlying nuclear charge and three-current operators. If these nuclear operators are approximated by their one-body forms and expanded in the nucleon velocity through order |p→|/M, where p→ and M are the nucleon momentum and mass, a set of seven multipole operators is obtained. Nuclear structure calculations are often performed in a basis of Slater determinants formed from harmonic oscillator orbitals, a choice that allows translational invariance to be preserved. Harmonic-oscillator single-particle matrix elements of the multipole operators can be evaluated analytically and expressed in terms of finite polynomials in q, where q is the magnitude of the three-momentum transfer. While results for such matrix elements are available in tabular form, with certain restriction on quantum numbers, the task of determining the analytic form of a response function can still be quite tedious, requiring the folding of the tabulated matrix elements with the nuclear density matrix, and subsequent algebra to evaluate products of operators. Here we provide a Mathematica script for generating these matrix elements, which will allow users to carry out all such calculations by symbolic manipulation. This will eliminate the errors that may accompany hand calculations and speed the calculation of electroweak nuclear cross sections and rates. We illustrate the use of the new script by calculating the cross sections for charged- and neutral-current neutrino scattering in 12C. Program summaryProgram title: SevenOperators Catalogue identifier: AEAY_v1_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEAY_v1_0.html Program obtainable from: CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions: Standard CPC licence, http://cpc.cs.qub.ac.uk/licence/licence.html No. of lines in distributed program, including test data, etc.: 2227 No. of bytes in distributed program, including test data, etc.: 19 382 Distribution format: tar.gz Programming language: Mathematica Computer: Any computer running Mathematica; tested on Mac OS X PowerPC (32-bit) running Mathematica 6.0.0 Operating system: Any running Mathematica RAM: Memory requirements determined by Mathematica; 512 MB or greater RAM and hard drive space of at least 3.0 GB recommended Classification: 17.16, 17.19 Nature of problem: Algebraic evaluation of harmonic oscillator nuclear matrix elements for the one-body multipole operators governing semi-leptonic weak interactions, such as charged- or neutral-current neutrino scattering off nuclei. Solution method: Mathematica evaluation of associated angular momentum algebra and spherical Bessel function radial integrals. Running time: Depends on the complexity of the one-body density matrix employed, but times of a few seconds are typical.

Coherent Microwave Scattering Model of Marsh Grass

NASA Astrophysics Data System (ADS)

Duan, Xueyang; Jones, Cathleen E.

2017-12-01

In this work, we developed an electromagnetic scattering model to analyze radar scattering from tall-grass-covered lands such as wetlands and marshes. The model adopts the generalized iterative extended boundary condition method (GIEBCM) algorithm, previously developed for buried cylindrical media such as vegetation roots, to simulate the scattering from the grass layer. The major challenge of applying GIEBCM to tall grass is the extremely time-consuming iteration among the large number of short subcylinders building up the grass. To overcome this issue, we extended the GIEBCM to multilevel GIEBCM, or M-GIEBCM, in which we first use GIEBCM to calculate a T matrix (transition matrix) database of "straws" with various lengths, thicknesses, orientations, curvatures, and dielectric properties; we then construct the grass with a group of straws from the database and apply GIEBCM again to calculate the T matrix of the overall grass scene. The grass T matrix is transferred to S matrix (scattering matrix) and combined with the ground S matrix, which is computed using the stabilized extended boundary condition method, to obtain the total scattering. In this article, we will demonstrate the capability of the model by simulating scattering from scenes with different grass densities, different grass structures, different grass water contents, and different ground moisture contents. This model will help with radar experiment design and image interpretation for marshland and wetland observations.

Electron density diagnostics for gaseous nebulae involving the O 4 intercombination lines near 1400 A

NASA Technical Reports Server (NTRS)

Keenan, F. P.; Conlon, E. S.; Bowden, D. A.; Feibelman, W. A.; Pradhan, Anil K.

1992-01-01

Theoretical O IV electron density sensitive emission line ratios, determined using electron impact excitation rates calculated with the R-matrix code, are presented for R(sub 1) = I(1407.4 A)/I(1401.2 A), R(sub 2) = I(1404.8 A)/I(1401.2A), R(sub 3) = I(1399.8 A)/(1401.2 A), and R(sub 4) = I(1397.2 A)/I(1401.2 A). The observed values of R(sub 1)-R(sub 4), measured from high resolution spectra obtained with the International Ultraviolet Explorer (IUE) satellite, lead to electron densities that are compatible, and which are also in good agreement with those deduced from line ratios in other species. This provides observational support for the accuracy of the atomic data adopted in the present calculations.

The initiation and growth of delaminations induced by matrix microcracks in laminated composites

NASA Technical Reports Server (NTRS)

Nairn, J. A.; Hu, S.

1992-01-01

A recent variational mechanics analysis of microcracking damage in cross-ply laminates of the form /(S)/90n/s, where (S) is any orthotropic sublaminate much stiffer than /90n/, has been extended to account for the presence of delaminations emanating from the tips of microcracks in the /90 2n/T sublaminate. The new two-dimensional stress analysis is used to calculate the total strain energy, effective modulus, and longitudinal thermal expansion coefficient for a laminate having microcracks and delaminations. These results are used to calculate the energy release rate for the initiation and growth of a delamination induced by a matrix microcrack. At low crack densities, /(S)/90n/s laminates are expected to fail by microcracking and to show little or no delamination. At some critical crack density, which is a function of laminate structure and material properties, the energy release rate for delamination exceeds that for microcracking and delamination is predicted to dominate over microcracking. A quasi-three-dimensional model is used to predict the propagation of arbitrarily shaped delamination fronts. All predictions agree with experimental observations.

The density matrix method in photonic bandgap and antiferromagnetic materials

NASA Astrophysics Data System (ADS)

Barrie, Scott B.

In this thesis, a theory for dispersive polaritonic bandgap (DPBG) and photonic bandgap (PBG) materials is developed. An ensemble of multi-level nanoparticles, such as non-interacting two-, three- and four-level atoms doped in DPBG and PBG materials is considered. The optical properties of these materials such as spontaneous emission, line broadening, fluorescence and narrowing of the natural linewidth have been studied using the density matrix method. Numerical simulations for these properties have been performed for the DPBG materials SiC and InAs, and for a PBG material with a 20 percent gap-to-midgap ratio. When a three-level nanoparticle is doped into a DPBG material, it is predicted that one or two bound states exist when one or both resonance energies, respectively, lie in the bandgap. It is shown when a resonance energy lies below the bandgap, its spectral density peak weakens and broadens as the resonance energy increases to the lower band edge. For the first time it is predicted that when a nanoparticle's resonance energy lies above the bandgap, its spectral density peak weakens and broadens as the resonance energy increases. A relation is also found between spectral structure and gap-to-midgap ratios. The dressed states of a two-level atom doped into a DPBG material under the influence of an intense monochromatic laser field are examined. The splitting of the dressed state energies is calculated, and it is predicted that the splitting depends on the polariton density of states and the Rabi frequency of laser field. The fluoresence is also examined, and for the first time two distinct control processes are found for the transition from one peak to three peaks. It was previously known that the Rabi frequency controlled the Stark effect, but this thesis predicts that the local of the peak with respect to the optical bandgap can cause a transition from one to three peaks even with a weak Rabi frequency. The transient linewidth narrowing of PBG crystal emission peaks doped with four-level atoms is studied. It is found that linewidth narrowing is only dependent upon time delay when the resonance energy is not near a band edge. This is a new discovery. The density matrix method is employed to find the critical magnetic field at which spin flopping occurs in antiferromagnetic high temperature superconductors. It is found that this magnetic field depends upon the temperature, the anisotropy parameter and the doping concentration. Results are calculated for 1-2-3 HTSCs. Keywords. Quantum Optics, Density Matrix, Photonic Bandgap Materials, Dispersive Polaritonic Bandgap Materials, Antiferromagnets.

The multifacet graphically contracted function method. I. Formulation and implementation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shepard, Ron; Brozell, Scott R.; Gidofalvi, Gergely

2014-08-14

The basic formulation for the multifacet generalization of the graphically contracted function (MFGCF) electronic structure method is presented. The analysis includes the discussion of linear dependency and redundancy of the arc factor parameters, the computation of reduced density matrices, Hamiltonian matrix construction, spin-density matrix construction, the computation of optimization gradients for single-state and state-averaged calculations, graphical wave function analysis, and the efficient computation of configuration state function and Slater determinant expansion coefficients. Timings are given for Hamiltonian matrix element and analytic optimization gradient computations for a range of model problems for full-CI Shavitt graphs, and it is observed that bothmore » the energy and the gradient computation scale as O(N{sup 2}n{sup 4}) for N electrons and n orbitals. The important arithmetic operations are within dense matrix-matrix product computational kernels, resulting in a computationally efficient procedure. An initial implementation of the method is used to present applications to several challenging chemical systems, including N{sub 2} dissociation, cubic H{sub 8} dissociation, the symmetric dissociation of H{sub 2}O, and the insertion of Be into H{sub 2}. The results are compared to the exact full-CI values and also to those of the previous single-facet GCF expansion form.« less

AFM-porosimetry: density and pore volume measurements of particulate materials.

PubMed

Sörensen, Malin H; Valle-Delgado, Juan J; Corkery, Robert W; Rutland, Mark W; Alberius, Peter C

2008-06-01

We introduced the novel technique of AFM-porosimetry and applied it to measure the total pore volume of porous particles with a spherical geometry. The methodology is based on using an atomic force microscope as a balance to measure masses of individual particles. Several particles within the same batch were measured, and by plotting particle mass versus particle volume, the bulk density of the sample can be extracted from the slope of the linear fit. The pore volume is then calculated from the densities of the bulk and matrix materials, respectively. In contrast to nitrogen sorption and mercury porosimetry, this method is capable of measuring the total pore volume regardless of pore size distribution and pore connectivity. In this study, three porous samples were investigated by AFM-porosimetry: one ordered mesoporous sample and two disordered foam structures. All samples were based on a matrix of amorphous silica templated by a block copolymer, Pluronic F127, swollen to various degrees with poly(propylene glycol). In addition, the density of silica spheres without a template was measured by two independent techniques: AFM and the Archimedes principle.

Ultrafast Saturation of Electronic-Resonance-Enhanced Coherent Anti-Stokes Raman Scattering and Comparison for Pulse Durations in the Nanosecond to Femtosecond Regime

DTIC Science & Technology

2016-02-05

electronic-resonance-enhanced CARS (ERE- CARS ) configuration is calculated. We demonstrate that while underdamping condition is a suffi- cient condition for...saturation of ERE- CARS with the long-pulse excitations, a transient-gain must be achieved to saturate ERE- CARS signal for ultrafast probe regime. We...ultrafast ERE- CARS . From a simplified analytical solution and a detailed numerical calculation based on density-matrix equations, the saturation threshold

Quantum Theory of Jaynes' Principle, Bayes' Theorem, and Information

NASA Astrophysics Data System (ADS)

Haken, Hermann

2014-12-01

After a reminder of Jaynes' maximum entropy principle and of my quantum theoretical extension, I consider two coupled quantum systems A,B and formulate a quantum version of Bayes' theorem. The application of Feynman's disentangling theorem allows me to calculate the conditional density matrix ρ (A|B) , if system A is an oscillator (or a set of them), linearly coupled to an arbitrary quantum system B. Expectation values can simply be calculated by means of the normalization factor of ρ (A|B) that is derived.

Extending density functional embedding theory for covalently bonded systems.

PubMed

Yu, Kuang; Carter, Emily A

2017-12-19

Quantum embedding theory aims to provide an efficient solution to obtain accurate electronic energies for systems too large for full-scale, high-level quantum calculations. It adopts a hierarchical approach that divides the total system into a small embedded region and a larger environment, using different levels of theory to describe each part. Previously, we developed a density-based quantum embedding theory called density functional embedding theory (DFET), which achieved considerable success in metals and semiconductors. In this work, we extend DFET into a density-matrix-based nonlocal form, enabling DFET to study the stronger quantum couplings between covalently bonded subsystems. We name this theory density-matrix functional embedding theory (DMFET), and we demonstrate its performance in several test examples that resemble various real applications in both chemistry and biochemistry. DMFET gives excellent results in all cases tested thus far, including predicting isomerization energies, proton transfer energies, and highest occupied molecular orbital-lowest unoccupied molecular orbital gaps for local chromophores. Here, we show that DMFET systematically improves the quality of the results compared with the widely used state-of-the-art methods, such as the simple capped cluster model or the widely used ONIOM method.

Charge-transfer contributions to the excitonic coupling matrix element in BODIPY-based energy transfer cassettes

NASA Astrophysics Data System (ADS)

Spiegel, J. Dominik; Lyskov, Igor; Kleinschmidt, Martin; Marian, Christel M.

2017-01-01

BODIPY-based dyads serve as model systems for the investigation of excitation energy transfer (EET). Through-space EET is brought about by direct and exchange interactions between the transition densities of donor and acceptor localized states. The presence of a molecular linker gives rise to additional charge transfer (CT) contributions. Here, we present a novel approach for the calculation of the excitonic coupling matrix element (ECME) including CT contributions which is based on supermolecular one-electron transition density matrices (STD). The validity of the approach is assessed for a model system of two π -stacked ethylene molecules at varying intermolecular separation. Wave functions and electronic excitation energies of five EET cassettes comprising anthracene as exciton donor and BODIPY as exciton acceptor are obtained by the redesigned combined density functional theory and multireference configuration interaction (DFT/MRCI-R) method. CT contributions to the ECME are shown to be important in the covalently linked EET cassettes.

Linear-scaling implementation of molecular response theory in self-consistent field electronic-structure theory.

PubMed

Coriani, Sonia; Høst, Stinne; Jansík, Branislav; Thøgersen, Lea; Olsen, Jeppe; Jørgensen, Poul; Reine, Simen; Pawłowski, Filip; Helgaker, Trygve; Sałek, Paweł

2007-04-21

A linear-scaling implementation of Hartree-Fock and Kohn-Sham self-consistent field theories for the calculation of frequency-dependent molecular response properties and excitation energies is presented, based on a nonredundant exponential parametrization of the one-electron density matrix in the atomic-orbital basis, avoiding the use of canonical orbitals. The response equations are solved iteratively, by an atomic-orbital subspace method equivalent to that of molecular-orbital theory. Important features of the subspace method are the use of paired trial vectors (to preserve the algebraic structure of the response equations), a nondiagonal preconditioner (for rapid convergence), and the generation of good initial guesses (for robust solution). As a result, the performance of the iterative method is the same as in canonical molecular-orbital theory, with five to ten iterations needed for convergence. As in traditional direct Hartree-Fock and Kohn-Sham theories, the calculations are dominated by the construction of the effective Fock/Kohn-Sham matrix, once in each iteration. Linear complexity is achieved by using sparse-matrix algebra, as illustrated in calculations of excitation energies and frequency-dependent polarizabilities of polyalanine peptides containing up to 1400 atoms.

Density matrix solutions for the susceptibilities of a three-level system with arbitrary relaxation rates and field strengths

NASA Technical Reports Server (NTRS)

Ryan, J. C.; Lawandy, N. M.

1986-01-01

The susceptibilities for a three-level system with arbitrary pump and signal field strengths are derived for arbitrary longitudinal and transverse relaxation rates. The results are of interest in connection with the calculation of the Raman gain in systems where resonance enhancement plays a dominant role.

Effects of bending on the superconducting critical current density of monofilamentary Nb3Sn wires

NASA Astrophysics Data System (ADS)

Kaiho, K.; Luhman, T. S.; Suenaga, M.; Sampson, W. B.

1980-02-01

Variations in the superconducting current density Jc of the Nb3Sn wires upon bending were measured for a series of monofilamentary wires in which the ratio Rv of the matrix (Cu+Sn) to the core (Nb3Sn,Nb) was changed from 0 to 58. In most cases Jc was found to increase slightly until the bending strain exceeded a value of ɛirrB , beyond which it severely and irreversibly degraded. For wires with intermediate values of Rv (˜2 to 10), ɛirrB , calculated by geometrical considerations, was substantially lower than the measured value of the tensile strain ɛirrT which was required to irreversibly degrade the critical current. The influence of bending strains on Jc can qualitatively be described by considering residual prestrains in the matrix and the core.

Simulation of Particle Size Effect on Dynamic Properties and Fracture of PTFE-W-Al Composites

NASA Astrophysics Data System (ADS)

Herbold, E. B.; Cai, J.; Benson, D. J.; Nesterenko, V. F.

2007-12-01

Recent investigations of the dynamic compressive strength of cold isostatically pressed composites of polytetrafluoroethylene (PTFE), tungsten (W) and aluminum (Al) powders show significant differences depending on the size of metallic particles. The addition of W increases the density and changes the overall strength of the sample depending on the size of W particles. To investigate relatively large deformations, multi-material Eulerian and arbitrary Lagrangian-Eulerian methods, which have the ability to efficiently handle the formation of free surfaces, were used. The calculations indicate that the increased sample strength with fine metallic particles is due to the dynamic formation of force chains. This phenomenon occurs for samples with a higher porosity of the PTFE matrix compared to samples with larger particle size of W and a higher density PTFE matrix.

Microscopically based energy density functionals for nuclei using the density matrix expansion. II. Full optimization and validation

NASA Astrophysics Data System (ADS)

Navarro Pérez, R.; Schunck, N.; Dyhdalo, A.; Furnstahl, R. J.; Bogner, S. K.

2018-05-01

Background: Energy density functional methods provide a generic framework to compute properties of atomic nuclei starting from models of nuclear potentials and the rules of quantum mechanics. Until now, the overwhelming majority of functionals have been constructed either from empirical nuclear potentials such as the Skyrme or Gogny forces, or from systematic gradient-like expansions in the spirit of the density functional theory for atoms. Purpose: We seek to obtain a usable form of the nuclear energy density functional that is rooted in the modern theory of nuclear forces. We thus consider a functional obtained from the density matrix expansion of local nuclear potentials from chiral effective field theory. We propose a parametrization of this functional carefully calibrated and validated on selected ground-state properties that is suitable for large-scale calculations of nuclear properties. Methods: Our energy functional comprises two main components. The first component is a non-local functional of the density and corresponds to the direct part (Hartree term) of the expectation value of local chiral potentials on a Slater determinant. Contributions to the mean field and the energy of this term are computed by expanding the spatial, finite-range components of the chiral potential onto Gaussian functions. The second component is a local functional of the density and is obtained by applying the density matrix expansion to the exchange part (Fock term) of the expectation value of the local chiral potential. We apply the UNEDF2 optimization protocol to determine the coupling constants of this energy functional. Results: We obtain a set of microscopically constrained functionals for local chiral potentials from leading order up to next-to-next-to-leading order with and without three-body forces and contributions from Δ excitations. These functionals are validated on the calculation of nuclear and neutron matter, nuclear mass tables, single-particle shell structure in closed-shell nuclei, and the fission barrier of 240Pu. Quantitatively, they perform noticeably better than the more phenomenological Skyrme functionals. Conclusions: The inclusion of higher-order terms in the chiral perturbation expansion seems to produce a systematic improvement in predicting nuclear binding energies while the impact on other observables is not really significant. This result is especially promising since all the fits have been performed at the single-reference level of the energy density functional approach, where important collective correlations such as center-of-mass correction, rotational correction, or zero-point vibrational energies have not been taken into account yet.

Grid-free density functional calculations on periodic systems.

PubMed

Varga, Stefan

2007-09-21

Density fitting scheme is applied to the exchange part of the Kohn-Sham potential matrix in a grid-free local density approximation for infinite systems with translational periodicity. It is shown that within this approach the computational demands for the exchange part scale in the same way as for the Coulomb part. The efficiency of the scheme is demonstrated on a model infinite polymer chain. For simplicity, the implementation with Dirac-Slater Xalpha exchange functional is presented only. Several choices of auxiliary basis set expansion coefficients were tested with both Coulomb and overlap metric. Their effectiveness is discussed also in terms of robustness and norm preservation.

Grid-free density functional calculations on periodic systems

NASA Astrophysics Data System (ADS)

Varga, Štefan

2007-09-01

Density fitting scheme is applied to the exchange part of the Kohn-Sham potential matrix in a grid-free local density approximation for infinite systems with translational periodicity. It is shown that within this approach the computational demands for the exchange part scale in the same way as for the Coulomb part. The efficiency of the scheme is demonstrated on a model infinite polymer chain. For simplicity, the implementation with Dirac-Slater Xα exchange functional is presented only. Several choices of auxiliary basis set expansion coefficients were tested with both Coulomb and overlap metric. Their effectiveness is discussed also in terms of robustness and norm preservation.

Harnessing molecular excited states with Lanczos chains.

PubMed

Baroni, Stefano; Gebauer, Ralph; Bariş Malcioğlu, O; Saad, Yousef; Umari, Paolo; Xian, Jiawei

2010-02-24

The recursion method of Haydock, Heine and Kelly is a powerful tool for calculating diagonal matrix elements of the resolvent of quantum-mechanical Hamiltonian operators by elegantly expressing them in terms of continued fractions. In this paper we extend the recursion method to off-diagonal matrix elements of general (possibly non-Hermitian) operators and apply it to the simulation of molecular optical absorption and photoemission spectra within time-dependent density-functional and many-body perturbation theories, respectively. This method is demonstrated with a couple of applications to the optical absorption and photoemission spectra of the caffeine molecule.

Harnessing molecular excited states with Lanczos chains

NASA Astrophysics Data System (ADS)

Baroni, Stefano; Gebauer, Ralph; Bariş Malcioğlu, O.; Saad, Yousef; Umari, Paolo; Xian, Jiawei

2010-02-01

The recursion method of Haydock, Heine and Kelly is a powerful tool for calculating diagonal matrix elements of the resolvent of quantum-mechanical Hamiltonian operators by elegantly expressing them in terms of continued fractions. In this paper we extend the recursion method to off-diagonal matrix elements of general (possibly non-Hermitian) operators and apply it to the simulation of molecular optical absorption and photoemission spectra within time-dependent density-functional and many-body perturbation theories, respectively. This method is demonstrated with a couple of applications to the optical absorption and photoemission spectra of the caffeine molecule.

Linear scaling computation of the Fock matrix. VI. Data parallel computation of the exchange-correlation matrix

NASA Astrophysics Data System (ADS)

Gan, Chee Kwan; Challacombe, Matt

2003-05-01

Recently, early onset linear scaling computation of the exchange-correlation matrix has been achieved using hierarchical cubature [J. Chem. Phys. 113, 10037 (2000)]. Hierarchical cubature differs from other methods in that the integration grid is adaptive and purely Cartesian, which allows for a straightforward domain decomposition in parallel computations; the volume enclosing the entire grid may be simply divided into a number of nonoverlapping boxes. In our data parallel approach, each box requires only a fraction of the total density to perform the necessary numerical integrations due to the finite extent of Gaussian-orbital basis sets. This inherent data locality may be exploited to reduce communications between processors as well as to avoid memory and copy overheads associated with data replication. Although the hierarchical cubature grid is Cartesian, naive boxing leads to irregular work loads due to strong spatial variations of the grid and the electron density. In this paper we describe equal time partitioning, which employs time measurement of the smallest sub-volumes (corresponding to the primitive cubature rule) to load balance grid-work for the next self-consistent-field iteration. After start-up from a heuristic center of mass partitioning, equal time partitioning exploits smooth variation of the density and grid between iterations to achieve load balance. With the 3-21G basis set and a medium quality grid, equal time partitioning applied to taxol (62 heavy atoms) attained a speedup of 61 out of 64 processors, while for a 110 molecule water cluster at standard density it achieved a speedup of 113 out of 128. The efficiency of equal time partitioning applied to hierarchical cubature improves as the grid work per processor increases. With a fine grid and the 6-311G(df,p) basis set, calculations on the 26 atom molecule α-pinene achieved a parallel efficiency better than 99% with 64 processors. For more coarse grained calculations, superlinear speedups are found to result from reduced computational complexity associated with data parallelism.

Infrared spectroscopy and density functional calculations on titanium-dinitrogen complexes

NASA Astrophysics Data System (ADS)

Yoo, Hae-Wook; Choi, Changhyeok; Cho, Soo Gyeong; Jung, Yousung; Choi, Myong Yong

2018-04-01

Titanium-nitrogen complexes were generated by laser ablated titanium (Ti) atoms and N2 gas molecules in this study. These complexes were isolated on the pre-deposited solid Ar matrix on the pre-cooled KBr window (T ∼ 5.4 K), allowing infrared spectra to be measured. Laser ablation experiments with 15N2 isotope provided distinct isotopic shifts in the infrared spectra that strongly implicated the formation of titanium-nitrogen complexes, Ti(NN)x. Density functional theory (DFT) calculations were employed to investigate the molecular structures, electronic ground state, relative energies, and IR frequencies of the anticipated Ti(NN)x complexes. Based on laser ablation experiments and DFT calculations, we were able to assign multiple Ti(NN)x (x = 1-6) species. Particularly, Ti(NN)5 and Ti(NN)6, which have high nitrogen content, may serve as good precursors in preparing polynitrogens.

Estimates of Stellar Weak Interaction Rates for Nuclei in the Mass Range A=65-80

NASA Astrophysics Data System (ADS)

Pruet, Jason; Fuller, George M.

2003-11-01

We estimate lepton capture and emission rates, as well as neutrino energy loss rates, for nuclei in the mass range A=65-80. These rates are calculated on a temperature/density grid appropriate for a wide range of astrophysical applications including simulations of late time stellar evolution and X-ray bursts. The basic inputs in our single-particle and empirically inspired model are (i) experimentally measured level information, weak transition matrix elements, and lifetimes, (ii) estimates of matrix elements for allowed experimentally unmeasured transitions based on the systematics of experimentally observed allowed transitions, and (iii) estimates of the centroids of the GT resonances motivated by shell model calculations in the fp shell as well as by (n, p) and (p, n) experiments. Fermi resonances (isobaric analog states) are also included, and it is shown that Fermi transitions dominate the rates for most interesting proton-rich nuclei for which an experimentally determined ground state lifetime is unavailable. For the purposes of comparing our results with more detailed shell model based calculations we also calculate weak rates for nuclei in the mass range A=60-65 for which Langanke & Martinez-Pinedo have provided rates. The typical deviation in the electron capture and β-decay rates for these ~30 nuclei is less than a factor of 2 or 3 for a wide range of temperature and density appropriate for presupernova stellar evolution. We also discuss some subtleties associated with the partition functions used in calculations of stellar weak rates and show that the proper treatment of the partition functions is essential for estimating high-temperature β-decay rates. In particular, we show that partition functions based on unconverged Lanczos calculations can result in errors in estimates of high-temperature β-decay rates.

Proceedings of Workshop on Atmospheric Density and Aerodynamic Drag Models for Air Force Operations Held at Air Force Geophysics Laboratory on 20-22 October 1987. Volume 1

DTIC Science & Technology

1990-02-13

considered with these production processes in a simple photochemical equilibrium calculation , we are able to determine the contribution each makes to the...Hessian matrix of second derivatives (which is required in the Newton-Raphson procedure) by the vector product of the gradient (VJ) and its transpose...was focused on the altitude region 80-250 Km. Papers were presented in the folowing areas: Air Force requirements , physics of density and drag

Ab initio calculation of resonant Raman intensities of transition metal dichalcogenides

NASA Astrophysics Data System (ADS)

Miranda, Henrique; Reichardt, Sven; Molina-Sanchez, Alejandro; Wirtz, Ludger

Raman spectroscopy is used to characterize optical and vibrational properties of materials. Its computational simulation is important for the interpretation of experimental results. Two approaches are the bond polarizability model and density functional perturbation theory. However, both are known to not capture resonance effects. These resonances and quantum interference effects are important to correctly reproduce the intensities as a function of laser energy as, e.g., reported for the case of multi-layer MoTe21.We present two fully ab initio approaches that overcome this limitation. In the first, we calculate finite difference derivatives of the dielectric susceptibility with the phonon displacements2. In the second we calculate electron-light and electron-phonon matrix elements from density functional theory and use them to evaluate expressions for the Raman intensity derived from time-dependent perturbation theory. These expressions are implemented in a computer code that performs the calculations as a post-processing step. We compare both methods and study the case of triple-layer MoTe2. Luxembourg National Research Fund (FNR).

Matrix isolation infrared spectra, assignment and DFT investigation on reactions of iron and manganese monoxides with CH3Cl.

PubMed

Zhao, Yanying; Fan, Kexue; Huang, Yongfei; Zheng, Xuming

2013-12-01

The reactions of iron and manganese monoxide molecules (FeO, and MnO) with monochloromethane in solid argon have been studied by matrix isolation infrared spectroscopy and quantum chemistry calculations. When annealing, the reactions of FeO and MnO with CH3Cl first form the OM-(η(Cl)-CH3Cl) (MMn, Fe) complexes, which can isomerize to CH3MOCl (MMn, Fe) upon 300<λ<580 nm irradiation. The products were characterized by isotopic IR studies with CD3Cl and (13)CH3Cl and density functional calculations. Based on theoretical calculations, the OFe-(η(Cl)-CH3Cl) and OMn-(η(Cl)-CH3Cl) complexes have (5)A' and (6)A' ground state with Cs symmetry, respectively. The accurate CCSD(T) single point calculations illustrate the CH3MOCl isomerism are 13.8 and 3.1 kcal/mol lower in energy than the OM-(η(Cl)-CH3Cl) (MMn, Fe) complexes. Copyright © 2013 The Authors. Published by Elsevier B.V. All rights reserved.

Tautomerism and infrared spectra of 2-thiopurine: an experimental matrix isolation and theoretical ab initio and density functional theory study

NASA Astrophysics Data System (ADS)

Stepanenko, Tetyana; Lapinski, Leszek; Nowak, Maciej J.; Kwiatkowski, Józef S.; Leszczynski, Jerzy

2001-02-01

Infrared spectra of 2-thiopurine (2-mercaptopurine, 2-purinethiol ) isolated in low-temperature Ar and N 2 matrixes are reported. These spectra indicate that the compound adopts exclusively the thiol N9H tautomeric form. The theoretical calculations of relative energies of 2-thiopurine tautomers have been carried out at the MP4(SDTQ)//HF level using the 6-31G( d, p) basis set. The thiol N9H tautomer was predicted to be the most stable of all isomers of 2-thiopurine. The infrared spectra of the tautomers of 2-thiopurine have been calculated at the DFT(B3LYP)/6-31G( d, p) level. Good agreement between the experimental spectra and the spectra calculated for thiol N9H tautomer supported the identification of the dominant tautomer. It has also allowed for the reliable assignment of the bands observed in the experimental IR spectrum.

Efficient calculation of beyond RPA correlation energies in the dielectric matrix formalism

NASA Astrophysics Data System (ADS)

Beuerle, Matthias; Graf, Daniel; Schurkus, Henry F.; Ochsenfeld, Christian

2018-05-01

We present efficient methods to calculate beyond random phase approximation (RPA) correlation energies for molecular systems with up to 500 atoms. To reduce the computational cost, we employ the resolution-of-the-identity and a double-Laplace transform of the non-interacting polarization propagator in conjunction with an atomic orbital formalism. Further improvements are achieved using integral screening and the introduction of Cholesky decomposed densities. Our methods are applicable to the dielectric matrix formalism of RPA including second-order screened exchange (RPA-SOSEX), the RPA electron-hole time-dependent Hartree-Fock (RPA-eh-TDHF) approximation, and RPA renormalized perturbation theory using an approximate exchange kernel (RPA-AXK). We give an application of our methodology by presenting RPA-SOSEX benchmark results for the L7 test set of large, dispersion dominated molecules, yielding a mean absolute error below 1 kcal/mol. The present work enables calculating beyond RPA correlation energies for significantly larger molecules than possible to date, thereby extending the applicability of these methods to a wider range of chemical systems.

An accurate and linear-scaling method for calculating charge-transfer excitation energies and diabatic couplings

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pavanello, Michele; Van Voorhis, Troy; Visscher, Lucas

2013-02-07

Quantum-mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those charge transfer excitations that take place between non-covalently bound molecules. In particular, we present a method that scales linearly with the number of non-covalently bound molecules in the system and is based on a two-pronged approach: The molecular electronic structure of broken-symmetry charge-localized states is obtained with the frozen density embedding formulation of subsystem density-functional theory; subsequently, in a post-SCF calculation, the full-electron Hamiltonian and overlapmore » matrix elements among the charge-localized states are evaluated with an algorithm which takes full advantage of the subsystem DFT density partitioning technique. The method is benchmarked against coupled-cluster calculations and achieves chemical accuracy for the systems considered for intermolecular separations ranging from hydrogen-bond distances to tens of Angstroms. Numerical examples are provided for molecular clusters comprised of up to 56 non-covalently bound molecules.« less

An accurate and linear-scaling method for calculating charge-transfer excitation energies and diabatic couplings.

PubMed

Pavanello, Michele; Van Voorhis, Troy; Visscher, Lucas; Neugebauer, Johannes

2013-02-07

Quantum-mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those charge transfer excitations that take place between non-covalently bound molecules. In particular, we present a method that scales linearly with the number of non-covalently bound molecules in the system and is based on a two-pronged approach: The molecular electronic structure of broken-symmetry charge-localized states is obtained with the frozen density embedding formulation of subsystem density-functional theory; subsequently, in a post-SCF calculation, the full-electron Hamiltonian and overlap matrix elements among the charge-localized states are evaluated with an algorithm which takes full advantage of the subsystem DFT density partitioning technique. The method is benchmarked against coupled-cluster calculations and achieves chemical accuracy for the systems considered for intermolecular separations ranging from hydrogen-bond distances to tens of Ångstroms. Numerical examples are provided for molecular clusters comprised of up to 56 non-covalently bound molecules.

Spectroscopic accuracy directly from quantum chemistry: application to ground and excited states of beryllium dimer.

PubMed

Sharma, Sandeep; Yanai, Takeshi; Booth, George H; Umrigar, C J; Chan, Garnet Kin-Lic

2014-03-14

We combine explicit correlation via the canonical transcorrelation approach with the density matrix renormalization group and initiator full configuration interaction quantum Monte Carlo methods to compute a near-exact beryllium dimer curve, without the use of composite methods. In particular, our direct density matrix renormalization group calculations produce a well-depth of D(e) = 931.2 cm(-1) which agrees very well with recent experimentally derived estimates D(e) = 929.7±2 cm(-1) [J. M. Merritt, V. E. Bondybey, and M. C. Heaven, Science 324, 1548 (2009)] and D(e) = 934.6 cm(-1) [K. Patkowski, V. Špirko, and K. Szalewicz, Science 326, 1382 (2009)], as well the best composite theoretical estimates, D(e) = 938±15 cm(-1) [K. Patkowski, R. Podeszwa, and K. Szalewicz, J. Phys. Chem. A 111, 12822 (2007)] and D(e) = 935.1±10 cm(-1) [J. Koput, Phys. Chem. Chem. Phys. 13, 20311 (2011)]. Our results suggest possible inaccuracies in the functional form of the potential used at shorter bond lengths to fit the experimental data [J. M. Merritt, V. E. Bondybey, and M. C. Heaven, Science 324, 1548 (2009)]. With the density matrix renormalization group we also compute near-exact vertical excitation energies at the equilibrium geometry. These provide non-trivial benchmarks for quantum chemical methods for excited states, and illustrate the surprisingly large error that remains for 1 ¹Σ(g)⁻ state with approximate multi-reference configuration interaction and equation-of-motion coupled cluster methods. Overall, we demonstrate that explicitly correlated density matrix renormalization group and initiator full configuration interaction quantum Monte Carlo methods allow us to fully converge to the basis set and correlation limit of the non-relativistic Schrödinger equation in small molecules.

Path Integrals for Electronic Densities, Reactivity Indices, and Localization Functions in Quantum Systems

PubMed Central

Putz, Mihai V.

2009-01-01

The density matrix theory, the ancestor of density functional theory, provides the immediate framework for Path Integral (PI) development, allowing the canonical density be extended for the many-electronic systems through the density functional closure relationship. Yet, the use of path integral formalism for electronic density prescription presents several advantages: assures the inner quantum mechanical description of the system by parameterized paths; averages the quantum fluctuations; behaves as the propagator for time-space evolution of quantum information; resembles Schrödinger equation; allows quantum statistical description of the system through partition function computing. In this framework, four levels of path integral formalism were presented: the Feynman quantum mechanical, the semiclassical, the Feynman-Kleinert effective classical, and the Fokker-Planck non-equilibrium ones. In each case the density matrix or/and the canonical density were rigorously defined and presented. The practical specializations for quantum free and harmonic motions, for statistical high and low temperature limits, the smearing justification for the Bohr’s quantum stability postulate with the paradigmatic Hydrogen atomic excursion, along the quantum chemical calculation of semiclassical electronegativity and hardness, of chemical action and Mulliken electronegativity, as well as by the Markovian generalizations of Becke-Edgecombe electronic focalization functions – all advocate for the reliability of assuming PI formalism of quantum mechanics as a versatile one, suited for analytically and/or computationally modeling of a variety of fundamental physical and chemical reactivity concepts characterizing the (density driving) many-electronic systems. PMID:20087467

Path integrals for electronic densities, reactivity indices, and localization functions in quantum systems.

PubMed

Putz, Mihai V

2009-11-10

The density matrix theory, the ancestor of density functional theory, provides the immediate framework for Path Integral (PI) development, allowing the canonical density be extended for the many-electronic systems through the density functional closure relationship. Yet, the use of path integral formalism for electronic density prescription presents several advantages: assures the inner quantum mechanical description of the system by parameterized paths; averages the quantum fluctuations; behaves as the propagator for time-space evolution of quantum information; resembles Schrödinger equation; allows quantum statistical description of the system through partition function computing. In this framework, four levels of path integral formalism were presented: the Feynman quantum mechanical, the semiclassical, the Feynman-Kleinert effective classical, and the Fokker-Planck non-equilibrium ones. In each case the density matrix or/and the canonical density were rigorously defined and presented. The practical specializations for quantum free and harmonic motions, for statistical high and low temperature limits, the smearing justification for the Bohr's quantum stability postulate with the paradigmatic Hydrogen atomic excursion, along the quantum chemical calculation of semiclassical electronegativity and hardness, of chemical action and Mulliken electronegativity, as well as by the Markovian generalizations of Becke-Edgecombe electronic focalization functions - all advocate for the reliability of assuming PI formalism of quantum mechanics as a versatile one, suited for analytically and/or computationally modeling of a variety of fundamental physical and chemical reactivity concepts characterizing the (density driving) many-electronic systems.

Anisotropy of the elastic properties of crystalline cellulose Iß from first principles density functional theory with Van der Waals interactions

Treesearch

Fernando L. Dri; Louis G. Jr. Hector; Robert J. Moon; Pablo D. Zavattieri

2013-01-01

In spite of the significant potential of cellulose nanocrystals as functional nanoparticles for numerous applications, a fundamental understanding of the mechanical properties of defect-free, crystalline cellulose is still lacking. In this paper, the elasticity matrix for cellulose Iß with hydrogen bonding network A was calculated using ab initio...

Mechanism for odd-electron anion generation of dihydroxybenzoic acid isomers in matrix-assisted laser desorption/ionization mass spectrometry with density functional theory calculations.

PubMed

Yamagaki, Tohru; Takeuchi, Michika; Watanabe, Takehiro; Sugahara, Kohtaro; Takeuchi, Takae

2016-12-30

Proton and radical are transferred between matrices and matrix and analyte in matrix-assisted laser desorption/ionization (MALDI) and these transfers drive ionization of analytes. The odd-electron anion [M-2H] •- was generated in dihydroxybenzoic acids (DHBs) and the ion abundance of the 2,5-DHB was the highest among six DHB isomers. We were interested in the mechanism of the ion generation of the odd-electron anion. The observed [M-2H] •- and [M-3H] - ions, which were generated with the hydrogen radical removed from the phenolic hydroxyl groups (OH) in DHB isomers, were analyzed using negative-ion MALDI-MS. The enthalpy for ion generation and their stable structures were calculated using the density functional theory (DFT) calculation program Gaussian 09 with the B3LYP functional and the 6-31+G(d) basis set. The number of observed [M-2H] •- and [M-3H] - ions of the DHB isomers was dependent on the positions of the phenolic OH groups in the DHB isomers because the carboxy group interacts with the ortho OH group due to neighboring group participation, as confirmed from the stable structures of the [M-2H] •- anions calculated with the Gaussian 09 program. The DHB isomers were placed into three categories according to the number of the ions. Odd-electron anions ([M-2H] •- ) and [M-2H • -H] - ([M-3H] - ) ions were generated from DHB isomers due to removal of the hydrogen radical from the phenolic groups. The enthalpy for ion generation revealed that ion formation proceeds via a two-step pathway through the [M-M] - ion as an intermediate. © 2016 The Authors. Rapid Communications in Mass Spectrometry Published by John Wiley & Sons Ltd. © 2016 The Authors. Rapid Communications in Mass Spectrometry Published by John Wiley & Sons Ltd.

Time-dependent density-functional tight-binding method with the third-order expansion of electron density

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nishimoto, Yoshio, E-mail: nishimoto.yoshio@fukui.kyoto-u.ac.jp

2015-09-07

We develop a formalism for the calculation of excitation energies and excited state gradients for the self-consistent-charge density-functional tight-binding method with the third-order contributions of a Taylor series of the density functional theory energy with respect to the fluctuation of electron density (time-dependent density-functional tight-binding (TD-DFTB3)). The formulation of the excitation energy is based on the existing time-dependent density functional theory and the older TD-DFTB2 formulae. The analytical gradient is computed by solving Z-vector equations, and it requires one to calculate the third-order derivative of the total energy with respect to density matrix elements due to the inclusion of themore » third-order contributions. The comparison of adiabatic excitation energies for selected small and medium-size molecules using the TD-DFTB2 and TD-DFTB3 methods shows that the inclusion of the third-order contributions does not affect excitation energies significantly. A different set of parameters, which are optimized for DFTB3, slightly improves the prediction of adiabatic excitation energies statistically. The application of TD-DFTB for the prediction of absorption and fluorescence energies of cresyl violet demonstrates that TD-DFTB3 reproduced the experimental fluorescence energy quite well.« less

Orbital stability close to asteroid 624 Hektor using the polyhedral model

NASA Astrophysics Data System (ADS)

Jiang, Yu; Baoyin, Hexi; Li, Hengnian

2018-03-01

We investigate the orbital stability close to the unique L4-point Jupiter binary Trojan asteroid 624 Hektor. The gravitational potential of 624 Hektor is calculated using the polyhedron model with observational data of 2038 faces and 1021 vertexes. Previous studies have presented three different density values for 624 Hektor. The equilibrium points in the gravitational potential of 624 Hektor with different density values have been studied in detail. There are five equilibrium points in the gravitational potential of 624 Hektor no matter the density value. The positions, Jacobian, eigenvalues, topological cases, stability, as well as the Hessian matrix of the equilibrium points are investigated. For the three different density values the number, topological cases, and the stability of the equilibrium points with different density values are the same. However, the positions of the equilibrium points vary with the density value of the asteroid 624 Hektor. The outer equilibrium points move away from the asteroid's mass center when the density increases, and the inner equilibrium point moves close to the asteroid's mass center when the density increases. There exist unstable periodic orbits near the surface of 624 Hektor. We calculated an orbit near the primary's equatorial plane of this binary Trojan asteroid; the results indicate that the orbit remains stable after 28.8375 d.

Time-dependent density-functional tight-binding method with the third-order expansion of electron density.

PubMed

Nishimoto, Yoshio

2015-09-07

We develop a formalism for the calculation of excitation energies and excited state gradients for the self-consistent-charge density-functional tight-binding method with the third-order contributions of a Taylor series of the density functional theory energy with respect to the fluctuation of electron density (time-dependent density-functional tight-binding (TD-DFTB3)). The formulation of the excitation energy is based on the existing time-dependent density functional theory and the older TD-DFTB2 formulae. The analytical gradient is computed by solving Z-vector equations, and it requires one to calculate the third-order derivative of the total energy with respect to density matrix elements due to the inclusion of the third-order contributions. The comparison of adiabatic excitation energies for selected small and medium-size molecules using the TD-DFTB2 and TD-DFTB3 methods shows that the inclusion of the third-order contributions does not affect excitation energies significantly. A different set of parameters, which are optimized for DFTB3, slightly improves the prediction of adiabatic excitation energies statistically. The application of TD-DFTB for the prediction of absorption and fluorescence energies of cresyl violet demonstrates that TD-DFTB3 reproduced the experimental fluorescence energy quite well.

Daubechies wavelets for linear scaling density functional theory.

PubMed

Mohr, Stephan; Ratcliff, Laura E; Boulanger, Paul; Genovese, Luigi; Caliste, Damien; Deutsch, Thierry; Goedecker, Stefan

2014-05-28

We demonstrate that Daubechies wavelets can be used to construct a minimal set of optimized localized adaptively contracted basis functions in which the Kohn-Sham orbitals can be represented with an arbitrarily high, controllable precision. Ground state energies and the forces acting on the ions can be calculated in this basis with the same accuracy as if they were calculated directly in a Daubechies wavelets basis, provided that the amplitude of these adaptively contracted basis functions is sufficiently small on the surface of the localization region, which is guaranteed by the optimization procedure described in this work. This approach reduces the computational costs of density functional theory calculations, and can be combined with sparse matrix algebra to obtain linear scaling with respect to the number of electrons in the system. Calculations on systems of 10,000 atoms or more thus become feasible in a systematic basis set with moderate computational resources. Further computational savings can be achieved by exploiting the similarity of the adaptively contracted basis functions for closely related environments, e.g., in geometry optimizations or combined calculations of neutral and charged systems.

Density-matrix simulation of small surface codes under current and projected experimental noise

NASA Astrophysics Data System (ADS)

O'Brien, T. E.; Tarasinski, B.; DiCarlo, L.

2017-09-01

We present a density-matrix simulation of the quantum memory and computing performance of the distance-3 logical qubit Surface-17, following a recently proposed quantum circuit and using experimental error parameters for transmon qubits in a planar circuit QED architecture. We use this simulation to optimize components of the QEC scheme (e.g., trading off stabilizer measurement infidelity for reduced cycle time) and to investigate the benefits of feedback harnessing the fundamental asymmetry of relaxation-dominated error in the constituent transmons. A lower-order approximate calculation extends these predictions to the distance-5 Surface-49. These results clearly indicate error rates below the fault-tolerance threshold of the surface code, and the potential for Surface-17 to perform beyond the break-even point of quantum memory. However, Surface-49 is required to surpass the break-even point of computation at state-of-the-art qubit relaxation times and readout speeds.

Drude weight of the spin-(1)/(2) XXZ chain: Density matrix renormalization group versus exact diagonalization

NASA Astrophysics Data System (ADS)

Karrasch, C.; Hauschild, J.; Langer, S.; Heidrich-Meisner, F.

2013-06-01

We revisit the problem of the spin Drude weight D of the integrable spin-1/2 XXZ chain using two complementary approaches, exact diagonalization (ED) and the time-dependent density-matrix renormalization group (tDMRG). We pursue two main goals. First, we present extensive results for the temperature dependence of D. By exploiting time translation invariance within tDMRG, one can extract D for significantly lower temperatures than in previous tDMRG studies. Second, we discuss the numerical quality of the tDMRG data and elaborate on details of the finite-size scaling of the ED results, comparing calculations carried out in the canonical and grand-canonical ensembles. Furthermore, we analyze the behavior of the Drude weight as the point with SU(2)-symmetric exchange is approached and discuss the relative contribution of the Drude weight to the sum rule as a function of temperature.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Theophilou, Iris; Helbig, Nicole; Lathiotakis, Nektarios N.

Functionals of the one-body reduced density matrix (1-RDM) are routinely minimized under Coleman’s ensemble N-representability conditions. Recently, the topic of pure-state N-representability conditions, also known as generalized Pauli constraints, received increased attention following the discovery of a systematic way to derive them for any number of electrons and any finite dimensionality of the Hilbert space. The target of this work is to assess the potential impact of the enforcement of the pure-state conditions on the results of reduced density-matrix functional theory calculations. In particular, we examine whether the standard minimization of typical 1-RDM functionals under the ensemble N-representability conditions violatesmore » the pure-state conditions for prototype 3-electron systems. We also enforce the pure-state conditions, in addition to the ensemble ones, for the same systems and functionals and compare the correlation energies and optimal occupation numbers with those obtained by the enforcement of the ensemble conditions alone.« less

Origin of terminal voltage variations due to self-mixing in terahertz frequency quantum cascade lasers.

PubMed

Grier, Andrew; Dean, Paul; Valavanis, Alexander; Keeley, James; Kundu, Iman; Cooper, Jonathan D; Agnew, Gary; Taimre, Thomas; Lim, Yah Leng; Bertling, Karl; Rakić, Aleksandar D; Li, Lianhe H; Harrison, Paul; Linfield, Edmund H; Ikonić, Zoran; Davies, A Giles; Indjin, Dragan

2016-09-19

We explain the origin of voltage variations due to self-mixing in a terahertz (THz) frequency quantum cascade laser (QCL) using an extended density matrix (DM) approach. Our DM model allows calculation of both the current-voltage (I-V) and optical power characteristics of the QCL under optical feedback by changing the cavity loss, to which the gain of the active region is clamped. The variation of intra-cavity field strength necessary to achieve gain clamping, and the corresponding change in bias required to maintain a constant current density through the heterostructure is then calculated. Strong enhancement of the self-mixing voltage signal due to non-linearity of the (I-V) characteristics is predicted and confirmed experimentally in an exemplar 2.6 THz bound-to-continuum QCL.

Excited states in polydiacetylene chains: A density matrix renormalization group study

NASA Astrophysics Data System (ADS)

Barcza, Gergely; Barford, William; Gebhard, Florian; Legeza, Örs

2013-06-01

We study theoretically polydiacetylene chains diluted in their monomer matrix. We employ the density matrix renormalization group method on finite chains to calculate the ground state and low-lying excitations of the corresponding Peierls-Hubbard-Ohno Hamiltonian which is characterized by the electron transfer amplitude t0 between nearest neighbors, by the electron-phonon coupling constant α, by the Hubbard interaction U, and by the long-range interaction V. We treat the lattice relaxation in the adiabatic limit, i.e., we calculate the polaronic lattice distortions for each excited state. Using chains with up to 102 lattice sites, we can safely perform the extrapolation to the thermodynamic limit for the ground-state energy and conformation, the single-particle gap, and the energies of the singlet exciton, the triplet ground state, and the optical excitation of the triplet ground state. The corresponding gaps are known with high precision from experiments. We determine a coherent parameter set (t0*=2.4eV,α*=3.4eV/Å,U*=6eV,V*=3eV) from a fit of the experimental gap energies to the theoretical values which we obtain for 81 parameter points in the four-dimensional search space (t0,α,U,V). We identify dark in-gap states in the singlet and triplet sectors as seen in experiments. Using a fairly stiff spring constant, the length of our unit cell is about 1% larger than its experimental value.

Theoretical approach to embed nanocrystallites into a bulk crystalline matrix and the embedding influence on the electronic band structure and optical properties of the resulting heterostructures

NASA Astrophysics Data System (ADS)

Balagan, Semyon A.; Nazarov, Vladimir U.; Shevlyagin, Alexander V.; Goroshko, Dmitrii L.; Galkin, Nikolay G.

2018-06-01

We develop an approach and present results of the combined molecular dynamics and density functional theory calculations of the structural and optical properties of the nanometer-sized crystallites embedded in a bulk crystalline matrix. The method is designed and implemented for both compatible and incompatible lattices of the nanocrystallite (NC) and the host matrix, when determining the NC optimal orientation relative to the matrix constitutes a challenging problem. We suggest and substantiate an expression for the cost function of the search algorithm, which is the energy per supercell generalized for varying number of atoms in the latter. The epitaxial relationships at the Si/NC interfaces and the optical properties are obtained and found to be in a reasonable agreement with experimental data. Dielectric functions show significant sensitivity to the NC’s orientation relative to the matrix at energies below 0.5 eV.

Theoretical approach to embed nanocrystallites into a bulk crystalline matrix and the embedding influence on the electronic band structure and optical properties of the resulting heterostructures.

PubMed

Balagan, Semyon Anatolyevich; Nazarov, Vladimir U; Shevlyagin, Alexander Vladimirovich; Goroshko, Dmitrii L; Galkin, N G

2018-05-03

We develop an approach and present results of the combined molecular dynamics and density functional theory calculations of the structural and optical properties of the nanometer-sized crystallites embedded in a bulk crystalline matrix. The method is designed and implemented for both compatible and incompatible lattices of the nanocrystallite (NC) and the host matrix, when determining the NC optimal orientation relative to the matrix constitutes a challenging problem. We suggest and substantiate an expression for the cost function of the search algorithm, which is the energy per supercell generalized for varying number of atoms in the latter. The epitaxial relationships at the Si/NC interfaces and the optical properties are obtained and found to be in a reasonable agreement with experimental data. Dielectric functions show significant sensitivity to the NC's orientation relative to the matrix at energies below 0.5 eV. © 2018 IOP Publishing Ltd.

Multiconfiguration Pair-Density Functional Theory.

PubMed

Li Manni, Giovanni; Carlson, Rebecca K; Luo, Sijie; Ma, Dongxia; Olsen, Jeppe; Truhlar, Donald G; Gagliardi, Laura

2014-09-09

We present a new theoretical framework, called Multiconfiguration Pair-Density Functional Theory (MC-PDFT), which combines multiconfigurational wave functions with a generalization of density functional theory (DFT). A multiconfigurational self-consistent-field (MCSCF) wave function with correct spin and space symmetry is used to compute the total electronic density, its gradient, the on-top pair density, and the kinetic and Coulomb contributions to the total electronic energy. We then use a functional of the total density, its gradient, and the on-top pair density to calculate the remaining part of the energy, which we call the on-top-density-functional energy in contrast to the exchange-correlation energy of Kohn-Sham DFT. Because the on-top pair density is an element of the two-particle density matrix, this goes beyond the Hohenberg-Kohn theorem that refers only to the one-particle density. To illustrate the theory, we obtain first approximations to the required new type of density functionals by translating conventional density functionals of the spin densities using a simple prescription, and we perform post-SCF density functional calculations using the total density, density gradient, and on-top pair density from the MCSCF calculations. Double counting of dynamic correlation or exchange does not occur because the MCSCF energy is not used. The theory is illustrated by applications to the bond energies and potential energy curves of H2, N2, F2, CaO, Cr2, and NiCl and the electronic excitation energies of Be, C, N, N(+), O, O(+), Sc(+), Mn, Co, Mo, Ru, N2, HCHO, C4H6, c-C5H6, and pyrazine. The method presented has a computational cost and scaling similar to MCSCF, but a quantitative accuracy, even with the present first approximations to the new types of density functionals, that is comparable to much more expensive multireference perturbation theory methods.

A projected preconditioned conjugate gradient algorithm for computing many extreme eigenpairs of a Hermitian matrix [A projected preconditioned conjugate gradient algorithm for computing a large eigenspace of a Hermitian matrix

DOE PAGES

Vecharynski, Eugene; Yang, Chao; Pask, John E.

2015-02-25

Here, we present an iterative algorithm for computing an invariant subspace associated with the algebraically smallest eigenvalues of a large sparse or structured Hermitian matrix A. We are interested in the case in which the dimension of the invariant subspace is large (e.g., over several hundreds or thousands) even though it may still be small relative to the dimension of A. These problems arise from, for example, density functional theory (DFT) based electronic structure calculations for complex materials. The key feature of our algorithm is that it performs fewer Rayleigh–Ritz calculations compared to existing algorithms such as the locally optimalmore » block preconditioned conjugate gradient or the Davidson algorithm. It is a block algorithm, and hence can take advantage of efficient BLAS3 operations and be implemented with multiple levels of concurrency. We discuss a number of practical issues that must be addressed in order to implement the algorithm efficiently on a high performance computer.« less

A program to compute the two-step excitation of mesospheric sodium atoms for the Polychromatic Laser Guide Star Project

NASA Astrophysics Data System (ADS)

Bellanger, Véronique; Courcelle, Arnaud; Petit, Alain

2004-09-01

A program to compute the two-step excitation of sodium atoms ( 3S→3P→4D) using the density-matrix formalism is presented. The BEACON program calculates population evolution and the number of photons emitted by fluorescence from the 3P, 4D, 4P, 4S levels. Program summaryTitle of program: BEACON Catalogue identifier:ADSX Program Summary URL:http://cpc.cs.qub.ac.uk/cpc/summaries/ADSX Program obtainable from: CPC Program Library, Queen's University of Belfast, N. Ireland Licensing provisions: none Operating systems under which the program has been tested: Win; Unix Programming language used: FORTRAN 77 Memory required to execute with typical data: 1 Mw Number of bits in a word: 32 Number of processors used: 1 (a parallel version of this code is also available and can be obtained on request) Number of lines in distributed program, including test data, etc.: 29 287 Number of bytes in distributed program, including test data, etc.: 830 331 Distribution format: tar.gz CPC Program Library subprograms used: none Nature of physical problem: Resolution of the Bloch equations in the case of the two-step laser excitation of sodium atoms. Method of solution: The program BEACON calculates the evolution of level population versus time using the density-matrix formalism. The number of photons emitted from the 3P, 4D and 4P levels is calculated using the branching ratios and the level lifetimes. Restriction on the complexity of the problem: Since the backscatter emission is calculated after the excitation process, excitation with laser pulse duration longer than the 4D level lifetime cannot be rigorously treated. Particularly, cw laser excitation cannot be calculated with this code. Typical running time:12 h

Quasi-exact solvability and entropies of the one-dimensional regularised Calogero model

NASA Astrophysics Data System (ADS)

Pont, Federico M.; Osenda, Omar; Serra, Pablo

2018-05-01

The Calogero model can be regularised through the introduction of a cutoff parameter which removes the divergence in the interaction term. In this work we show that the one-dimensional two-particle regularised Calogero model is quasi-exactly solvable and that for certain values of the Hamiltonian parameters the eigenfunctions can be written in terms of Heun’s confluent polynomials. These eigenfunctions are such that the reduced density matrix of the two-particle density operator can be obtained exactly as well as its entanglement spectrum. We found that the number of non-zero eigenvalues of the reduced density matrix is finite in these cases. The limits for the cutoff distance going to zero (Calogero) and infinity are analysed and all the previously obtained results for the Calogero model are reproduced. Once the exact eigenfunctions are obtained, the exact von Neumann and Rényi entanglement entropies are studied to characterise the physical traits of the model. The quasi-exactly solvable character of the model is assessed studying the numerically calculated Rényi entropy and entanglement spectrum for the whole parameter space.

Interaction effects in Aharonov-Bohm-Kondo rings

NASA Astrophysics Data System (ADS)

Komijani, Yashar; Yoshii, Ryosuke; Affleck, Ian

2013-12-01

We study the conductance through an Aharonov-Bohm ring, containing a quantum dot in the Kondo regime in one arm, at finite temperature and arbitrary electronic density. We develop a general method for this calculation based on changing the basis to the screening and nonscreening channels. We show that an unusual term appears in the conductance, involving the connected four-point Green's function of the conduction electrons. However, this term and the terms quadratic in the T matrix can be eliminated at sufficiently low temperatures, leading to an expression for the conductance linear in the Kondo T matrix. Explicit results are given for temperatures that are high compared to the Kondo temperature.

Properties of quantum systems via diagonalization of transition amplitudes. II. Systematic improvements of short-time propagation

NASA Astrophysics Data System (ADS)

Vidanović, Ivana; Bogojević, Aleksandar; Balaž, Antun; Belić, Aleksandar

2009-12-01

In this paper, building on a previous analysis [I. Vidanović, A. Bogojević, and A. Belić, preceding paper, Phys. Rev. E 80, 066705 (2009)] of exact diagonalization of the space-discretized evolution operator for the study of properties of nonrelativistic quantum systems, we present a substantial improvement to this method. We apply recently introduced effective action approach for obtaining short-time expansion of the propagator up to very high orders to calculate matrix elements of space-discretized evolution operator. This improves by many orders of magnitude previously used approximations for discretized matrix elements and allows us to numerically obtain large numbers of accurate energy eigenvalues and eigenstates using numerical diagonalization. We illustrate this approach on several one- and two-dimensional models. The quality of numerically calculated higher-order eigenstates is assessed by comparison with semiclassical cumulative density of states.

Photochromic properties of the N-Salicylideneaniline in Polyvinyl Butyral matrix: Experimental and theoretical investigations

NASA Astrophysics Data System (ADS)

Shahab, Siyamak; Filippovich, Liudmila; Aharodnikova, M.; Almodarresiyeh, Hora A.; Hajikolaee, Fatemeh Haji; Kumar, Rakesh; Mashayekhi, Mahsa

2017-04-01

In the present work, isomerization, photophysical properties, thermal conductivity (λ) and spectral study of the N-Salicylideneaniline: 2-[(E)-(phenylimino)methyl]phenol (SA) under the action of UV radiation in the Polyvinyl Butyral (PVB) matrix were studied using the Indicator method and Density Functional Theory (DFT). The electronic absorption spectra of SA and its isomers (SA1 and SA2) in dimethylformamide (DMF) solutions were also calculated. The nature of absorption bands of SA, SA1 and SA2 in the visible and near ultraviolet spectral regions was interpreted. The excitation energies, electronic transitions and oscillator strengths for SA, SA1 and SA2 have also been calculated. Thermal Conductivity of PVB-films containing SA before and after UV radiation was also measured. A Photochromic PVB - film on the basis of SA for application in optical devices and display technologies was made.

Thermodynamics of fission products in UO(2 ± x).

PubMed

Nerikar, P V; Liu, X-Y; Uberuaga, B P; Stanek, C R; Phillpot, S R; Sinnott, S B

2009-10-28

The stabilities of selected fission products-Xe, Cs, and Sr-are investigated as a function of non-stoichiometry x in UO(2 ± x). In particular, density functional theory (DFT) is used to calculate the incorporation and solution energies of these fission products at the anion and cation vacancy sites, at the divacancy, and at the bound Schottky defect. In order to reproduce the correct insulating state of UO(2), the DFT calculations are performed using spin polarization and with the Hubbard U term. In general, higher charge defects are more soluble in the fuel matrix and the solubility of fission products increases as the hyperstoichiometry increases. The solubility of fission product oxides is also explored. Cs(2)O is observed as a second stable phase and SrO is found to be soluble in the UO(2) matrix for all stoichiometries. These observations mirror experimentally observed phenomena.

Gas sorption and barrier properties of polymeric membranes from molecular dynamics and Monte Carlo simulations.

PubMed

Cozmuta, Ioana; Blanco, Mario; Goddard, William A

2007-03-29

It is important for many industrial processes to design new materials with improved selective permeability properties. Besides diffusion, the molecule's solubility contributes largely to the overall permeation process. This study presents a method to calculate solubility coefficients of gases such as O2, H2O (vapor), N2, and CO2 in polymeric matrices from simulation methods (Molecular Dynamics and Monte Carlo) using first principle predictions. The generation and equilibration (annealing) of five polymer models (polypropylene, polyvinyl alcohol, polyvinyl dichloride, polyvinyl chloride-trifluoroethylene, and polyethylene terephtalate) are extensively described. For each polymer, the average density and Hansen solubilities over a set of ten samples compare well with experimental data. For polyethylene terephtalate, the average properties between a small (n = 10) and a large (n = 100) set are compared. Boltzmann averages and probability density distributions of binding and strain energies indicate that the smaller set is biased in sampling configurations with higher energies. However, the sample with the lowest cohesive energy density from the smaller set is representative of the average of the larger set. Density-wise, low molecular weight polymers tend to have on average lower densities. Infinite molecular weight samples do however provide a very good representation of the experimental density. Solubility constants calculated with two ensembles (grand canonical and Henry's constant) are equivalent within 20%. For each polymer sample, the solubility constant is then calculated using the faster (10x) Henry's constant ensemble (HCE) from 150 ps of NPT dynamics of the polymer matrix. The influence of various factors (bad contact fraction, number of iterations) on the accuracy of Henry's constant is discussed. To validate the calculations against experimental results, the solubilities of nitrogen and carbon dioxide in polypropylene are examined over a range of temperatures between 250 and 650 K. The magnitudes of the calculated solubilities agree well with experimental results, and the trends with temperature are predicted correctly. The HCE method is used to predict the solubility constants at 298 K of water vapor and oxygen. The water vapor solubilities follow more closely the experimental trend of permeabilities, both ranging over 4 orders of magnitude. For oxygen, the calculated values do not follow entirely the experimental trend of permeabilities, most probably because at this temperature some of the polymers are in the glassy regime and thus are diffusion dominated. Our study also concludes large confidence limits are associated with the calculated Henry's constants. By investigating several factors (terminal ends of the polymer chains, void distribution, etc.), we conclude that the large confidence limits are intimately related to the polymer's conformational changes caused by thermal fluctuations and have to be regarded--at least at microscale--as a characteristic of each polymer and the nature of its interaction with the solute. Reducing the mobility of the polymer matrix as well as controlling the distribution of the free (occupiable) volume would act as mechanisms toward lowering both the gas solubility and the diffusion coefficients.

[Properties and infiltration arts of machinable infiltration ceramic(MIC)].

PubMed

Yang, H; Xian, S; Liao, Y; Xue, Y; Chai, F

2000-06-01

The purpose of this study is to explore the infiltration arts of MIC and study the effects of different packing density of Al2O3 matrix on the properties of MIC. alpha-Al2O3 specimens were fabricated by pouring alpha-Al2O3 slip with different powder/liquid ratios(P/L = 3.5, 7.5, 10.5) into a mold, and subsequently pre-fired at 1160 degrees C for 6 hours to form Al2O3 matrix. The packing density of the matrices were measured. Infiltration concepts were introduced into this study by infiltrating molten mica micro-crystalline glass into the porous Al2O3 matrix at 1160 degrees C for 6 hours to form a continuous interpenetrating composite. The composite then underwent micro-crystallization by nucleating at 550 degrees C for 1 hour and crystallizing at 900 degrees C for 1 hour, which resulted in the MIC. Mechanical properties including three point flexural strength, elastic modulus, Vicker's hardness, indentation fracture toughness and Weibull's modulus of flexural strength were determined. Parameters of machinability(H/KIC)2 of MIC were calculated. XRD and SEM were employed to study its microstructure. The resulted matrices reached packing densities of 63%, 76%, 78% with P/L of 3.5, 7.5 and 10.5. The MIC attained high strength and good machinability after infiltration. Three-point flexural strength and indentation fracture toughness were 342, 431, 374 MPa and 4.05, 4.14, 5.02 MPa m1/2 for MIC with packing density of 63%, 76%, 78% separately. And parameters of machinability were 5.41, 6.84 and 7.39 respectively. Packing density of Al2O3 matrix significantly influenced the mechanical properties. Maximum properties were obtained with a matrix packing density of 75%(P/L = 7.5), with a Weibull's modulus of flexural strength of 6.8. Machinability decreased with the increase of P/L ratio. Micro-crystallizing treatment resulted in the formation of evenly distributed mica crystalline in the composite, which contributed to the high strength of this composite material. MIC is a new infiltrated ceramic with favorable strength and machinability which can satisfy the prosthodontic requirements as all ceramic crown and bridge materials, it also shows promising outlook for future developments and clinical usage.

Anatomical relationships between serotonin 5-HT2A and dopamine D2 receptors in living human brain.

PubMed

Ishii, Tatsuya; Kimura, Yasuyuki; Ichise, Masanori; Takahata, Keisuke; Kitamura, Soichiro; Moriguchi, Sho; Kubota, Manabu; Zhang, Ming-Rong; Yamada, Makiko; Higuchi, Makoto; Okubo, Yoshinori; Suhara, Tetsuya

2017-01-01

Seven healthy volunteers underwent PET scans with [18F]altanserin and [11C]FLB 457 for 5-HT2A and D2 receptors, respectively. As a measure of receptor density, a binding potential (BP) was calculated from PET data for 76 cerebral cortical regions. A correlation matrix was calculated between the binding potentials of [18F]altanserin and [11C]FLB 457 for those regions. The regional relationships were investigated using a bicluster analysis of the correlation matrix with an iterative signature algorithm. We identified two clusters of regions. The first cluster identified a distinct profile of correlation coefficients between 5-HT2A and D2 receptors, with the former in regions related to sensorimotor integration (supplementary motor area, superior parietal gyrus, and paracentral lobule) and the latter in most cortical regions. The second cluster identified another distinct profile of correlation coefficients between 5-HT2A receptors in the bilateral hippocampi and D2 receptors in most cortical regions. The observation of two distinct clusters in the correlation matrix suggests regional interactions between 5-HT2A and D2 receptors in sensorimotor integration and hippocampal function. A bicluster analysis of the correlation matrix of these neuroreceptors may be beneficial in understanding molecular networks in the human brain.

A new time dependent density functional algorithm for large systems and plasmons in metal clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baseggio, Oscar; Fronzoni, Giovanna; Stener, Mauro, E-mail: stener@univ.trieste.it

2015-07-14

A new algorithm to solve the Time Dependent Density Functional Theory (TDDFT) equations in the space of the density fitting auxiliary basis set has been developed and implemented. The method extracts the spectrum from the imaginary part of the polarizability at any given photon energy, avoiding the bottleneck of Davidson diagonalization. The original idea which made the present scheme very efficient consists in the simplification of the double sum over occupied-virtual pairs in the definition of the dielectric susceptibility, allowing an easy calculation of such matrix as a linear combination of constant matrices with photon energy dependent coefficients. The methodmore » has been applied to very different systems in nature and size (from H{sub 2} to [Au{sub 147}]{sup −}). In all cases, the maximum deviations found for the excitation energies with respect to the Amsterdam density functional code are below 0.2 eV. The new algorithm has the merit not only to calculate the spectrum at whichever photon energy but also to allow a deep analysis of the results, in terms of transition contribution maps, Jacob plasmon scaling factor, and induced density analysis, which have been all implemented.« less

Flavin Charge Transfer Transitions Assist DNA Photolyase Electron Transfer

NASA Astrophysics Data System (ADS)

Skourtis, Spiros S.; Prytkova, Tatiana; Beratan, David N.

2007-12-01

This contribution describes molecular dynamics, semi-empirical and ab-initio studies of the primary photo-induced electron transfer reaction in DNA photolyase. DNA photolyases are FADH--containing proteins that repair UV-damaged DNA by photo-induced electron transfer. A DNA photolyase recognizes and binds to cyclobutatne pyrimidine dimer lesions of DNA. The protein repairs a bound lesion by transferring an electron to the lesion from FADH-, upon photo-excitation of FADH- with 350-450 nm light. We compute the lowest singlet excited states of FADH- in DNA photolyase using INDO/S configuration interaction, time-dependent density-functional, and time-dependent Hartree-Fock methods. The calculations identify the lowest singlet excited state of FADH- that is populated after photo-excitation and that acts as the electron donor. For this donor state we compute conformationally-averaged tunneling matrix elements to empty electron-acceptor states of a thymine dimer bound to photolyase. The conformational averaging involves different FADH--thymine dimer confromations obtained from molecular dynamics simulations of the solvated protein with a thymine dimer docked in its active site. The tunneling matrix element computations use INDO/S-level Green's function, energy splitting, and Generalized Mulliken-Hush methods. These calculations indicate that photo-excitation of FADH- causes a π→π* charge-transfer transition that shifts electron density to the side of the flavin isoalloxazine ring that is adjacent to the docked thymine dimer. This shift in electron density enhances the FADH--to-dimer electronic coupling, thus inducing rapid electron transfer.

XAFSmass: a program for calculating the optimal mass of XAFS samples

NASA Astrophysics Data System (ADS)

Klementiev, K.; Chernikov, R.

2016-05-01

We present a new implementation of the XAFSmass program that calculates the optimal mass of XAFS samples. It has several improvements as compared to the old Windows based program XAFSmass: 1) it is truly platform independent, as provided by Python language, 2) it has an improved parser of chemical formulas that enables parentheses and nested inclusion-to-matrix weight percentages. The program calculates the absorption edge height given the total optical thickness, operates with differently determined sample amounts (mass, pressure, density or sample area) depending on the aggregate state of the sample and solves the inverse problem of finding the elemental composition given the experimental absorption edge jump and the chemical formula.

Isoscalar and isovector giant resonances in a self-consistent phonon coupling approach

NASA Astrophysics Data System (ADS)

Lyutorovich, N.; Tselyaev, V.; Speth, J.; Krewald, S.; Grümmer, F.; Reinhard, P.-G.

2015-10-01

We present fully self-consistent calculations of isoscalar giant monopole and quadrupole as well as isovector giant dipole resonances in heavy and light nuclei. The description is based on Skyrme energy-density functionals determining the static Hartree-Fock ground state and the excitation spectra within random-phase approximation (RPA) and RPA extended by including the quasiparticle-phonon coupling at the level of the time-blocking approximation (TBA). All matrix elements were derived consistently from the given energy-density functional and calculated without any approximation. As a new feature in these calculations, the single-particle continuum was included thus avoiding the artificial discretization usually implied in RPA and TBA. The step to include phonon coupling in TBA leads to small, but systematic, down shifts of the centroid energies of the giant resonances. These shifts are similar in size for all Skyrme parametrizations investigated here. After all, we demonstrate that one can find Skyrme parametrizations which deliver a good simultaneous reproduction of all three giant resonances within TBA.

Correlation matrix renormalization theory for correlated-electron materials with application to the crystalline phases of atomic hydrogen

DOE PAGES

Zhao, Xin; Liu, Jun; Yao, Yong-Xin; ...

2018-01-23

Developing accurate and computationally efficient methods to calculate the electronic structure and total energy of correlated-electron materials has been a very challenging task in condensed matter physics and materials science. Recently, we have developed a correlation matrix renormalization (CMR) method which does not assume any empirical Coulomb interaction U parameters and does not have double counting problems in the ground-state total energy calculation. The CMR method has been demonstrated to be accurate in describing both the bonding and bond breaking behaviors of molecules. In this study, we extend the CMR method to the treatment of electron correlations in periodic solidmore » systems. By using a linear hydrogen chain as a benchmark system, we show that the results from the CMR method compare very well with those obtained recently by accurate quantum Monte Carlo (QMC) calculations. We also study the equation of states of three-dimensional crystalline phases of atomic hydrogen. We show that the results from the CMR method agree much better with the available QMC data in comparison with those from density functional theory and Hartree-Fock calculations.« less

Correlation matrix renormalization theory for correlated-electron materials with application to the crystalline phases of atomic hydrogen

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhao, Xin; Liu, Jun; Yao, Yong-Xin

Developing accurate and computationally efficient methods to calculate the electronic structure and total energy of correlated-electron materials has been a very challenging task in condensed matter physics and materials science. Recently, we have developed a correlation matrix renormalization (CMR) method which does not assume any empirical Coulomb interaction U parameters and does not have double counting problems in the ground-state total energy calculation. The CMR method has been demonstrated to be accurate in describing both the bonding and bond breaking behaviors of molecules. In this study, we extend the CMR method to the treatment of electron correlations in periodic solidmore » systems. By using a linear hydrogen chain as a benchmark system, we show that the results from the CMR method compare very well with those obtained recently by accurate quantum Monte Carlo (QMC) calculations. We also study the equation of states of three-dimensional crystalline phases of atomic hydrogen. We show that the results from the CMR method agree much better with the available QMC data in comparison with those from density functional theory and Hartree-Fock calculations.« less

Molecular properties of excited electronic state: Formalism, implementation, and applications of analytical second energy derivatives within the framework of the time-dependent density functional theory/molecular mechanics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zeng, Qiao; Liang, WanZhen, E-mail: liangwz@xmu.edu.cn; Liu, Jie

2014-05-14

This work extends our previous works [J. Liu and W. Z. Liang, J. Chem. Phys. 135, 014113 (2011); J. Liu and W. Z. Liang, J. Chem. Phys. 135, 184111 (2011)] on analytical excited-state energy Hessian within the framework of time-dependent density functional theory (TDDFT) to couple with molecular mechanics (MM). The formalism, implementation, and applications of analytical first and second energy derivatives of TDDFT/MM excited state with respect to the nuclear and electric perturbations are presented. Their performances are demonstrated by the calculations of adiabatic excitation energies, and excited-state geometries, harmonic vibrational frequencies, and infrared intensities for a number ofmore » benchmark systems. The consistent results with the full quantum mechanical method and other hybrid theoretical methods indicate the reliability of the current numerical implementation of developed algorithms. The computational accuracy and efficiency of the current analytical approach are also checked and the computational efficient strategies are suggested to speed up the calculations of complex systems with many MM degrees of freedom. Finally, we apply the current analytical approach in TDDFT/MM to a realistic system, a red fluorescent protein chromophore together with part of its nearby protein matrix. The calculated results indicate that the rearrangement of the hydrogen bond interactions between the chromophore and the protein matrix is responsible for the large Stokes shift.« less

Combining Density Functional Theory and Green's Function Theory: Range-Separated, Nonlocal, Dynamic, and Orbital-Dependent Hybrid Functional.

PubMed

Kananenka, Alexei A; Zgid, Dominika

2017-11-14

We present a rigorous framework which combines single-particle Green's function theory with density functional theory based on a separation of electron-electron interactions into short- and long-range components. Short-range contribution to the total energy and exchange-correlation potential is provided by a density functional approximation, while the long-range contribution is calculated using an explicit many-body Green's function method. Such a hybrid results in a nonlocal, dynamic, and orbital-dependent exchange-correlation functional of a single-particle Green's function. In particular, we present a range-separated hybrid functional called srSVWN5-lrGF2 which combines the local-density approximation and the second-order Green's function theory. We illustrate that similarly to density functional approximations, the new functional is weakly basis-set dependent. Furthermore, it offers an improved description of the short-range dynamic correlation. The many-body contribution to the functional mitigates the many-electron self-interaction error present in many density functional approximations and provides a better description of molecular properties. Additionally, we illustrate that the new functional can be used to scale down the self-energy and, therefore, introduce an additional sparsity to the self-energy matrix that in the future can be exploited in calculations for large molecules or periodic systems.

Multiresolution quantum chemistry in multiwavelet bases: excited states from time-dependent Hartree–Fock and density functional theory via linear response

DOE PAGES

Yanai, Takeshi; Fann, George I.; Beylkin, Gregory; ...

2015-02-25

Using the fully numerical method for time-dependent Hartree–Fock and density functional theory (TD-HF/DFT) with the Tamm–Dancoff (TD) approximation we use a multiresolution analysis (MRA) approach to present our findings. From a reformulation with effective use of the density matrix operator, we obtain a general form of the HF/DFT linear response equation in the first quantization formalism. It can be readily rewritten as an integral equation with the bound-state Helmholtz (BSH) kernel for the Green's function. The MRA implementation of the resultant equation permits excited state calculations without virtual orbitals. Moreover, the integral equation is efficiently and adaptively solved using amore » numerical multiresolution solver with multiwavelet bases. Our implementation of the TD-HF/DFT methods is applied for calculating the excitation energies of H 2, Be, N 2, H 2O, and C 2H 4 molecules. The numerical errors of the calculated excitation energies converge in proportion to the residuals of the equation in the molecular orbitals and response functions. The energies of the excited states at a variety of length scales ranging from short-range valence excitations to long-range Rydberg-type ones are consistently accurate. It is shown that the multiresolution calculations yield the correct exponential asymptotic tails for the response functions, whereas those computed with Gaussian basis functions are too diffuse or decay too rapidly. Finally, we introduce a simple asymptotic correction to the local spin-density approximation (LSDA) so that in the TDDFT calculations, the excited states are correctly bound.« less

A Least-Squares Commutator in the Iterative Subspace Method for Accelerating Self-Consistent Field Convergence.

PubMed

Li, Haichen; Yaron, David J

2016-11-08

A least-squares commutator in the iterative subspace (LCIIS) approach is explored for accelerating self-consistent field (SCF) calculations. LCIIS is similar to direct inversion of the iterative subspace (DIIS) methods in that the next iterate of the density matrix is obtained as a linear combination of past iterates. However, whereas DIIS methods find the linear combination by minimizing a sum of error vectors, LCIIS minimizes the Frobenius norm of the commutator between the density matrix and the Fock matrix. This minimization leads to a quartic problem that can be solved iteratively through a constrained Newton's method. The relationship between LCIIS and DIIS is discussed. Numerical experiments suggest that LCIIS leads to faster convergence than other SCF convergence accelerating methods in a statistically significant sense, and in a number of cases LCIIS leads to stable SCF solutions that are not found by other methods. The computational cost involved in solving the quartic minimization problem is small compared to the typical cost of SCF iterations and the approach is easily integrated into existing codes. LCIIS can therefore serve as a powerful addition to SCF convergence accelerating methods in computational quantum chemistry packages.

A Comparative Study of Collagen Matrix Density Effect on Endothelial Sprout Formation Using Experimental and Computational Approaches.

PubMed

Shamloo, Amir; Mohammadaliha, Negar; Heilshorn, Sarah C; Bauer, Amy L

2016-04-01

A thorough understanding of determining factors in angiogenesis is a necessary step to control the development of new blood vessels. Extracellular matrix density is known to have a significant influence on cellular behaviors and consequently can regulate vessel formation. The utilization of experimental platforms in combination with numerical models can be a powerful method to explore the mechanisms of new capillary sprout formation. In this study, using an integrative method, the interplay between the matrix density and angiogenesis was investigated. Owing the fact that the extracellular matrix density is a global parameter that can affect other parameters such as pore size, stiffness, cell-matrix adhesion and cross-linking, deeper understanding of the most important biomechanical or biochemical properties of the ECM causing changes in sprout morphogenesis is crucial. Here, we implemented both computational and experimental methods to analyze the mechanisms responsible for the influence of ECM density on the sprout formation that is difficult to be investigated comprehensively using each of these single methods. For this purpose, we first utilized an innovative approach to quantify the correspondence of the simulated collagen fibril density to the collagen density in the experimental part. Comparing the results of the experimental study and computational model led to some considerable achievements. First, we verified the results of the computational model using the experimental results. Then, we reported parameters such as the ratio of proliferating cells to migrating cells that was difficult to obtain from experimental study. Finally, this integrative system led to gain an understanding of the possible mechanisms responsible for the effect of ECM density on angiogenesis. The results showed that stable and long sprouts were observed at an intermediate collagen matrix density of 1.2 and 1.9 mg/ml due to a balance between the number of migrating and proliferating cells. As a result of weaker connections between the cells and matrix, a lower collagen matrix density (0.7 mg/ml) led to unstable and broken sprouts. However, higher matrix density (2.7 mg/ml) suppressed sprout formation due to the high level of matrix entanglement, which inhibited cell migration. This study also showed that extracellular matrix density can influence sprout branching. Our experimental results support this finding.

Communication: Symmetrical quasi-classical analysis of linear optical spectroscopy

NASA Astrophysics Data System (ADS)

Provazza, Justin; Coker, David F.

2018-05-01

The symmetrical quasi-classical approach for propagation of a many degree of freedom density matrix is explored in the context of computing linear spectra. Calculations on a simple two state model for which exact results are available suggest that the approach gives a qualitative description of peak positions, relative amplitudes, and line broadening. Short time details in the computed dipole autocorrelation function result in exaggerated tails in the spectrum.

Reexamination of relaxation of spins due to a magnetic field gradient: Identity of the Redfield and Torrey theories

DOE Office of Scientific and Technical Information (OSTI.GOV)

Golub, R.; Rohm, Ryan M.; Swank, C. M.

2011-02-15

There is an extensive literature on magnetic-gradient-induced spin relaxation. Cates, Schaefer, and Happer, in a seminal publication, have solved the problem in the regime where diffusion theory (the Torrey equation) is applicable using an expansion of the density matrix in diffusion equation eigenfunctions and angular momentum tensors. McGregor has solved the problem in the same regime using a slightly more general formulation using the Redfield theory formulated in terms of the autocorrelation function of the fluctuating field seen by the spins and calculating the correlation functions using the diffusion-theory Green's function. The results of both calculations were shown to agreemore » for a special case. In the present work, we show that the eigenfunction expansion of the Torrey equation yields the expansion of the Green's function for the diffusion equation, thus showing the identity of this approach with that of the Redfield theory. The general solution can also be obtained directly from the Torrey equation for the density matrix. Thus, the physical content of the Redfield and Torrey approaches are identical. We then introduce a more general expression for the position autocorrelation function of particles moving in a closed cell, extending the range of applicability of the theory.« less

Theory of time-resolved photoelectron imaging. Comparison of a density functional with a time-dependent density functional approach

NASA Astrophysics Data System (ADS)

Suzuki, Yoshi-ichi; Seideman, Tamar; Stener, Mauro

2004-01-01

Time-resolved photoelectron differential cross sections are computed within a quantum dynamical theory that combines a formally exact solution of the nuclear dynamics with density functional theory (DFT)-based approximations of the electronic dynamics. Various observables of time-resolved photoelectron imaging techniques are computed at the Kohn-Sham and at the time-dependent DFT levels. Comparison of the results serves to assess the reliability of the former method and hence its usefulness as an economic approach for time-domain photoelectron cross section calculations, that is applicable to complex polyatomic systems. Analysis of the matrix elements that contain the electronic dynamics provides insight into a previously unexplored aspect of femtosecond-resolved photoelectron imaging.

Semiclassics for matrix Hamiltonians: The Gutzwiller trace formula with applications to graphene-type systems

NASA Astrophysics Data System (ADS)

Vogl, M.; Pankratov, O.; Shallcross, S.

2017-07-01

We present a tractable and physically transparent semiclassical theory of matrix-valued Hamiltonians, i.e., those that describe quantum systems with internal degrees of freedoms, based on a generalization of the Gutzwiller trace formula for a n ×n dimensional Hamiltonian H (p ̂,q ̂) . The classical dynamics is governed by n Hamilton-Jacobi (HJ) equations that act in a phase space endowed with a classical Berry curvature encoding anholonomy in the parallel transport of the eigenvectors of H (p ,q ) ; these vectors describe the internal structure of the semiclassical particles. At the O (ℏ1) level and for nondegenerate HJ systems, this curvature results in an additional semiclassical phase composed of (i) a Berry phase and (ii) a dynamical phase resulting from the classical particles "moving through the Berry curvature". We show that the dynamical part of this semiclassical phase will, generally, be zero only for the case in which the Berry phase is topological (i.e., depends only on the winding number). We illustrate the method by calculating the Landau spectrum for monolayer graphene, the four-band model of AB bilayer graphene, and for a more complicated matrix Hamiltonian describing the silicene band structure. Finally, we apply our method to an inhomogeneous system consisting of a strain engineered one-dimensional moiré in bilayer graphene, finding localized states near the Dirac point that arise from electron trapping in a semiclassical moiré potential. The semiclassical density of states of these localized states we show to be in perfect agreement with an exact quantum mechanical calculation of the density of states.

A reformulation of the coupled perturbed self-consistent field equations entirely within a local atomic orbital density matrix-based scheme

NASA Astrophysics Data System (ADS)

Ochsenfeld, Christian; Head-Gordon, Martin

1997-05-01

To exploit the exponential decay found in numerical studies for the density matrix and its derivative with respect to nuclear displacements, we reformulate the coupled perturbed self-consistent field (CPSCF) equations and a quadratically convergent SCF (QCSCF) method for Hartree-Fock and density functional theory within a local density matrix-based scheme. Our D-CPSCF (density matrix-based CPSCF) and D-QCSCF schemes open the way for exploiting sparsity and to achieve asymptotically linear scaling of computational complexity with molecular size ( M), in case of D-CPSCF for all O( M) derivative densities. Furthermore, these methods are even for small molecules strongly competitive to conventional algorithms.

Density functional calculations of multiphonon capture cross sections at defects in semiconductors

NASA Astrophysics Data System (ADS)

Barmparis, Georgios D.; Puzyrev, Yevgeniy S.; Zhang, X.-G.; Pantelides, Sokrates T.

2014-03-01

The theory of electron capture cross sections by multiphonon processes in semiconductors has a long and controversial history. Here we present a comprehensive theory and describe its implementation for realistic calculations. The Born-Oppenheimer and the Frank-Condon approximations are employed. The transition probability of an incoming electron is written as a product of an instantaneous electronic transition in the initial defect configuration and the line shape function (LSF) that describes the multiphonon processes that lead to lattice relaxation. The electronic matrix elements are calculated using the Projector Augmented Wave (PAW) method which yields the true wave functions while still employing a plane-wave basis. The LSF is calculated by employing a Monte Carlo method and the real phonon modes of the defect, calculated using density functional theory in the PAW scheme. Initial results of the capture cross section for a prototype system, namely a triply hydrogenated vacancy in Si are presented. The results are relevant for modeling device degradation by hot electron effects. This work is supported in part by the Samsung Advanced Institute of Technology (SAIT)'s Global Research Outreach (GRO) Program and by the LDRD program at ORNL.

Cucheb: A GPU implementation of the filtered Lanczos procedure

NASA Astrophysics Data System (ADS)

Aurentz, Jared L.; Kalantzis, Vassilis; Saad, Yousef

2017-11-01

This paper describes the software package Cucheb, a GPU implementation of the filtered Lanczos procedure for the solution of large sparse symmetric eigenvalue problems. The filtered Lanczos procedure uses a carefully chosen polynomial spectral transformation to accelerate convergence of the Lanczos method when computing eigenvalues within a desired interval. This method has proven particularly effective for eigenvalue problems that arise in electronic structure calculations and density functional theory. We compare our implementation against an equivalent CPU implementation and show that using the GPU can reduce the computation time by more than a factor of 10. Program Summary Program title: Cucheb Program Files doi:http://dx.doi.org/10.17632/rjr9tzchmh.1 Licensing provisions: MIT Programming language: CUDA C/C++ Nature of problem: Electronic structure calculations require the computation of all eigenvalue-eigenvector pairs of a symmetric matrix that lie inside a user-defined real interval. Solution method: To compute all the eigenvalues within a given interval a polynomial spectral transformation is constructed that maps the desired eigenvalues of the original matrix to the exterior of the spectrum of the transformed matrix. The Lanczos method is then used to compute the desired eigenvectors of the transformed matrix, which are then used to recover the desired eigenvalues of the original matrix. The bulk of the operations are executed in parallel using a graphics processing unit (GPU). Runtime: Variable, depending on the number of eigenvalues sought and the size and sparsity of the matrix. Additional comments: Cucheb is compatible with CUDA Toolkit v7.0 or greater.

A sparse matrix-vector multiplication based algorithm for accurate density matrix computations on systems of millions of atoms

NASA Astrophysics Data System (ADS)

Ghale, Purnima; Johnson, Harley T.

2018-06-01

We present an efficient sparse matrix-vector (SpMV) based method to compute the density matrix P from a given Hamiltonian in electronic structure computations. Our method is a hybrid approach based on Chebyshev-Jackson approximation theory and matrix purification methods like the second order spectral projection purification (SP2). Recent methods to compute the density matrix scale as O(N) in the number of floating point operations but are accompanied by large memory and communication overhead, and they are based on iterative use of the sparse matrix-matrix multiplication kernel (SpGEMM), which is known to be computationally irregular. In addition to irregularity in the sparse Hamiltonian H, the nonzero structure of intermediate estimates of P depends on products of H and evolves over the course of computation. On the other hand, an expansion of the density matrix P in terms of Chebyshev polynomials is straightforward and SpMV based; however, the resulting density matrix may not satisfy the required constraints exactly. In this paper, we analyze the strengths and weaknesses of the Chebyshev-Jackson polynomials and the second order spectral projection purification (SP2) method, and propose to combine them so that the accurate density matrix can be computed using the SpMV computational kernel only, and without having to store the density matrix P. Our method accomplishes these objectives by using the Chebyshev polynomial estimate as the initial guess for SP2, which is followed by using sparse matrix-vector multiplications (SpMVs) to replicate the behavior of the SP2 algorithm for purification. We demonstrate the method on a tight-binding model system of an oxide material containing more than 3 million atoms. In addition, we also present the predicted behavior of our method when applied to near-metallic Hamiltonians with a wide energy spectrum.

A method to estimate statistical errors of properties derived from charge-density modelling

PubMed Central

Lecomte, Claude

2018-01-01

Estimating uncertainties of property values derived from a charge-density model is not straightforward. A methodology, based on calculation of sample standard deviations (SSD) of properties using randomly deviating charge-density models, is proposed with the MoPro software. The parameter shifts applied in the deviating models are generated in order to respect the variance–covariance matrix issued from the least-squares refinement. This ‘SSD methodology’ procedure can be applied to estimate uncertainties of any property related to a charge-density model obtained by least-squares fitting. This includes topological properties such as critical point coordinates, electron density, Laplacian and ellipticity at critical points and charges integrated over atomic basins. Errors on electrostatic potentials and interaction energies are also available now through this procedure. The method is exemplified with the charge density of compound (E)-5-phenylpent-1-enylboronic acid, refined at 0.45 Å resolution. The procedure is implemented in the freely available MoPro program dedicated to charge-density refinement and modelling. PMID:29724964

Entanglement and magnetism in high-spin graphene nanodisks

NASA Astrophysics Data System (ADS)

Hagymási, I.; Legeza, Ö.

2018-01-01

We investigate the ground-state properties of triangular graphene nanoflakes with zigzag edge configurations. The description of zero-dimensional nanostructures requires accurate many-body techniques since the widely used density-functional theory with local density approximation or Hartree-Fock methods cannot handle the strong quantum fluctuations. Applying the unbiased density-matrix renormalization group algorithm we calculate the magnetization and entanglement patterns with high accuracy for different interaction strengths and compare them to the mean-field results. With the help of quantum information analysis and subsystem density matrices we reveal that the edges are strongly entangled with each other. We also address the effect of electron and hole doping and demonstrate that the magnetic properties of triangular nanoflakes can be controlled by an electric field, which reveals features of flat-band ferromagnetism. This may open up new avenues in graphene based spintronics.

Hartree and Exchange in Ensemble Density Functional Theory: Avoiding the Nonuniqueness Disaster.

PubMed

Gould, Tim; Pittalis, Stefano

2017-12-15

Ensemble density functional theory is a promising method for the efficient and accurate calculation of excitations of quantum systems, at least if useful functionals can be developed to broaden its domain of practical applicability. Here, we introduce a guaranteed single-valued "Hartree-exchange" ensemble density functional, E_{Hx}[n], in terms of the right derivative of the universal ensemble density functional with respect to the coupling constant at vanishing interaction. We show that E_{Hx}[n] is straightforwardly expressible using block eigenvalues of a simple matrix [Eq. (14)]. Specialized expressions for E_{Hx}[n] from the literature, including those involving superpositions of Slater determinants, can now be regarded as originating from the unifying picture presented here. We thus establish a clear and practical description for Hartree and exchange in ensemble systems.

Lanczos algorithm with matrix product states for dynamical correlation functions

NASA Astrophysics Data System (ADS)

Dargel, P. E.; Wöllert, A.; Honecker, A.; McCulloch, I. P.; Schollwöck, U.; Pruschke, T.

2012-05-01

The density-matrix renormalization group (DMRG) algorithm can be adapted to the calculation of dynamical correlation functions in various ways which all represent compromises between computational efficiency and physical accuracy. In this paper we reconsider the oldest approach based on a suitable Lanczos-generated approximate basis and implement it using matrix product states (MPS) for the representation of the basis states. The direct use of matrix product states combined with an ex post reorthogonalization method allows us to avoid several shortcomings of the original approach, namely the multitargeting and the approximate representation of the Hamiltonian inherent in earlier Lanczos-method implementations in the DMRG framework, and to deal with the ghost problem of Lanczos methods, leading to a much better convergence of the spectral weights and poles. We present results for the dynamic spin structure factor of the spin-1/2 antiferromagnetic Heisenberg chain. A comparison to Bethe ansatz results in the thermodynamic limit reveals that the MPS-based Lanczos approach is much more accurate than earlier approaches at minor additional numerical cost.

Unifying model for random matrix theory in arbitrary space dimensions

NASA Astrophysics Data System (ADS)

Cicuta, Giovanni M.; Krausser, Johannes; Milkus, Rico; Zaccone, Alessio

2018-03-01

A sparse random block matrix model suggested by the Hessian matrix used in the study of elastic vibrational modes of amorphous solids is presented and analyzed. By evaluating some moments, benchmarked against numerics, differences in the eigenvalue spectrum of this model in different limits of space dimension d , and for arbitrary values of the lattice coordination number Z , are shown and discussed. As a function of these two parameters (and their ratio Z /d ), the most studied models in random matrix theory (Erdos-Renyi graphs, effective medium, and replicas) can be reproduced in the various limits of block dimensionality d . Remarkably, the Marchenko-Pastur spectral density (which is recovered by replica calculations for the Laplacian matrix) is reproduced exactly in the limit of infinite size of the blocks, or d →∞ , which clarifies the physical meaning of space dimension in these models. We feel that the approximate results for d =3 provided by our method may have many potential applications in the future, from the vibrational spectrum of glasses and elastic networks to wave localization, disordered conductors, random resistor networks, and random walks.

Detection of Matrix Crack Density of CFRP using an Electrical Potential Change Method with Multiple Probes

NASA Astrophysics Data System (ADS)

Todoroki, Akira; Omagari, Kazuomi

Carbon Fiber Reinforced Plastic (CFRP) laminates are adopted for fuel tank structures of next generation space rockets or automobiles. Matrix cracks may cause fuel leak or trigger fatigue damage. A monitoring system of the matrix crack density is required. The authors have developed an electrical resistance change method for the monitoring of delamination cracks in CFRP laminates. Reinforcement fibers are used as a self-sensing system. In the present study, the electric potential method is adopted for matrix crack density monitoring. Finite element analysis (FEA) was performed to investigate the possibility of monitoring matrix crack density using multiple electrodes mounted on a single surface of a specimen. The FEA reveals the matrix crack density increases electrical resistance for a target segment between electrodes. Experimental confirmation was also performed using cross-ply laminates. Eight electrodes were mounted on a single surface of a specimen using silver paste after polishing of the specimen surface with sandpaper. The two outermost electrodes applied electrical current, and the inner electrodes measured electric voltage changes. The slope of electrical resistance during reloading is revealed to be an appropriate index for the detection of matrix crack density.

Blending Determinism with Evolutionary Computing: Applications to the Calculation of the Molecular Electronic Structure of Polythiophene.

PubMed

Sarkar, Kanchan; Sharma, Rahul; Bhattacharyya, S P

2010-03-09

A density matrix based soft-computing solution to the quantum mechanical problem of computing the molecular electronic structure of fairly long polythiophene (PT) chains is proposed. The soft-computing solution is based on a "random mutation hill climbing" scheme which is modified by blending it with a deterministic method based on a trial single-particle density matrix [P((0))(R)] for the guessed structural parameters (R), which is allowed to evolve under a unitary transformation generated by the Hamiltonian H(R). The Hamiltonian itself changes as the geometrical parameters (R) defining the polythiophene chain undergo mutation. The scale (λ) of the transformation is optimized by making the energy [E(λ)] stationary with respect to λ. The robustness and the performance levels of variants of the algorithm are analyzed and compared with those of other derivative free methods. The method is further tested successfully with optimization of the geometry of bipolaron-doped long PT chains.

Leucine/Pd-loaded (5,5) single-walled carbon nanotube matrix as a novel nanobiosensors for in silico detection of protein.

PubMed

Yoosefian, Mehdi; Etminan, Nazanin

2018-06-01

We have designed a novel nanobiosensor for in silico detecting proteins based on leucine/Pd-loaded single-walled carbon nanotube matrix. Density functional theory at the B3LYP/6-31G (d) level of theory was realized to analyze the geometrical and electronic structure of the proposed nanobiosensor. The solvent effects were investigated using the Tomasi's polarized continuum model. Atoms-in-molecules theory was used to study the nature of interactions by calculating the electron density ρ(r) and Laplacian at the bond critical points. Natural bond orbital analysis was performed to achieve a deep understanding of the nature of the interactions. The biosensor has potential application for high sensitive and rapid response to protein due to the chemical adsorption of L-leucine amino acid onto Pd-loaded single-walled carbon nanotube and reactive functional groups that can incorporate in hydrogen binding, hydrophobic interactions and van der Waals forces with the protein surface in detection process.

Many-body expansion of the Fock matrix in the fragment molecular orbital method

NASA Astrophysics Data System (ADS)

Fedorov, Dmitri G.; Kitaura, Kazuo

2017-09-01

A many-body expansion of the Fock matrix in the fragment molecular orbital method is derived up to three-body terms for restricted Hartree-Fock and density functional theory in the atomic orbital basis and compared to the expansion in the basis of fragment molecular orbitals (MOs). The physical nature of many-body corrections is revealed in terms of charge transfer terms. An improvement of the fragment MO expansion is proposed by adding exchange to the embedding. The accuracy of all developed methods is demonstrated in comparison to unfragmented results for polyalanines, a water cluster, Trp-cage (PDB: 1L2Y) and crambin (PDB: 1CRN) proteins, a zeolite cluster, a Si nano-wire, and a boron nitride ribbon. The physical nature of metallicity is discussed, and it is shown what kinds of metallic systems can be treated by fragment-based methods. The density of states is calculated for a fully closed and a partially open nano-ring of boron nitride with a diameter of 105 nm.

Diffusion of Conserved Charges in Relativistic Heavy Ion Collisions

NASA Astrophysics Data System (ADS)

Greif, Moritz; Fotakis, Jan. A.; Denicol, Gabriel S.; Greiner, Carsten

2018-06-01

We demonstrate that the diffusion currents do not depend only on gradients of their corresponding charge density, but that the different diffusion charge currents are coupled. This happens in such a way that it is possible for density gradients of a given charge to generate dissipative currents of another charge. Within this scheme, the charge diffusion coefficient is best viewed as a matrix, in which the diagonal terms correspond to the usual charge diffusion coefficients, while the off-diagonal terms describe the coupling between the different currents. In this Letter, we calculate for the first time the complete diffusion matrix for hot and dense nuclear matter, including baryon, electric, and strangeness charges. We find that the baryon diffusion current is strongly affected by baryon charge gradients but also by its coupling to gradients in strangeness. The electric charge diffusion current is found to be strongly affected by electric and strangeness gradients, whereas strangeness currents depend mostly on strange and baryon gradients.

Transport properties of C and O in UN fuels

NASA Astrophysics Data System (ADS)

Schuler, Thomas; Lopes, Denise Adorno; Claisse, Antoine; Olsson, Pär

2017-03-01

Uranium nitride fuel is considered for fast reactors (GEN-IV generation and space reactors) and for light water reactors as a high-density fuel option. Despite this large interest, there is a lack of information about its behavior for in-pile and out-of-pile conditions. From the present literature, it is known that C and O impurities have significant influence on the fuel performance. Here we perform a systematic study of these impurities in the UN matrix using electronic-structure calculations of solute-defect interactions and microscopic jump frequencies. These quantities were calculated in the DFT +U approximation combined with the occupation matrix control scheme, to avoid convergence to metastable states for the 5 f levels. The transport coefficients of the system were evaluated with the self-consistent mean-field theory. It is demonstrated that carbon and oxygen impurities have different diffusion properties in the UN matrix, with O atoms having a higher mobility, and C atoms showing a strong flux coupling anisotropy. The kinetic interplay between solutes and vacancies is expected to be the main cause for surface segregation, as incorporation energies show no strong thermodynamic segregation preference for (001) surfaces compared with the bulk.

Use of an Inverse Method for Time Series to Estimate the Dynamics of and Management Strategies for the Box Jellyfish Carybdea marsupialis.

PubMed

Bordehore, Cesar; Fuentes, Verónica L; Segarra, Jose G; Acevedo, Melisa; Canepa, Antonio; Raventós, Josep

2015-01-01

Frequently, population ecology of marine organisms uses a descriptive approach in which their sizes and densities are plotted over time. This approach has limited usefulness for design strategies in management or modelling different scenarios. Population projection matrix models are among the most widely used tools in ecology. Unfortunately, for the majority of pelagic marine organisms, it is difficult to mark individuals and follow them over time to determine their vital rates and built a population projection matrix model. Nevertheless, it is possible to get time-series data to calculate size structure and densities of each size, in order to determine the matrix parameters. This approach is known as a "demographic inverse problem" and it is based on quadratic programming methods, but it has rarely been used on aquatic organisms. We used unpublished field data of a population of cubomedusae Carybdea marsupialis to construct a population projection matrix model and compare two different management strategies to lower population to values before year 2008 when there was no significant interaction with bathers. Those strategies were by direct removal of medusae and by reducing prey. Our results showed that removal of jellyfish from all size classes was more effective than removing only juveniles or adults. When reducing prey, the highest efficiency to lower the C. marsupialis population occurred when prey depletion affected prey of all medusae sizes. Our model fit well with the field data and may serve to design an efficient management strategy or build hypothetical scenarios such as removal of individuals or reducing prey. TThis This sdfsdshis method is applicable to other marine or terrestrial species, for which density and population structure over time are available.

Generalized Wishart Mixtures for Unsupervised Classification of PolSAR Data

NASA Astrophysics Data System (ADS)

Li, Lan; Chen, Erxue; Li, Zengyuan

2013-01-01

This paper presents an unsupervised clustering algorithm based upon the expectation maximization (EM) algorithm for finite mixture modelling, using the complex wishart probability density function (PDF) for the probabilities. The mixture model enables to consider heterogeneous thematic classes which could not be better fitted by the unimodal wishart distribution. In order to make it fast and robust to calculate, we use the recently proposed generalized gamma distribution (GΓD) for the single polarization intensity data to make the initial partition. Then we use the wishart probability density function for the corresponding sample covariance matrix to calculate the posterior class probabilities for each pixel. The posterior class probabilities are used for the prior probability estimates of each class and weights for all class parameter updates. The proposed method is evaluated and compared with the wishart H-Alpha-A classification. Preliminary results show that the proposed method has better performance.

Infrared spectra and density functional calculations for SMO2 molecules (M = Cr, Mo, W).

PubMed

Wang, Xuefeng; Andrews, Lester

2009-08-06

Infrared absorptions of the matrix isolated SMO2 (M = Cr, Mo, W) molecules were observed following laser-ablated metal atom reactions with SO2 during condensation in solid argon and neon. The symmetric and antisymmetric M-O stretching mode assignments were confirmed by appropriate S18O2 and S(16,18)O2 isotopic shifts. The much weaker Cr-S stretching mode was identified through its 34S shift. Density functional (B3LYP and BPW91) calculations were performed to obtain molecular structures and to reproduce the infrared spectra. Computed pyramidal structures for the SMO2 molecules are very similar to those for the analogous trioxides and this functional group in [MO2S(bdt)]2- complexes. Additional weaker absorptions are assigned to the (SO2)(SMO2) adducts, which are stabilized by a four-membered ring.

A cubic scaling algorithm for excited states calculations in particle-particle random phase approximation

NASA Astrophysics Data System (ADS)

Lu, Jianfeng; Yang, Haizhao

2017-07-01

The particle-particle random phase approximation (pp-RPA) has been shown to be capable of describing double, Rydberg, and charge transfer excitations, for which the conventional time-dependent density functional theory (TDDFT) might not be suitable. It is thus desirable to reduce the computational cost of pp-RPA so that it can be efficiently applied to larger molecules and even solids. This paper introduces an O (N3) algorithm, where N is the number of orbitals, based on an interpolative separable density fitting technique and the Jacobi-Davidson eigensolver to calculate a few low-lying excitations in the pp-RPA framework. The size of the pp-RPA matrix can also be reduced by keeping only a small portion of orbitals with orbital energy close to the Fermi energy. This reduced system leads to a smaller prefactor of the cubic scaling algorithm, while keeping the accuracy for the low-lying excitation energies.

ELSI: A unified software interface for Kohn–Sham electronic structure solvers

DOE PAGES

Yu, Victor Wen-zhe; Corsetti, Fabiano; Garcia, Alberto; ...

2017-09-15

Solving the electronic structure from a generalized or standard eigenproblem is often the bottleneck in large scale calculations based on Kohn-Sham density-functional theory. This problem must be addressed by essentially all current electronic structure codes, based on similar matrix expressions, and by high-performance computation. We here present a unified software interface, ELSI, to access different strategies that address the Kohn-Sham eigenvalue problem. Currently supported algorithms include the dense generalized eigensolver library ELPA, the orbital minimization method implemented in libOMM, and the pole expansion and selected inversion (PEXSI) approach with lower computational complexity for semilocal density functionals. The ELSI interface aimsmore » to simplify the implementation and optimal use of the different strategies, by offering (a) a unified software framework designed for the electronic structure solvers in Kohn-Sham density-functional theory; (b) reasonable default parameters for a chosen solver; (c) automatic conversion between input and internal working matrix formats, and in the future (d) recommendation of the optimal solver depending on the specific problem. As a result, comparative benchmarks are shown for system sizes up to 11,520 atoms (172,800 basis functions) on distributed memory supercomputing architectures.« less

ELSI: A unified software interface for Kohn-Sham electronic structure solvers

NASA Astrophysics Data System (ADS)

Yu, Victor Wen-zhe; Corsetti, Fabiano; García, Alberto; Huhn, William P.; Jacquelin, Mathias; Jia, Weile; Lange, Björn; Lin, Lin; Lu, Jianfeng; Mi, Wenhui; Seifitokaldani, Ali; Vázquez-Mayagoitia, Álvaro; Yang, Chao; Yang, Haizhao; Blum, Volker

2018-01-01

Solving the electronic structure from a generalized or standard eigenproblem is often the bottleneck in large scale calculations based on Kohn-Sham density-functional theory. This problem must be addressed by essentially all current electronic structure codes, based on similar matrix expressions, and by high-performance computation. We here present a unified software interface, ELSI, to access different strategies that address the Kohn-Sham eigenvalue problem. Currently supported algorithms include the dense generalized eigensolver library ELPA, the orbital minimization method implemented in libOMM, and the pole expansion and selected inversion (PEXSI) approach with lower computational complexity for semilocal density functionals. The ELSI interface aims to simplify the implementation and optimal use of the different strategies, by offering (a) a unified software framework designed for the electronic structure solvers in Kohn-Sham density-functional theory; (b) reasonable default parameters for a chosen solver; (c) automatic conversion between input and internal working matrix formats, and in the future (d) recommendation of the optimal solver depending on the specific problem. Comparative benchmarks are shown for system sizes up to 11,520 atoms (172,800 basis functions) on distributed memory supercomputing architectures.

ELSI: A unified software interface for Kohn–Sham electronic structure solvers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yu, Victor Wen-zhe; Corsetti, Fabiano; Garcia, Alberto

Solving the electronic structure from a generalized or standard eigenproblem is often the bottleneck in large scale calculations based on Kohn-Sham density-functional theory. This problem must be addressed by essentially all current electronic structure codes, based on similar matrix expressions, and by high-performance computation. We here present a unified software interface, ELSI, to access different strategies that address the Kohn-Sham eigenvalue problem. Currently supported algorithms include the dense generalized eigensolver library ELPA, the orbital minimization method implemented in libOMM, and the pole expansion and selected inversion (PEXSI) approach with lower computational complexity for semilocal density functionals. The ELSI interface aimsmore » to simplify the implementation and optimal use of the different strategies, by offering (a) a unified software framework designed for the electronic structure solvers in Kohn-Sham density-functional theory; (b) reasonable default parameters for a chosen solver; (c) automatic conversion between input and internal working matrix formats, and in the future (d) recommendation of the optimal solver depending on the specific problem. As a result, comparative benchmarks are shown for system sizes up to 11,520 atoms (172,800 basis functions) on distributed memory supercomputing architectures.« less

Gradient-based stochastic estimation of the density matrix

NASA Astrophysics Data System (ADS)

Wang, Zhentao; Chern, Gia-Wei; Batista, Cristian D.; Barros, Kipton

2018-03-01

Fast estimation of the single-particle density matrix is key to many applications in quantum chemistry and condensed matter physics. The best numerical methods leverage the fact that the density matrix elements f(H)ij decay rapidly with distance rij between orbitals. This decay is usually exponential. However, for the special case of metals at zero temperature, algebraic decay of the density matrix appears and poses a significant numerical challenge. We introduce a gradient-based probing method to estimate all local density matrix elements at a computational cost that scales linearly with system size. For zero-temperature metals, the stochastic error scales like S-(d+2)/2d, where d is the dimension and S is a prefactor to the computational cost. The convergence becomes exponential if the system is at finite temperature or is insulating.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yanai, Takeshi; Fann, George I.; Beylkin, Gregory

Using the fully numerical method for time-dependent Hartree–Fock and density functional theory (TD-HF/DFT) with the Tamm–Dancoff (TD) approximation we use a multiresolution analysis (MRA) approach to present our findings. From a reformulation with effective use of the density matrix operator, we obtain a general form of the HF/DFT linear response equation in the first quantization formalism. It can be readily rewritten as an integral equation with the bound-state Helmholtz (BSH) kernel for the Green's function. The MRA implementation of the resultant equation permits excited state calculations without virtual orbitals. Moreover, the integral equation is efficiently and adaptively solved using amore » numerical multiresolution solver with multiwavelet bases. Our implementation of the TD-HF/DFT methods is applied for calculating the excitation energies of H 2, Be, N 2, H 2O, and C 2H 4 molecules. The numerical errors of the calculated excitation energies converge in proportion to the residuals of the equation in the molecular orbitals and response functions. The energies of the excited states at a variety of length scales ranging from short-range valence excitations to long-range Rydberg-type ones are consistently accurate. It is shown that the multiresolution calculations yield the correct exponential asymptotic tails for the response functions, whereas those computed with Gaussian basis functions are too diffuse or decay too rapidly. Finally, we introduce a simple asymptotic correction to the local spin-density approximation (LSDA) so that in the TDDFT calculations, the excited states are correctly bound.« less

Time-dependent quantum transport: An efficient method based on Liouville-von-Neumann equation for single-electron density matrix

NASA Astrophysics Data System (ADS)

Xie, Hang; Jiang, Feng; Tian, Heng; Zheng, Xiao; Kwok, Yanho; Chen, Shuguang; Yam, ChiYung; Yan, YiJing; Chen, Guanhua

2012-07-01

Basing on our hierarchical equations of motion for time-dependent quantum transport [X. Zheng, G. H. Chen, Y. Mo, S. K. Koo, H. Tian, C. Y. Yam, and Y. J. Yan, J. Chem. Phys. 133, 114101 (2010), 10.1063/1.3475566], we develop an efficient and accurate numerical algorithm to solve the Liouville-von-Neumann equation. We solve the real-time evolution of the reduced single-electron density matrix at the tight-binding level. Calculations are carried out to simulate the transient current through a linear chain of atoms, with each represented by a single orbital. The self-energy matrix is expanded in terms of multiple Lorentzian functions, and the Fermi distribution function is evaluated via the Padè spectrum decomposition. This Lorentzian-Padè decomposition scheme is employed to simulate the transient current. With sufficient Lorentzian functions used to fit the self-energy matrices, we show that the lead spectral function and the dynamics response can be treated accurately. Compared to the conventional master equation approaches, our method is much more efficient as the computational time scales cubically with the system size and linearly with the simulation time. As a result, the simulations of the transient currents through systems containing up to one hundred of atoms have been carried out. As density functional theory is also an effective one-particle theory, the Lorentzian-Padè decomposition scheme developed here can be generalized for first-principles simulation of realistic systems.

Matrix and energy effects during in-situ determination of Cu isotope ratios by ultraviolet-femtosecond laser ablation multicollector inductively coupled plasma mass spectrometry

NASA Astrophysics Data System (ADS)

Lazarov, Marina; Horn, Ingo

2015-09-01

Copper isotope compositions in Cu-bearing metals and minerals have been measured by deep (194 nm) ultraviolet femtosecond laser ablation multi-collector inductively coupled plasma mass spectrometry (UV-fsLA-MC-ICP-MS). Pure Cu-metal, brass, and several Cu-rich minerals (chalcopyrite, enargite, covellite, malachite and cuprite) have been investigated. A long-term reproducibility of better than 0.08‰ at the 95% confidence limit on the NIST SRM 976 (National Institute of Standards and Technology) Cu-metal standard has been achieved with this technique. The δ65Cu values for all samples have been calculated by standard-sample-standard bracketing with NIST SRM 976. All analyses have been carried out using Ni as a mass discrimination monitor added by nebulization prior to entering the plasma torch. For further verification samples have been analysed by conventional solution nebulization MC-ICP-MS and the results obtained have been compared with those from UV-fsLA-MC-ICP-MS. Several potential matrix-induced molecular interferences on the mineral copper isotope ratio, such as (32S33S)+ and (32S-16O17O)+ do not affect the Cu isotope measurements on sulfides, while hydrides, such as Zn-H or doubly-charged Sn2 + that interfere Ni isotopes can be either neglected or stripped by calculation. Matrix independent Cu-isotope measurements are sensitive to the energy density (fluence) applied onto the sample and can produce artificial shifts in the obtained δ65Cu values which are on the order of 3‰ for Cu-metal, 0.5‰ for brass and 0.3‰ for malachite when using energy density of up to 2 J/cm2 for ablation. A positive correlation between applied energy density and the magnitude of the isotope ratio shift has been found in the energy density range from 0.2 to 1.3 J/cm2 which is below the ablation threshold for ns-laser ablation. The results demonstrate that by using appropriate low fluence it is possible to measure Cu isotopic ratios in native copper and Cu-bearing sulfides, carbonates and oxides in situ with a precision of better than 0.1‰ (2SD) without using a matrix-matched standard during laser ablation analyses. Thus, this is a suitable tool to resolve Cu isotopic zoning larger than 0.1‰ in Cu-sulfides, carbonates and oxides.

Surface Snow Density of East Antarctica Derived from In-Situ Observations

NASA Astrophysics Data System (ADS)

Tian, Y.; Zhang, S.; Du, W.; Chen, J.; Xie, H.; Tong, X.; Li, R.

2018-04-01

Models based on physical principles or semi-empirical parameterizations have used to compute the firn density, which is essential for the study of surface processes in the Antarctic ice sheet. However, parameterization of surface snow density is often challenged by the description of detailed local characterization. In this study we propose to generate a surface density map for East Antarctica from all the filed observations that are available. Considering that the observations are non-uniformly distributed around East Antarctica, obtained by different methods, and temporally inhomogeneous, the field observations are used to establish an initial density map with a grid size of 30 × 30 km2 in which the observations are averaged at a temporal scale of five years. We then construct an observation matrix with its columns as the map grids and rows as the temporal scale. If a site has an unknown density value for a period, we will set it to 0 in the matrix. In order to construct the main spatial and temple information of surface snow density matrix we adopt Empirical Orthogonal Function (EOF) method to decompose the observation matrix and only take first several lower-order modes, because these modes already contain most information of the observation matrix. However, there are a lot of zeros in the matrix and we solve it by using matrix completion algorithm, and then we derive the time series of surface snow density at each observation site. Finally, we can obtain the surface snow density by multiplying the modes interpolated by kriging with the corresponding amplitude of the modes. Comparative analysis have done between our surface snow density map and model results. The above details will be introduced in the paper.

Effects of increased collagen-matrix density on the mechanical properties and in vivo absorbability of hydroxyapatite-collagen composites as artificial bone materials.

PubMed

Yunoki, Shunji; Sugiura, Hiroaki; Ikoma, Toshiyuki; Kondo, Eiji; Yasuda, Kazunori; Tanaka, Junzo

2011-02-01

The aim of this study was to evaluate the effects of increased collagen-matrix density on the mechanical properties and in vivo absorbability of porous hydroxyapatite (HAp)-collagen composites as artificial bone materials. Seven types of porous HAp-collagen composites were prepared from HAp nanocrystals and dense collagen fibrils. Their densities and HAp/collagen weight ratios ranged from 122 to 331 mg cm⁻³ and from 20/80 to 80/20, respectively. The flexural modulus and strength increased with an increase in density, reaching 2.46 ± 0.48 and 0.651 ± 0.103 MPa, respectively. The porous composites with a higher collagen-matrix density exhibited much higher mechanical properties at the same densities, suggesting that increasing the collagen-matrix density is an effective way of improving the mechanical properties. It was also suggested that other structural factors in addition to collagen-matrix density are required to achieve bone-like mechanical properties. The in vivo absorbability of the composites was investigated in bone defects of rabbit femurs, demonstrating that the absorption rate decreased with increases in the composite density. An exhaustive increase in density is probably limited by decreases in absorbability as artificial bones.

Ab initio molecular dynamics in a finite homogeneous electric field.

PubMed

Umari, P; Pasquarello, Alfredo

2002-10-07

We treat homogeneous electric fields within density functional calculations with periodic boundary conditions. A nonlocal energy functional depending on the applied field is used within an ab initio molecular dynamics scheme. The reliability of the method is demonstrated in the case of bulk MgO for the Born effective charges, and the high- and low-frequency dielectric constants. We evaluate the static dielectric constant by performing a damped molecular dynamics in an electric field and avoiding the calculation of the dynamical matrix. Application of this method to vitreous silica shows good agreement with experiment and illustrates its potential for systems of large size.

Single inclusive jet production and the nuclear modification ratio at very forward rapidity in proton-lead collisions with √{sNN } = 5.02 TeV

NASA Astrophysics Data System (ADS)

Bury, Marcin; Van Haevermaet, Hans; Van Hameren, Andreas; Van Mechelen, Pierre; Kutak, Krzysztof; Serino, Mirko

2018-05-01

We present calculations of single inclusive jet transverse momentum and energy spectra at forward rapidity (5.2 < y < 6.6) in proton-lead collisions with √{sNN } = 5.02 TeV. The predictions are obtained with the KaTie Monte Carlo event generator, which allows to calculate interactions within the High Energy Factorisation framework. The tree-level matrix element results are subsequently interfaced with the CASCADE Monte Carlo event generator to account for hadronisation. The effects of the saturation of the gluon density, leading to suppression of the cross section, are investigated.

Tailoring of physical properties in highly filled experimental nanohybrid resin composites.

PubMed

Pick, Bárbara; Pelka, Matthias; Belli, Renan; Braga, Roberto R; Lohbauer, Ulrich

2011-07-01

To assess the elastic modulus (EM), volumetric shrinkage (VS), and polymerization shrinkage stress (PSS) of experimental highly filled nanohybrid composites as a function of matrix composition, filler distribution, and density. One regular viscosity nanohybrid composite (Grandio, VOCO, Germany) and one flowable nanohybrid composite (Grandio Flow, VOCO) were tested as references along with six highly filled experimental nanohybrid composites (four Bis-GMA-based, one UDMA-based, and one Ormocer®-based). The experimental composites varied in filler size and density. EM values were obtained from the "three-point bending" load-displacement curve. VS was calculated with Archimedes' buoyancy principle. PSS was determined in 1-mm thick specimens placed between two (poly)methyl methacrylate rods (Ø=6mm) attached to an universal testing machine. Data were analyzed using oneway ANOVA, Tukey's test (α=0.05), and linear regression analyses. The flowable composite exhibited the highest VS and PSS but lowest EM. The PSS was significantly lower with Ormocer. The EM was significantly higher among experimental composites with highest filler levels. No significant differences were found between all other experimental composites regarding VS and PSS. Filler density and size did not influence EM, VS, or PSS. Neither the filler configuration nor matrix composition in the investigated materials significantly influenced composite shrinkage and mechanical properties. The highest filled experimental composite seemed to increase EM by keeping VS and PSS low; however, matrix composition seemed to be the determinant factor for shrinkage and stress development. The Ormocer, with reduced PSS, deserves further investigation. Filler size and density did not influence the tested parameters. Copyright © 2011 Academy of Dental Materials. Published by Elsevier Ltd. All rights reserved.

Direct Measurement of the Density Matrix of a Quantum System

NASA Astrophysics Data System (ADS)

Thekkadath, G. S.; Giner, L.; Chalich, Y.; Horton, M. J.; Banker, J.; Lundeen, J. S.

2016-09-01

One drawback of conventional quantum state tomography is that it does not readily provide access to single density matrix elements since it requires a global reconstruction. Here, we experimentally demonstrate a scheme that can be used to directly measure individual density matrix elements of general quantum states. The scheme relies on measuring a sequence of three observables, each complementary to the last. The first two measurements are made weak to minimize the disturbance they cause to the state, while the final measurement is strong. We perform this joint measurement on polarized photons in pure and mixed states to directly measure their density matrix. The weak measurements are achieved using two walk-off crystals, each inducing a polarization-dependent spatial shift that couples the spatial and polarization degrees of freedom of the photons. This direct measurement method provides an operational meaning to the density matrix and promises to be especially useful for large dimensional states.

Direct Measurement of the Density Matrix of a Quantum System.

PubMed

Thekkadath, G S; Giner, L; Chalich, Y; Horton, M J; Banker, J; Lundeen, J S

2016-09-16

One drawback of conventional quantum state tomography is that it does not readily provide access to single density matrix elements since it requires a global reconstruction. Here, we experimentally demonstrate a scheme that can be used to directly measure individual density matrix elements of general quantum states. The scheme relies on measuring a sequence of three observables, each complementary to the last. The first two measurements are made weak to minimize the disturbance they cause to the state, while the final measurement is strong. We perform this joint measurement on polarized photons in pure and mixed states to directly measure their density matrix. The weak measurements are achieved using two walk-off crystals, each inducing a polarization-dependent spatial shift that couples the spatial and polarization degrees of freedom of the photons. This direct measurement method provides an operational meaning to the density matrix and promises to be especially useful for large dimensional states.

A Sparse Self-Consistent Field Algorithm and Its Parallel Implementation: Application to Density-Functional-Based Tight Binding.

PubMed

Scemama, Anthony; Renon, Nicolas; Rapacioli, Mathias

2014-06-10

We present an algorithm and its parallel implementation for solving a self-consistent problem as encountered in Hartree-Fock or density functional theory. The algorithm takes advantage of the sparsity of matrices through the use of local molecular orbitals. The implementation allows one to exploit efficiently modern symmetric multiprocessing (SMP) computer architectures. As a first application, the algorithm is used within the density-functional-based tight binding method, for which most of the computational time is spent in the linear algebra routines (diagonalization of the Fock/Kohn-Sham matrix). We show that with this algorithm (i) single point calculations on very large systems (millions of atoms) can be performed on large SMP machines, (ii) calculations involving intermediate size systems (1000-100 000 atoms) are also strongly accelerated and can run efficiently on standard servers, and (iii) the error on the total energy due to the use of a cutoff in the molecular orbital coefficients can be controlled such that it remains smaller than the SCF convergence criterion.

Self-Avoiding Walks on the Random Lattice and the Random Hopping Model on a Cayley Tree

NASA Astrophysics Data System (ADS)

Kim, Yup

Using a field theoretic method based on the replica trick, it is proved that the three-parameter renormalization group for an n-vector model with quenched randomness reduces to a two-parameter one in the limit n (--->) 0 which corresponds to self-avoiding walks (SAWs). This is also shown by the explicit calculation of the renormalization group recursion relations to second order in (epsilon). From this reduction we find that SAWs on the random lattice are in the same universality class as SAWs on the regular lattice. By analogy with the case of the n-vector model with cubic anisotropy in the limit n (--->) 1, the fixed-point structure of the n-vector model with randomness is analyzed in the SAW limit, so that a physical interpretation of the unphysical fixed point is given. Corrections of the values of critical exponents of the unphysical fixed point published previously is also given. Next we formulate an integral equation and recursion relations for the configurationally averaged one particle Green's function of the random hopping model on a Cayley tree of coordination number ((sigma) + 1). This formalism is tested by applying it successfully to the nonrandom model. Using this scheme for 1 << (sigma) < (INFIN) we calculate the density of states of this model with a Gaussian distribution of hopping matrix elements in the range of energy E('2) > E(,c)('2), where E(,c) is a critical energy described below. The singularity in the Green's function which occurs at energy E(,1)('(0)) for (sigma) = (INFIN) is shifted to complex energy E(,1) (on the unphysical sheet of energy E) for small (sigma)('-1). This calculation shows that the density of states is smooth function of energy E around the critical energy E(,c) = Re E(,1) in accord with Wegner's theorem. In this formulation the density of states has no sharp phase transition on the real axis of E because E(,1) has developed an imaginary part. Using the Lifschitz argument, we calculate the density of states near the band edge for the model when the hopping matrix elements are governed by a bounded probability distribution. It is also shown within the dynamical system language that the density of states of the model with a bounded distribution never vanishes inside the band and we suggest a theoretical mechanism for the formation of energy bands.

Application of relativistic mean field and effective field theory densities to scattering observables for Ca isotopes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bhuyan, M.; School of Physics, Sambalpur University, Jyotivihar, Burla 768 019; Panda, R. N.

In the framework of relativistic mean field (RMF) theory, we have calculated the density distribution of protons and neutrons for {sup 40,42,44,48}Ca with NL3 and G2 parameter sets. The microscopic proton-nucleus optical potentials for p+{sup 40,42,44,48}Ca systems are evaluated from the Dirac nucleon-nucleon scattering amplitude and the density of the target nucleus using relativistic-Love-Franey and McNeil-Ray-Wallace parametrizations. We have estimated the scattering observables, such as the elastic differential scattering cross section, analyzing power and the spin observables with the relativistic impulse approximation (RIA). The results have been compared with the experimental data for a few selective cases and we findmore » that the use of density as well as the scattering matrix parametrizations are crucial for the theoretical prediction.« less

Accurate Semilocal Density Functional for Condensed-Matter Physics and Quantum Chemistry.

PubMed

Tao, Jianmin; Mo, Yuxiang

2016-08-12

Most density functionals have been developed by imposing the known exact constraints on the exchange-correlation energy, or by a fit to a set of properties of selected systems, or by both. However, accurate modeling of the conventional exchange hole presents a great challenge, due to the delocalization of the hole. Making use of the property that the hole can be made localized under a general coordinate transformation, here we derive an exchange hole from the density matrix expansion, while the correlation part is obtained by imposing the low-density limit constraint. From the hole, a semilocal exchange-correlation functional is calculated. Our comprehensive test shows that this functional can achieve remarkable accuracy for diverse properties of molecules, solids, and solid surfaces, substantially improving upon the nonempirical functionals proposed in recent years. Accurate semilocal functionals based on their associated holes are physically appealing and practically useful for developing nonlocal functionals.

Quantum confinement effects on electronic photomobilities at nanostructured semiconductor surfaces: Si(111) without and with adsorbed Ag clusters

NASA Astrophysics Data System (ADS)

Hembree, Robert H.; Vazhappilly, Tijo; Micha, David A.

2017-12-01

The conductivity of holes and electrons photoexcited in Si slabs is affected by the slab thickness and by adsorbates. The mobilities of those charged carriers depend on how many layers compose the slab, and this has important scientific and technical consequences for the understanding of photovoltaic materials. A previously developed general computational procedure combining density matrix and electronic band structure treatments has been applied to extensive calculations of mobilities of photoexcited electrons and holes at Si(111) nanostructured surfaces with varying slab thickness and for varying photon energies, to investigate the expected change in mobility magnitudes as the slab thickness is increased. Results have been obtained with and without adsorbed silver clusters for comparison of their optical and photovoltaic properties. Band states were generated using a modified ab initio density functional treatment with the PBE exchange and correlation density functionals and with periodic boundary conditions for large atomic supercells. An energy gap correction was applied to the unoccupied orbital energies of each band structure by running more accurate HSE hybrid functional calculations for a Si(111) slab. Photoexcited state populations for slabs with 6, 8, 10, and 12 layers were generated using a steady state reduced density matrix including dissipative effects due to energy exchange with excitons and phonons in the medium. Mobilities have been calculated from the derivatives of voltage-driven electronic energies with respect to electronic momentum, for each energy band and for the average over bands. Results show two clear trends: (a) adding Ag increases the hole photomobilities and (b) decreasing the slab thickness increases hole photomobilities. The increased hole populations in 6- and 8-layer systems and the large increase in hole mobility for these thinner slabs can be interpreted as a quantum confinement effect of hole orbitals. As the slab thickness increases to ten and twelve layers, the effect of silver adsorbates decreases leading to smaller relative enhancements to the conduction electron and hole mobilities, but the addition of the silver nanoclusters still increases the absorbance of light and the mobility of holes compared to their mobilities in the pure Si slabs.

Excitation rate coefficients and line ratios for the optical and ultraviolet transitions in S II

NASA Technical Reports Server (NTRS)

Cai, Wei; Pradhan, Anil K.

1993-01-01

New calculations are reported for electron excitation collision strengths, rate coefficients, transition probabilities, and line ratios for the astrophysically important optical and UV lines in S II. The collision strengths are calculated in the close coupling approximation using the R-matrix method. The present calculations are more extensive than previous ones, including all transitions among the 12 lowest LS terms and the corresponding 28 fine-structure levels in the collisional-radiative model for S II. While the present rate coefficients for electron impact excitation are within 10-30 percent of the previous values for the low-lying optical transitions employed as density diagnostics of H II regions and nebulae, the excitation rates for the UV transitions 4S super 0 sub 3/2 - 4Psub 1/2,3/2,5/2 differ significantly from earlier calculations, by up to factor of 2. We describe temperature and density sensitive flux ratios for a number of UV lines. The present UV results are likely to be of interest in a more accurate interpretation of S II emission from the Io plasma torus in the magnetosphere of Jupiter, as well as other UV sources observed from the IUE, ASTRO 1, and the HST.

Model representations of kerogen structures: An insight from density functional theory calculations and spectroscopic measurements

DOE PAGES

Weck, Philippe F.; Kim, Eunja; Wang, Yifeng; ...

2017-08-01

Molecular structures of kerogen control hydrocarbon production in unconventional reservoirs. Significant progress has been made in developing model representations of various kerogen structures. These models have been widely used for the prediction of gas adsorption and migration in shale matrix. However, using density functional perturbation theory (DFPT) calculations and vibrational spectroscopic measurements, we here show that a large gap may still remain between the existing model representations and actual kerogen structures, therefore calling for new model development. Using DFPT, we calculated Fourier transform infrared (FTIR) spectra for six most widely used kerogen structure models. The computed spectra were then systematicallymore » compared to the FTIR absorption spectra collected for kerogen samples isolated from Mancos, Woodford and Marcellus formations representing a wide range of kerogen origin and maturation conditions. Limited agreement between the model predictions and the measurements highlights that the existing kerogen models may still miss some key features in structural representation. A combination of DFPT calculations with spectroscopic measurements may provide a useful diagnostic tool for assessing the adequacy of a proposed structural model as well as for future model development. This approach may eventually help develop comprehensive infrared (IR)-fingerprints for tracing kerogen evolution.« less

Model representations of kerogen structures: An insight from density functional theory calculations and spectroscopic measurements.

PubMed

Weck, Philippe F; Kim, Eunja; Wang, Yifeng; Kruichak, Jessica N; Mills, Melissa M; Matteo, Edward N; Pellenq, Roland J-M

2017-08-01

Molecular structures of kerogen control hydrocarbon production in unconventional reservoirs. Significant progress has been made in developing model representations of various kerogen structures. These models have been widely used for the prediction of gas adsorption and migration in shale matrix. However, using density functional perturbation theory (DFPT) calculations and vibrational spectroscopic measurements, we here show that a large gap may still remain between the existing model representations and actual kerogen structures, therefore calling for new model development. Using DFPT, we calculated Fourier transform infrared (FTIR) spectra for six most widely used kerogen structure models. The computed spectra were then systematically compared to the FTIR absorption spectra collected for kerogen samples isolated from Mancos, Woodford and Marcellus formations representing a wide range of kerogen origin and maturation conditions. Limited agreement between the model predictions and the measurements highlights that the existing kerogen models may still miss some key features in structural representation. A combination of DFPT calculations with spectroscopic measurements may provide a useful diagnostic tool for assessing the adequacy of a proposed structural model as well as for future model development. This approach may eventually help develop comprehensive infrared (IR)-fingerprints for tracing kerogen evolution.

Model representations of kerogen structures: An insight from density functional theory calculations and spectroscopic measurements

DOE Office of Scientific and Technical Information (OSTI.GOV)

Weck, Philippe F.; Kim, Eunja; Wang, Yifeng

Molecular structures of kerogen control hydrocarbon production in unconventional reservoirs. Significant progress has been made in developing model representations of various kerogen structures. These models have been widely used for the prediction of gas adsorption and migration in shale matrix. However, using density functional perturbation theory (DFPT) calculations and vibrational spectroscopic measurements, we here show that a large gap may still remain between the existing model representations and actual kerogen structures, therefore calling for new model development. Using DFPT, we calculated Fourier transform infrared (FTIR) spectra for six most widely used kerogen structure models. The computed spectra were then systematicallymore » compared to the FTIR absorption spectra collected for kerogen samples isolated from Mancos, Woodford and Marcellus formations representing a wide range of kerogen origin and maturation conditions. Limited agreement between the model predictions and the measurements highlights that the existing kerogen models may still miss some key features in structural representation. A combination of DFPT calculations with spectroscopic measurements may provide a useful diagnostic tool for assessing the adequacy of a proposed structural model as well as for future model development. This approach may eventually help develop comprehensive infrared (IR)-fingerprints for tracing kerogen evolution.« less

Addressing the computational cost of large EIT solutions.

PubMed

Boyle, Alistair; Borsic, Andrea; Adler, Andy

2012-05-01

Electrical impedance tomography (EIT) is a soft field tomography modality based on the application of electric current to a body and measurement of voltages through electrodes at the boundary. The interior conductivity is reconstructed on a discrete representation of the domain using a finite-element method (FEM) mesh and a parametrization of that domain. The reconstruction requires a sequence of numerically intensive calculations. There is strong interest in reducing the cost of these calculations. An improvement in the compute time for current problems would encourage further exploration of computationally challenging problems such as the incorporation of time series data, wide-spread adoption of three-dimensional simulations and correlation of other modalities such as CT and ultrasound. Multicore processors offer an opportunity to reduce EIT computation times but may require some restructuring of the underlying algorithms to maximize the use of available resources. This work profiles two EIT software packages (EIDORS and NDRM) to experimentally determine where the computational costs arise in EIT as problems scale. Sparse matrix solvers, a key component for the FEM forward problem and sensitivity estimates in the inverse problem, are shown to take a considerable portion of the total compute time in these packages. A sparse matrix solver performance measurement tool, Meagre-Crowd, is developed to interface with a variety of solvers and compare their performance over a range of two- and three-dimensional problems of increasing node density. Results show that distributed sparse matrix solvers that operate on multiple cores are advantageous up to a limit that increases as the node density increases. We recommend a selection procedure to find a solver and hardware arrangement matched to the problem and provide guidance and tools to perform that selection.

Fragment approach to constrained density functional theory calculations using Daubechies wavelets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ratcliff, Laura E.; Genovese, Luigi; Mohr, Stephan

2015-06-21

In a recent paper, we presented a linear scaling Kohn-Sham density functional theory (DFT) code based on Daubechies wavelets, where a minimal set of localized support functions are optimized in situ and therefore adapted to the chemical properties of the molecular system. Thanks to the systematically controllable accuracy of the underlying basis set, this approach is able to provide an optimal contracted basis for a given system: accuracies for ground state energies and atomic forces are of the same quality as an uncontracted, cubic scaling approach. This basis set offers, by construction, a natural subset where the density matrix ofmore » the system can be projected. In this paper, we demonstrate the flexibility of this minimal basis formalism in providing a basis set that can be reused as-is, i.e., without reoptimization, for charge-constrained DFT calculations within a fragment approach. Support functions, represented in the underlying wavelet grid, of the template fragments are roto-translated with high numerical precision to the required positions and used as projectors for the charge weight function. We demonstrate the interest of this approach to express highly precise and efficient calculations for preparing diabatic states and for the computational setup of systems in complex environments.« less

Use of radial symmetry for the calculation of cylindrical absorption coefficients and optimal capillary loadings

DOE PAGES

Khalifah, Peter

2015-02-01

The problem of numerically evaluating absorption correction factors for cylindrical samples has been revisited using a treatment that fully takes advantage of the sample symmetry. It is shown that the path lengths for all points within the sample at all possible diffraction angles can be trivially determined once the angle-dependent distance distribution for a single line of points is calculated. This provides advantages in both computational efficiency and in gaining an intuitive understanding of the effects of absorption on diffraction data. A matrix of absorption coefficients calculated for µR products between 0 and 20 for diffraction angles θ D ofmore » 0° to 90° were used to examine the influence of (1) capillary diameter and of (2) sample density on the overall scattered intensity as a function of diffraction angle, where µ is the linear absorption coefficient for the sample and R is the capillary radius. Based on this analysis, the optimal sample loading for a capillary experiment to maximize diffraction at angles of 0 – 50° is in general expected to be achieved when the maximum radius capillary compatible with the beam is used, and when the sample density is adjusted to be 3/(4µR) of its original density.« less

First-principles method for calculating the rate constants of internal-conversion and intersystem-crossing transitions.

PubMed

Valiev, R R; Cherepanov, V N; Baryshnikov, G V; Sundholm, D

2018-02-28

A method for calculating the rate constants for internal-conversion (k IC ) and intersystem-crossing (k ISC ) processes within the adiabatic and Franck-Condon (FC) approximations is proposed. The applicability of the method is demonstrated by calculation of k IC and k ISC for a set of organic and organometallic compounds with experimentally known spectroscopic properties. The studied molecules were pyrromethene-567 dye, psoralene, hetero[8]circulenes, free-base porphyrin, naphthalene, and larger polyacenes. We also studied fac-Alq 3 and fac-Ir(ppy) 3 , which are important molecules in organic light emitting diodes (OLEDs). The excitation energies were calculated at the multi-configuration quasi-degenerate second-order perturbation theory (XMC-QDPT2) level, which is found to yield excitation energies in good agreement with experimental data. Spin-orbit coupling matrix elements, non-adiabatic coupling matrix elements, Huang-Rhys factors, and vibrational energies were calculated at the time-dependent density functional theory (TDDFT) and complete active space self-consistent field (CASSCF) levels. The computed fluorescence quantum yields for the pyrromethene-567 dye, psoralene, hetero[8]circulenes, fac-Alq 3 and fac-Ir(ppy) 3 agree well with experimental data, whereas for the free-base porphyrin, naphthalene, and the polyacenes, the obtained quantum yields significantly differ from the experimental values, because the FC and adiabatic approximations are not accurate for these molecules.

Relative Contribution of Matrix Structure, Patch Resources and Management to the Local Densities of Two Large Blue Butterfly Species

PubMed Central

Skórka, Piotr; Nowicki, Piotr; Bonk, Maciej; Król, Wiesław; Szpiłyk, Damian; Woyciechowski, Michal

2016-01-01

The type of matrix, the landscape surrounding habitat patches, may determine the distribution and function of local populations. However, the matrix is often heterogeneous, and its various components may differentially contribute to metapopulation processes at different spatial scales, a phenomenon that has rarely been investigated. The aim of this study was to estimate the relative importance of matrix composition and spatial scale, habitat quality, and management intensity on the occurrence and density of local populations of two endangered large blue butterflies: Phengaris teleius and P. nausithous. Presence and abundance data were assessed over two years, 2011–12, in 100 local patches within two heterogeneous regions (near Kraków and Tarnów, southern Poland). The matrix composition was analyzed at eight spatial scales. We observed high occupancy rates in both species, regions and years. With the exception of area and isolation, almost all of the matrix components contributed to Phengaris sp. densities. The different matrix components acted at different spatial scales (grassland cover within 4 and 3 km, field cover within 0.4 and 0.3 km and water cover within 4 km radii for P. teleius and P. nausithous, respectively) and provided the highest independent contribution to the butterfly densities. Additionally, the effects of a 0.4 km radius of forest cover and a food plant cover on P. teleius, and a 1 km radius of settlement cover and management intensity on P. nausithous densities were observed. Contrary to former studies we conclude that the matrix heterogeneity and spatial scale rather than general matrix type are of relevance for densities of butterflies. Conservation strategies for these umbrella species should concentrate on maintaining habitat quality and managing matrix composition at the most appropriate spatial scales. PMID:28005942

Relative Contribution of Matrix Structure, Patch Resources and Management to the Local Densities of Two Large Blue Butterfly Species.

PubMed

Kajzer-Bonk, Joanna; Skórka, Piotr; Nowicki, Piotr; Bonk, Maciej; Król, Wiesław; Szpiłyk, Damian; Woyciechowski, Michal

2016-01-01

The type of matrix, the landscape surrounding habitat patches, may determine the distribution and function of local populations. However, the matrix is often heterogeneous, and its various components may differentially contribute to metapopulation processes at different spatial scales, a phenomenon that has rarely been investigated. The aim of this study was to estimate the relative importance of matrix composition and spatial scale, habitat quality, and management intensity on the occurrence and density of local populations of two endangered large blue butterflies: Phengaris teleius and P. nausithous. Presence and abundance data were assessed over two years, 2011-12, in 100 local patches within two heterogeneous regions (near Kraków and Tarnów, southern Poland). The matrix composition was analyzed at eight spatial scales. We observed high occupancy rates in both species, regions and years. With the exception of area and isolation, almost all of the matrix components contributed to Phengaris sp. densities. The different matrix components acted at different spatial scales (grassland cover within 4 and 3 km, field cover within 0.4 and 0.3 km and water cover within 4 km radii for P. teleius and P. nausithous, respectively) and provided the highest independent contribution to the butterfly densities. Additionally, the effects of a 0.4 km radius of forest cover and a food plant cover on P. teleius, and a 1 km radius of settlement cover and management intensity on P. nausithous densities were observed. Contrary to former studies we conclude that the matrix heterogeneity and spatial scale rather than general matrix type are of relevance for densities of butterflies. Conservation strategies for these umbrella species should concentrate on maintaining habitat quality and managing matrix composition at the most appropriate spatial scales.

Ammonium nitrate-polymer glasses: a new concept for phase and thermal stabilization of ammonium nitrate.

PubMed

Lang, Anthony J; Vyazovkin, Sergey

2008-09-11

Dissolving of ammonium nitrate in highly polar polymers such as poly(vinylpyrrolidone) and/or poly(acrylamide) can result in the formation of single-phase glassy solid materials, in which NH 4 (+) and NO 3 (-) are separated through an ion-dipole interaction with the polymer matrix. Below the glass transition temperature of the polymer matrix the resulting materials remain phase and thermally stable as demonstrated through the absence of decomposition as well as the solid-solid transitions and melting of ammonium nitrate. The structure of the materials is explored by Fourier transform infrared spectroscopy and density functional calculations. Differential scanning calorimetry, thermogravimetry, and isoconversional kinetic analysis are applied to characterize the thermal behavior of the materials.

Understanding the inelastic electron-tunneling spectra of alkanedithiols on gold.

PubMed

Solomon, Gemma C; Gagliardi, Alessio; Pecchia, Alessandro; Frauenheim, Thomas; Di Carlo, Aldo; Reimers, Jeffrey R; Hush, Noel S

2006-03-07

We present results for a simulated inelastic electron-tunneling spectra (IETS) from calculations using the "gDFTB" code. The geometric and electronic structure is obtained from calculations using a local-basis density-functional scheme, and a nonequilibrium Green's function formalism is employed to deal with the transport aspects of the problem. The calculated spectrum of octanedithiol on gold(111) shows good agreement with experimental results and suggests further details in the assignment of such spectra. We show that some low-energy peaks, unassigned in the experimental spectrum, occur in a region where a number of molecular modes are predicted to be active, suggesting that these modes are the cause of the peaks rather than a matrix signal, as previously postulated. The simulations also reveal the qualitative nature of the processes dominating IETS. It is highly sensitive only to the vibrational motions that occur in the regions of the molecule where there is electron density in the low-voltage conduction channel. This result is illustrated with an examination of the predicted variation of IETS with binding site and alkane chain length.

Effective Elastic and Neutron Capture Cross Section Calculations Corresponding to Simulated Fluid Properties from CO2 Push-Pull Simulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chugunov, Nikita; Altundas, Bilgin

The submission contains a .xls files consisting of 10 excel sheets, which contain combined list of pressure, saturation, salinity, temperature profiles from the simulation of CO2 push-pull using Brady reservoir model and the corresponding effective compressional and shear velocity, bulk density, and fluid and time-lapse neutron capture cross section profiles of rock at times 0 day (baseline) through 14 days. First 9 sheets (each named after the corresponding CO2 push-pull simulation time) contains simulated pressure, saturation, temperature, salinity profiles and the corresponding effective elastic and neutron capture cross section profiles of rock matrix at the time of CO2 injection. Eachmore » sheet contains two sets of effective compressional velocity profiles of the rock, one based on Gassmann and the other based on Patchy saturation model. Effective neutron capture cross section calculations are done using a proprietary neutron cross-section simulator (SNUPAR) whereas for the thermodynamic properties of CO2 and bulk density of rock matrix filled with fluid, a standalone fluid substitution tool by Schlumberger is used. Last sheet in the file contains the bulk modulus of solid rock, which is inverted from the rock properties (porosity, sound speed etc) based on Gassmann model. Bulk modulus of solid rock in turn is used in the fluid substitution.« less

Infrared Spectrum and UV-Induced Photochemistry of Matrix-Isolated 5-Hydroxyquinoline.

PubMed

Kuş, Nihal; Sagdinc, Seda; Fausto, Rui

2015-06-18

The structure, infrared spectrum, and photochemistry of 5-hydroxyquinoline (5HQ) were studied by matrix isolation infrared spectroscopy, complemented by theoretical calculations performed at the DFT(B3LYP)/6-311++G(d,p) level of approximation. According to the calculations, the trans conformer of 5HQ (with the OH group pointing to the opposite direction of the pyridine ring of the molecule) is more stable than the cis form (by ∼8.8 kJ mol(-1)). The main factors determining the relative stability of the two conformers were rationalized through natural bond orbital (NBO) and charge density analyses. The compound was trapped in solid nitrogen at 10 K, and its infrared spectra registered and interpreted, showing the sole presence in the matrix of the more stable trans conformer. Broadband in situ UV irradiations (λ ≥ 288 nm and λ ≥ 235 nm) allowed for the observation of different chemical transformations, which started by excitation to the S1 state of 5HQ, followed by homolytic cleavage of the O-H bond, and subsequent reattachment of the H atom to the 5HQ radical to form quinolin-5(6H)-one and quinolin-5(8H)-one. The first of these two quinolinones was found to convert to open-ring isomeric ketenes, especially when irradiation was performed at higher energy, whereas the second is rather stable under the used experimental conditions. As a whole, the observed photochemistry of matrix-isolated 5HQ closely matches those previously reported for phenol and thiophenol. A detailed mechanistic interpretation for the observed photochemical processes is here proposed, which received support from time-dependent DFT calculations.

Water in the presence of inert Lennard-Jones obstacles

NASA Astrophysics Data System (ADS)

Kurtjak, Mario; Urbic, Tomaz

2014-04-01

Water confined by the presence of a 'sea' of inert obstacles was examined. In the article, freely mobile two-dimensional Mercedes-Benz (MB) water put to a disordered, but fixed, matrix of Lennard-Jones disks was studied by the Monte Carlo computer simulations. For the MB water molecules in the matrix of Lennard-Jones disks, we explored the structures, hydrogen-bond-network formation and thermodynamics as a function of temperature and size and density of matrix particles. We found that the structure of model water is perturbed by the presence of the obstacles. Density of confined water, which was in equilibrium with the bulk water, was smaller than the density of the bulk water and the temperature dependence of the density of absorbed water did not show the density anomaly in the studied temperature range. The behaviour observed as a consequence of confinement is similar to that of increasing temperature, which can for a matrix lead to a process similar to capillary evaporation. At the same occupancy of space, smaller matrix molecules cause higher destruction effect on the absorbed water molecules than the bigger ones. We have also tested the hypothesis that at low matrix densities the obstacles induce an increased ordering and 'hydrogen bonding' of the MB model molecules, relative to pure fluid, while at high densities the obstacles reduce MB water structuring, as they prevent the fluid to form good 'hydrogen-bonding' networks. However, for the size of matrix molecules similar to that of water, we did not observe this effect.

Image-based 3D modeling study of the influence of vessel density and blood hemoglobin concentration on tumor oxygenation and response to irradiation.

PubMed

Lagerlöf, Jakob H; Kindblom, Jon; Cortez, Eliane; Pietras, Kristian; Bernhardt, Peter

2013-02-01

Hypoxia is one of the most important factors influencing clinical outcome after radiotherapy. Improved knowledge of factors affecting the levels and distribution of oxygen within a tumor is needed. The authors constructed a theoretical 3D model based on histological images to analyze the influence of vessel density and hemoglobin (Hb) concentration on the response to irradiation. The pancreases of a Rip-Tag2 mouse, a model of malignant insulinoma, were excised, cryosectioned, immunostained, and photographed. Vessels were identified by image thresholding and a 3D vessel matrix assembled. The matrix was reduced to functional vessel segments and enlarged by replication. The steady-state oxygen tension field of the tumor was calculated by iteratively employing Green's function method for diffusion and the Michaelis-Menten model for consumption. The impact of vessel density on the radiation response was studied by removing a number of randomly selected vessels. The impact of Hb concentration was studied by independently changing vessel oxygen partial pressure (pO(2)). For each oxygen distribution, the oxygen enhancement ratio (OER) was calculated and the mean absorbed dose at which the tumor control probability (TCP) was 0.99 (D(99)) was determined using the linear-quadratic cell survival model (LQ model). Decreased pO(2) shifted the oxygen distribution to lower values, whereas decreased vessel density caused the distribution to widen and shift to lower values. Combined scenarios caused lower-shifted distributions, emphasising log-normal characteristics. Vessel reduction combined with increased blood pO(2) caused the distribution to widen due to a lack of vessels. The most pronounced radiation effect of increased pO(2) occurred with tumor tissue with 50% of the maximum vessel density used in the simulations. A 51% decrease in D(99), from 123 to 60 Gy, was found between the lowest and highest pO(2) concentrations. Our results indicate that an intermediate vascular density region exists where enhanced blood oxygen concentration may be beneficial for radiation response. The results also suggest that it is possible to distinguish between diffusion-limited and anemic hypoxia from the characteristics of the pO(2) distribution.

Identification of metal s states in Sn-doped anatase by polarisation dependent hard X-ray photoelectron spectroscopy

NASA Astrophysics Data System (ADS)

Regoutz, A.; Oropeza, F. E.; Poll, C. G.; Payne, D. J.; Palgrave, R. G.; Panaccione, G.; Borgatti, F.; Agrestini, S.; Utsumi, Y.; Tsuei, K. D.; Liao, Y. F.; Watson, G. W.; Egdell, R. G.

2016-03-01

The contributions of Sn 5s and Ti 4s states to the valence band electronic structure of Sn-doped anatase have been identified by hard X-ray photoelectron spectroscopy. The metal s state intensity is strongly enhanced relative to that of O 2p states at high photon energies due to matrix element effects when electrons are detected parallel to the direction of the polarisation vector of the synchrotron beam, but becomes negligible in the perpendicular direction. The experimental spectra in both polarisations are in good agreement with cross section and asymmetry parameter weighted partial densities of states derived from density functional theory calculations.

Theory of Tunneling Spectroscopy in a Mn12 Single-Electron Transistor by Density-Functional Theory Methods

NASA Astrophysics Data System (ADS)

Michalak, Ł.; Canali, C. M.; Pederson, M. R.; Paulsson, M.; Benza, V. G.

2010-01-01

We consider tunneling transport through a Mn12 molecular magnet using spin density functional theory. A tractable methodology for constructing many-body wave functions from Kohn-Sham orbitals allows for the determination of spin-dependent matrix elements for use in transport calculations. The tunneling conductance at finite bias is characterized by peaks representing transitions between spin multiplets, separated by an energy on the order of the magnetic anisotropy. The energy splitting of the spin multiplets and the spatial part of their many-body wave functions, describing the orbital degrees of freedom of the excess charge, strongly affect the electronic transport, and can lead to negative differential conductance.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Askari, Nasim; Eslami, Esmaeil, E-mail: eeslami@iust.ac.ir; Mirzaie, Reza

2015-11-15

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.

Theory of tunneling spectroscopy in a Mn12 single-electron transistor by density-functional theory methods.

PubMed

Michalak, Ł; Canali, C M; Pederson, M R; Paulsson, M; Benza, V G

2010-01-08

We consider tunneling transport through a Mn12 molecular magnet using spin density functional theory. A tractable methodology for constructing many-body wave functions from Kohn-Sham orbitals allows for the determination of spin-dependent matrix elements for use in transport calculations. The tunneling conductance at finite bias is characterized by peaks representing transitions between spin multiplets, separated by an energy on the order of the magnetic anisotropy. The energy splitting of the spin multiplets and the spatial part of their many-body wave functions, describing the orbital degrees of freedom of the excess charge, strongly affect the electronic transport, and can lead to negative differential conductance.

Kohn-Sham potentials from electron densities using a matrix representation within finite atomic orbital basis sets

NASA Astrophysics Data System (ADS)

Zhang, Xing; Carter, Emily A.

2018-01-01

We revisit the static response function-based Kohn-Sham (KS) inversion procedure for determining the KS effective potential that corresponds to a given target electron density within finite atomic orbital basis sets. Instead of expanding the potential in an auxiliary basis set, we directly update the potential in its matrix representation. Through numerical examples, we show that the reconstructed density rapidly converges to the target density. Preliminary results are presented to illustrate the possibility of obtaining a local potential in real space from the optimized potential in its matrix representation. We have further applied this matrix-based KS inversion approach to density functional embedding theory. A proof-of-concept study of a solvated proton transfer reaction demonstrates the method's promise.

On Schrödinger's bridge problem

NASA Astrophysics Data System (ADS)

Friedland, S.

2017-11-01

In the first part of this paper we generalize Georgiou-Pavon's result that a positive square matrix can be scaled uniquely to a column stochastic matrix which maps a given positive probability vector to another given positive probability vector. In the second part we prove that a positive quantum channel can be scaled to another positive quantum channel which maps a given positive definite density matrix to another given positive definite density matrix using Brouwer's fixed point theorem. This result proves the Georgiou-Pavon conjecture for two positive definite density matrices, made in their recent paper. We show that the fixed points are unique for certain pairs of positive definite density matrices. Bibliography: 15 titles.

Excitation energies from range-separated time-dependent density and density matrix functional theory.

PubMed

Pernal, Katarzyna

2012-05-14

Time-dependent density functional theory (TD-DFT) in the adiabatic formulation exhibits known failures when applied to predicting excitation energies. One of them is the lack of the doubly excited configurations. On the other hand, the time-dependent theory based on a one-electron reduced density matrix functional (time-dependent density matrix functional theory, TD-DMFT) has proven accurate in determining single and double excitations of H(2) molecule if the exact functional is employed in the adiabatic approximation. We propose a new approach for computing excited state energies that relies on functionals of electron density and one-electron reduced density matrix, where the latter is applied in the long-range region of electron-electron interactions. A similar approach has been recently successfully employed in predicting ground state potential energy curves of diatomic molecules even in the dissociation limit, where static correlation effects are dominating. In the paper, a time-dependent functional theory based on the range-separation of electronic interaction operator is rigorously formulated. To turn the approach into a practical scheme the adiabatic approximation is proposed for the short- and long-range components of the coupling matrix present in the linear response equations. In the end, the problem of finding excitation energies is turned into an eigenproblem for a symmetric matrix. Assignment of obtained excitations is discussed and it is shown how to identify double excitations from the analysis of approximate transition density matrix elements. The proposed method used with the short-range local density approximation (srLDA) and the long-range Buijse-Baerends density matrix functional (lrBB) is applied to H(2) molecule (at equilibrium geometry and in the dissociation limit) and to Be atom. The method accounts for double excitations in the investigated systems but, unfortunately, the accuracy of some of them is poor. The quality of the other excitations is in general much better than that offered by TD-DFT-LDA or TD-DMFT-BB approximations if the range-separation parameter is properly chosen. The latter remains an open problem.

Emission and evaporation properties of 75 at.% Re-25 at.% W mixed matrix impregnated cathode

NASA Astrophysics Data System (ADS)

Lai, Chen; Wang, Jinshu; Zhou, Fan; Liu, Wei; den Engelsen, Daniel; Miao, Naihua

2018-01-01

We present a comprehensive study on the phase, emission performance, surface composition, chemical states and evaporation properties of a 75 at.% Re-25 at.% W (75Re) mixed matrix impregnated cathode by several modern analyzers, including XRD, electron emission test device, in situ AES, XPS and Quartz Crystal Oscillation Instrument (QCOI). On the basis of experimental results, the adsorption energy and charge transfer of the Ba-O dipole adsorbed on cathode surface was investigated by the first-principles density functional theory calculations. The in situ AES analyses indicate that the atomic ratio of Ba:O of the active emission layer on the cathode surface converged to 3:2 for a conventional Ba-W cathode and to about 3:1 for the 75Re cathode. Due to the larger adsorption energy of Ba and Ba-O on 75Re cathode surface, the total evaporation rate of Ba and BaO in the 75Re cathode is much lower than that for the Ba-W cathode, which is agreed favorably with the experimental evaporation data. Our characterizations and calculations suggest that rhenium in the matrix of impregnated cathodes improves the stability of Ba-O dipole on the cathode surface and enhances the emission capability substantially.

Monte Carlo Calculation of Thermal Neutron Inelastic Scattering Cross Section Uncertainties by Sampling Perturbed Phonon Spectra

NASA Astrophysics Data System (ADS)

Holmes, Jesse Curtis

Nuclear data libraries provide fundamental reaction information required by nuclear system simulation codes. The inclusion of data covariances in these libraries allows the user to assess uncertainties in system response parameters as a function of uncertainties in the nuclear data. Formats and procedures are currently established for representing covariances for various types of reaction data in ENDF libraries. This covariance data is typically generated utilizing experimental measurements and empirical models, consistent with the method of parent data production. However, ENDF File 7 thermal neutron scattering library data is, by convention, produced theoretically through fundamental scattering physics model calculations. Currently, there is no published covariance data for ENDF File 7 thermal libraries. Furthermore, no accepted methodology exists for quantifying or representing uncertainty information associated with this thermal library data. The quality of thermal neutron inelastic scattering cross section data can be of high importance in reactor analysis and criticality safety applications. These cross sections depend on the material's structure and dynamics. The double-differential scattering law, S(alpha, beta), tabulated in ENDF File 7 libraries contains this information. For crystalline solids, S(alpha, beta) is primarily a function of the material's phonon density of states (DOS). Published ENDF File 7 libraries are commonly produced by calculation and processing codes, such as the LEAPR module of NJOY, which utilize the phonon DOS as the fundamental input for inelastic scattering calculations to directly output an S(alpha, beta) matrix. To determine covariances for the S(alpha, beta) data generated by this process, information about uncertainties in the DOS is required. The phonon DOS may be viewed as a probability density function of atomic vibrational energy states that exist in a material. Probable variation in the shape of this spectrum may be established that depends on uncertainties in the physics models and methodology employed to produce the DOS. Through Monte Carlo sampling of perturbations from the reference phonon spectrum, an S(alpha, beta) covariance matrix may be generated. In this work, density functional theory and lattice dynamics in the harmonic approximation are used to calculate the phonon DOS for hexagonal crystalline graphite. This form of graphite is used as an example material for the purpose of demonstrating procedures for analyzing, calculating and processing thermal neutron inelastic scattering uncertainty information. Several sources of uncertainty in thermal neutron inelastic scattering calculations are examined, including sources which cannot be directly characterized through a description of the phonon DOS uncertainty, and their impacts are evaluated. Covariances for hexagonal crystalline graphite S(alpha, beta) data are quantified by coupling the standard methodology of LEAPR with a Monte Carlo sampling process. The mechanics of efficiently representing and processing this covariance information is also examined. Finally, with appropriate sensitivity information, it is shown that an S(alpha, beta) covariance matrix can be propagated to generate covariance data for integrated cross sections, secondary energy distributions, and coupled energy-angle distributions. This approach enables a complete description of thermal neutron inelastic scattering cross section uncertainties which may be employed to improve the simulation of nuclear systems.

Efficient evaluation of Coulomb integrals in a mixed Gaussian and plane-wave basis using the density fitting and Cholesky decomposition.

PubMed

Čársky, Petr; Čurík, Roman; Varga, Štefan

2012-03-21

The objective of this paper is to show that the density fitting (resolution of the identity approximation) can also be applied to Coulomb integrals of the type (k(1)(1)k(2)(1)|g(1)(2)g(2)(2)), where k and g symbols refer to plane-wave functions and gaussians, respectively. We have shown how to achieve the accuracy of these integrals that is needed in wave-function MO and density functional theory-type calculations using mixed Gaussian and plane-wave basis sets. The crucial issues for achieving such a high accuracy are application of constraints for conservation of the number electrons and components of the dipole moment, optimization of the auxiliary basis set, and elimination of round-off errors in the matrix inversion. © 2012 American Institute of Physics

Information loss in effective field theory: Entanglement and thermal entropies

NASA Astrophysics Data System (ADS)

Boyanovsky, Daniel

2018-03-01

Integrating out high energy degrees of freedom to yield a low energy effective field theory leads to a loss of information with a concomitant increase in entropy. We obtain the effective field theory of a light scalar field interacting with heavy fields after tracing out the heavy degrees of freedom from the time evolved density matrix. The initial density matrix describes the light field in its ground state and the heavy fields in equilibrium at a common temperature T . For T =0 , we obtain the reduced density matrix in a perturbative expansion; it reveals an emergent mixed state as a consequence of the entanglement between light and heavy fields. We obtain the effective action that determines the time evolution of the reduced density matrix for the light field in a nonperturbative Dyson resummation of one-loop correlations of the heavy fields. The Von-Neumann entanglement entropy associated with the reduced density matrix is obtained for the nonresonant and resonant cases in the asymptotic long time limit. In the nonresonant case the reduced density matrix displays an incipient thermalization albeit with a wave-vector, time and coupling dependent effective temperature as a consequence of memory of initial conditions. The entanglement entropy is time independent and is the thermal entropy for this effective, nonequilibrium temperature. In the resonant case the light field fully thermalizes with the heavy fields, the reduced density matrix loses memory of the initial conditions and the entanglement entropy becomes the thermal entropy of the light field. We discuss the relation between the entanglement entropy ultraviolet divergences and renormalization.

The influence of hyaluronic acid hydrogel crosslinking density and macromolecular diffusivity on human MSC chondrogenesis and hypertrophy.

PubMed

Bian, Liming; Hou, Chieh; Tous, Elena; Rai, Reena; Mauck, Robert L; Burdick, Jason A

2013-01-01

Hyaluronic acid (HA) hydrogels formed via photocrosslinking provide stable 3D hydrogel environments that support the chondrogenesis of mesenchymal stem cells (MSCs). Crosslinking density has a significant impact on the physical properties of hydrogels, including their mechanical stiffness and macromolecular diffusivity. Variations in the HA hydrogel crosslinking density can be obtained by either changes in the HA macromer concentration (1, 3, or 5% w/v at 15 min exposure) or the extent of reaction through light exposure time (5% w/v at 5, 10, or 15 min). In this work, increased crosslinking by either method resulted in an overall decrease in cartilage matrix content and more restricted matrix distribution. Increased crosslinking also promoted hypertrophic differentiation of the chondrogenically induced MSCs, resulting in more matrix calcification in vitro. For example, type X collagen expression in the high crosslinking density 5% 15 min group was ~156 and 285% higher when compared to the low crosslinking density 1% 15 min and 5% 5 min groups on day 42, respectively. Supplementation with inhibitors of the small GTPase pathway involved in cytoskeletal tension or myosin II had no effect on hypertrophic differentiation and matrix calcification, indicating that the differential response is unlikely to be related to force-sensing mechanotransduction mechanisms. When implanted subcutaneously in nude mice, higher crosslinking density again resulted in reduced cartilage matrix content, restricted matrix distribution, and increased matrix calcification. This study demonstrates that hydrogel properties mediated through alterations in crosslinking density must be considered in the context of the hypertrophic differentiation of chondrogenically induced MSCs. Copyright © 2012 Elsevier Ltd. All rights reserved.

Variational Two-Particle Density Matrix Calculation for the Hubbard Model Below Half Filling Using Spin-Adapted Lifting Conditions

NASA Astrophysics Data System (ADS)

Verstichel, Brecht; van Aggelen, Helen; Poelmans, Ward; Van Neck, Dimitri

2012-05-01

The variational determination of the two-particle density matrix is an interesting, but not yet fully explored technique that allows us to obtain ground-state properties of a quantum many-body system without reference to an N-particle wave function. The one-dimensional fermionic Hubbard model has been studied before with this method, using standard two- and three-index conditions on the density matrix [J. R. Hammond , Phys. Rev. A 73, 062505 (2006)PLRAAN1050-294710.1103/PhysRevA.73.062505], while a more recent study explored so-called subsystem constraints [N. Shenvi , Phys. Rev. Lett. 105, 213003 (2010)PRLTAO0031-900710.1103/PhysRevLett.105.213003]. These studies reported good results even with only standard two-index conditions, but have always been limited to the half-filled lattice. In this Letter, we establish the fact that the two-index approach fails for other fillings. In this case, a subset of three-index conditions is absolutely needed to describe the correct physics in the strong-repulsion limit. We show that applying lifting conditions [J. R. Hammond , Phys. Rev. APLRAAN1050-2947 71, 062503 (2005)10.1103/PhysRevA.71.062503] is the most economical way to achieve this, while still avoiding the computationally much heavier three-index conditions. A further extension to spin-adapted lifting conditions leads to increased accuracy in the intermediate repulsion regime. At the same time, we establish the feasibility of such studies to the more complicated phase diagram in two-dimensional Hubbard models.

Five- and six-electron harmonium atoms: Highly accurate electronic properties and their application to benchmarking of approximate 1-matrix functionals

NASA Astrophysics Data System (ADS)

Cioslowski, Jerzy; Strasburger, Krzysztof

2018-04-01

Electronic properties of several states of the five- and six-electron harmonium atoms are obtained from large-scale calculations employing explicitly correlated basis functions. The high accuracy of the computed energies (including their components), natural spinorbitals, and their occupation numbers makes them suitable for testing, calibration, and benchmarking of approximate formalisms of quantum chemistry and solid state physics. In the case of the five-electron species, the availability of the new data for a wide range of the confinement strengths ω allows for confirmation and generalization of the previously reached conclusions concerning the performance of the presently known approximations for the electron-electron repulsion energy in terms of the 1-matrix that are at heart of the density matrix functional theory (DMFT). On the other hand, the properties of the three low-lying states of the six-electron harmonium atom, computed at ω = 500 and ω = 1000, uncover deficiencies of the 1-matrix functionals not revealed by previous studies. In general, the previously published assessment of the present implementations of DMFT being of poor accuracy is found to hold. Extending the present work to harmonically confined systems with even more electrons is most likely counterproductive as the steep increase in computational cost required to maintain sufficient accuracy of the calculated properties is not expected to be matched by the benefits of additional information gathered from the resulting benchmarks.

Absolute empirical rate coefficient for the excitation of the 117.6 nm line in C III

NASA Astrophysics Data System (ADS)

Gardner, L. D.; Daw, A. N.; Janzen, P. H.; Atkins, N.; Kohl, J. L.

2005-05-01

We have measured the absolute cross sections for electron impact excitation (EIE) of C2+ (2s2p 3P° - 2p2 3P) for energies from below threshold to 17 eV above and derived EIE rate coefficients required for astrophysical applications. The uncertainty in the rate coefficient at a typical solar temperature of formation of C2+ is less than ± 6 %. Ions are produced in a 5 GHz Electron Cyclotron Resonance (ECR) ion source, extracted, formed into a beam, and transported to a collision chamber where they collide with electrons from an electron beam inclined at 45 degrees. The beams are modulated and the radiation from the decay of the excited ions at λ 117.6 nm is detected synchronously using an absolutely calibrated optical system that subtends slightly over π steradians. The fractional population of the C2+ metastable state in the incident ion beam has been determined experimentally to be 0.42 ± 0.03 (1.65 σ). At the reported ± 15 % total experimental uncertainty level (1.65 σ), the measured structure and absolute scale of the cross section are in fairly good agreement with 6-term close-coupling R-matrix calculations and 90-term R-matrix with pseudo-states calculations, although some minor differences are seen just above threshold. As density-sensitive line intensity ratios vary by only about a factor of 5 as the density changes by nearly a factor of 100, even a 30 % uncertainty in the excitation rate can lead to a factor of 3 error in density. This work is supported by NASA Supporting Research and Technology grants NAG5- 9516 and NAG5-12863 in Solar and Heliospheric Physics and by the Smithsonian Astrophysical Observatory.

Accelerating molecular property calculations with nonorthonormal Krylov space methods

DOE Office of Scientific and Technical Information (OSTI.GOV)

Furche, Filipp; Krull, Brandon T.; Nguyen, Brian D.

Here, we formulate Krylov space methods for large eigenvalue problems and linear equation systems that take advantage of decreasing residual norms to reduce the cost of matrix-vector multiplication. The residuals are used as subspace basis without prior orthonormalization, which leads to generalized eigenvalue problems or linear equation systems on the Krylov space. These nonorthonormal Krylov space (nKs) algorithms are favorable for large matrices with irregular sparsity patterns whose elements are computed on the fly, because fewer operations are necessary as the residual norm decreases as compared to the conventional method, while errors in the desired eigenpairs and solution vectors remainmore » small. We consider real symmetric and symplectic eigenvalue problems as well as linear equation systems and Sylvester equations as they appear in configuration interaction and response theory. The nKs method can be implemented in existing electronic structure codes with minor modifications and yields speed-ups of 1.2-1.8 in typical time-dependent Hartree-Fock and density functional applications without accuracy loss. The algorithm can compute entire linear subspaces simultaneously which benefits electronic spectra and force constant calculations requiring many eigenpairs or solution vectors. The nKs approach is related to difference density methods in electronic ground state calculations, and particularly efficient for integral direct computations of exchange-type contractions. By combination with resolution-of-the-identity methods for Coulomb contractions, three- to fivefold speed-ups of hybrid time-dependent density functional excited state and response calculations are achieved.« less

Accelerating molecular property calculations with nonorthonormal Krylov space methods

DOE PAGES

Furche, Filipp; Krull, Brandon T.; Nguyen, Brian D.; ...

2016-05-03

Here, we formulate Krylov space methods for large eigenvalue problems and linear equation systems that take advantage of decreasing residual norms to reduce the cost of matrix-vector multiplication. The residuals are used as subspace basis without prior orthonormalization, which leads to generalized eigenvalue problems or linear equation systems on the Krylov space. These nonorthonormal Krylov space (nKs) algorithms are favorable for large matrices with irregular sparsity patterns whose elements are computed on the fly, because fewer operations are necessary as the residual norm decreases as compared to the conventional method, while errors in the desired eigenpairs and solution vectors remainmore » small. We consider real symmetric and symplectic eigenvalue problems as well as linear equation systems and Sylvester equations as they appear in configuration interaction and response theory. The nKs method can be implemented in existing electronic structure codes with minor modifications and yields speed-ups of 1.2-1.8 in typical time-dependent Hartree-Fock and density functional applications without accuracy loss. The algorithm can compute entire linear subspaces simultaneously which benefits electronic spectra and force constant calculations requiring many eigenpairs or solution vectors. The nKs approach is related to difference density methods in electronic ground state calculations, and particularly efficient for integral direct computations of exchange-type contractions. By combination with resolution-of-the-identity methods for Coulomb contractions, three- to fivefold speed-ups of hybrid time-dependent density functional excited state and response calculations are achieved.« less

A Numerical Model of Laser-Induced Fluorescence in a Hydrogen Plasma

DTIC Science & Technology

1991-03-10

cross-sections. Lee, et al., cited screened Coulomb potential calculations by several groups to place an up- per limit of 30 A on the Debye length...intensity: RL(t)(1/sec) = B,,(cir 2/erg . sec) . (J,)(erg/sec .cm -. liz) (3.5) 35 The Einstein coefficients are related by the statistical weights of the...impact processes.) These rate matrices were then added together to obtain the total rate matrix for both groups of electrons. The total electron density

Disorder effect on the Friedel oscillations in a one-dimensional Mott insulator

NASA Astrophysics Data System (ADS)

Weiss, Y.; Goldstein, M.; Berkovits, R.

2007-07-01

The Friedel oscillations resulting from coupling a quantum dot to one edge of a disordered one-dimensional wire in the Mott insulator regime are calculated numerically using the density matrix renormalization group method. By investigating the influence of a constant weak disorder on the Friedel oscillations decay we find that the effect of disorder is reduced by increasing the interaction strength. This behavior is opposite to the recently reported influence of disorder in the Anderson insulator regime.

Physical and optical properties of lithium borosilicate glasses doped with Dy3+ ions

NASA Astrophysics Data System (ADS)

Ramteke, D. D.; Gedam, R. S.; Swart, H. C.

2018-04-01

The borosilicate glasses with Dy3+ ions were prepared by the melt quench technique with varying concentration of Dy2O3. The glasses were characterized by the density calculation, absorbance and photoluminescence (PL) spectroscopy measurements. Density and molar volume of the glasses increases with increase in Dy3+ ions in the glass matrix. This behavior is correlated with the higher molecular weight and larger ionic radius of Dy3+ ion compared to the other constituents of glass matrix. Emission of Dy3+ doped glasses showed three bands at 482, 573 and at 665 nm which correspond to 6H15/2 (blue), 6H13/2 (yellow) and 6H11/2 (red) transitions. The emission spectra of glasses with different concentration of Dy3+ ions shows that, glasses with 0.5 mol% of Dy2O3 shows highest emission and decreases with further doping. CIE 1931 chromaticity diagram showed that the emission of these glasses was in the white region. Photographs of these glasses under 349 nm Light emitting diode excitation also confirmed the white light emission from these glasses.

Ground-state properties of anyons in a one-dimensional lattice

NASA Astrophysics Data System (ADS)

Tang, Guixin; Eggert, Sebastian; Pelster, Axel

2015-12-01

Using the Anyon-Hubbard Hamiltonian, we analyze the ground-state properties of anyons in a one-dimensional lattice. To this end we map the hopping dynamics of correlated anyons to an occupation-dependent hopping Bose-Hubbard model using the fractional Jordan-Wigner transformation. In particular, we calculate the quasi-momentum distribution of anyons, which interpolates between Bose-Einstein and Fermi-Dirac statistics. Analytically, we apply a modified Gutzwiller mean-field approach, which goes beyond a classical one by including the influence of the fractional phase of anyons within the many-body wavefunction. Numerically, we use the density-matrix renormalization group by relying on the ansatz of matrix product states. As a result it turns out that the anyonic quasi-momentum distribution reveals both a peak-shift and an asymmetry which mainly originates from the nonlocal string property. In addition, we determine the corresponding quasi-momentum distribution of the Jordan-Wigner transformed bosons, where, in contrast to the hard-core case, we also observe an asymmetry for the soft-core case, which strongly depends on the particle number density.

A comparison of the C III, O V, F VI, and Ne VII Delta n = 0 (2-2) line emissions from a laboratory plasma with theoretical predictions and astrophysical observations

NASA Technical Reports Server (NTRS)

Finkenthal, M.; Yu, . L.; Lippmann, S.; Huang, L. K.; Moos, H. W.; Stratton, B. C.; Bhatia, A. K.

1987-01-01

Spectra of the Delta n = 0 (2-2) transitions of Be I-like ions, C III, O V, F VI, and Ne VII emitted from the TEXT tokamak, were measured with photometrically calibrated instrumentation and compared to the predictions of several models which differ in their treatment of electron impact excitation, using either the distorted wave or R-matrix approach. It was found that the ions from C III to Ne VII were located near the edge of the plasma, at densities between 10 to the 12th and 13th/cu cm. The experimental line ratios were compared with several sets of computations. Agreement is obtained between the experimental data and computations by using the R-matrix technique. This leads to the conclusion that the effect resonances must be included in collision strength calculations, particularly at low nuclear charge. The results show that the line ratios studied may be used with confidence as electron density diagnostics for laboratory or astrophysical plasmas.

Stage-structured transmission of phocine distemper virus in the Dutch 2002 outbreak

PubMed Central

Klepac, Petra; Pomeroy, Laura W.; Bjørnstad, Ottar N.; Kuiken, Thijs; Osterhaus, Albert D.M.E.; Rijks, Jolianne M.

2009-01-01

Heterogeneities in transmission among hosts can be very important in shaping infectious disease dynamics. In mammals with strong social organization, such heterogeneities are often structured by functional stage: juveniles, subadults and adults. We investigate the importance of such stage-related heterogeneities in shaping the 2002 phocine distemper virus (PDV) outbreak in the Dutch Wadden Sea, when more than 40 per cent of the harbour seals were killed. We do this by comparing the statistical fit of a hierarchy of models with varying transmission complexity: homogeneous versus heterogeneous mixing and density- versus frequency-dependent transmission. We use the stranding data as a proxy for incidence and use Poisson likelihoods to estimate the ‘who acquires infection from whom’ (WAIFW) matrix. Statistically, the model with strong heterogeneous mixing and density-dependent transmission was found to best describe the transmission dynamics. However, patterns of incidence support a model of frequency-dependent transmission among adults and juveniles. Based on the maximum-likelihood WAIFW matrix estimates, we use the next-generation formalism to calculate an R0 between 2 and 2.5 for the Dutch 2002 PDV epidemic. PMID:19364743

Electron-impact excitation of diatomic hydride cations - I. HeH+, CH+, ArH+

NASA Astrophysics Data System (ADS)

Hamilton, James R.; Faure, Alexandre; Tennyson, Jonathan

2016-01-01

R-matrix calculations combined with the adiabatic nuclei approximation are used to compute electron-impact rotational excitation rates for three closed-shell diatomic cations, HeH+, CH+, ArH+. Comparisons with previous studies show that an improved treatment of threshold effects leads to significant changes in the low temperature rates; furthermore the new calculations suggest that excitation of CH+ is dominated by ΔJ = 1 transitions as is expected for cations with a large dipole moment. A model for ArH+ excitation in the Crab nebula is presented which gives results consistent with the observations for electron densities in the range 2-3 × 103 cm-3.

Dangling bond defects in SiC: An ab initio study

NASA Astrophysics Data System (ADS)

Tuttle, Blair R.

2018-01-01

We report first-principles microscopic calculations of the properties of defects with dangling bonds in crystalline 3 C -SiC. Specifically, we focus on hydrogenated Si and C vacancies, divacancies, and multivacancies. The latter is a generic model for an isolated dangling bond within a bulk SiC matrix. Hydrogen serves to passivate electrically active defects to allow the isolation of a single dangling-bond defect. We used hybrid density-functional methods to determine energetics and electrical activity. The present results are compared to previous 3 C -SiC calculations and experiments. Finally, we identify homopolar carbon dangling-bond defects as the leakage causing defects in nanoporous SiC alloys.

Matrix Methods for Estimating the Coherence Functions from Estimates of the Cross-Spectral Density Matrix

DOE PAGES

Smallwood, D. O.

1996-01-01

It is shown that the usual method for estimating the coherence functions (ordinary, partial, and multiple) for a general multiple-input! multiple-output problem can be expressed as a modified form of Cholesky decomposition of the cross-spectral density matrix of the input and output records. The results can be equivalently obtained using singular value decomposition (SVD) of the cross-spectral density matrix. Using SVD suggests a new form of fractional coherence. The formulation as a SVD problem also suggests a way to order the inputs when a natural physical order of the inputs is absent.

Squared eigenvalue condition numbers and eigenvector correlations from the single ring theorem

NASA Astrophysics Data System (ADS)

Belinschi, Serban; Nowak, Maciej A.; Speicher, Roland; Tarnowski, Wojciech

2017-03-01

We extend the so-called ‘single ring theorem’ (Feinberg and Zee 1997 Nucl. Phys. B 504 579), also known as the Haagerup-Larsen theorem (Haagerup and Larsen 2000 J. Funct. Anal. 176 331). We do this by showing that in the limit when the size of the matrix goes to infinity a particular correlator between left and right eigenvectors of the relevant non-hermitian matrix X, being the spectral density weighted by the squared eigenvalue condition number, is given by a simple formula involving only the radial spectral cumulative distribution function of X. We show that this object allows the calculation of the conditional expectation of the squared eigenvalue condition number. We give examples and provide a cross-check of the analytic prediction by the large scale numerics.

The rate constant of a quantum-diffusion-controlled bimolecular reaction

NASA Astrophysics Data System (ADS)

Bondarev, B. V.

1986-04-01

A quantum-mechanical equation is derived in the tight-bond approximation which describes the motion and chemical interaction of a pair of species A and B when their displacement in the matrix is caused by tunnelling. Within the framework of the discrete model of random walks, definitions are given of the probability and rate constant of a reaction A + B → P (products) proceeding in a condensed medium. A method is suggested for calculating the rate constant of a quantum-diffusion-controlled bimolecular reaction. By this method, an expression is obtained for the rate constant in the stationary spherically symmetrical case. An equation for the density matrix is also proposed which describes the motion and chemical interaction of a pair of species when the quantum and classical diffusion are competitive.

Photoionization of Benzene and Small Polycyclic Aromatic Hydrocarbons in Ultraviolet-Processed Astrophysical Ices: A Computational Study

NASA Technical Reports Server (NTRS)

Woon, D. E.; Park, J.-Y.

2004-01-01

We employed density functional theory (DFT) calculations to model the photoionization behavior of benzene and small polycyclic aromatic hydrocarbons when they are embedded in a matrix of water ice in order to investigate issues raised by recent experimental work by Gudipati and Allamandola. The ionization energies of benzene, naphthalene, anthracene, and pyrene were found to be lowered by 1.5-2.1 eV in water ice. Low-lying vertical electronic excitation energies were computed with time-dependent DFT for both neutral and ionized species and are found in both cases to be remarkably unaffected by the ice matrix. Chemical behavior in ultraviolet-photoprocessed ices is also discussed, with a focus on electron recombination and pathways leading to phenol and analogous products.

Origin of the quasiparticle peak in the spectral density of Cr(001) surfaces

NASA Astrophysics Data System (ADS)

Peters, L.; Jacob, D.; Karolak, M.; Lichtenstein, A. I.; Katsnelson, M. I.

2017-12-01

In the spectral density of Cr(001) surfaces, a sharp resonance close to the Fermi level is observed in both experiment and theory. For the physical origin of this peak, two mechanisms were proposed: a single-particle dz2 surface state renormalized by electron-phonon coupling and an orbital Kondo effect due to the degenerate dx z/dy z states. Despite several experimental and theoretical investigations, the origin is still under debate. In this work, we address this problem by two different approaches of the dynamical mean-field theory: first, by the spin-polarized T -matrix fluctuation exchange approximation suitable for weakly and moderately correlated systems; second, by the noncrossing approximation derived in the limit of weak hybridization (i.e., for strongly correlated systems) capturing Kondo-type processes. By using recent continuous-time quantum Monte Carlo calculations as a benchmark, we find that the high-energy features, everything except the resonance, of the spectrum are captured within the spin-polarized T -matrix fluctuation exchange approximation. More precisely, the particle-particle processes provide the main contribution. For the noncrossing approximation, it appears that spin-polarized calculations suffer from spurious behavior at the Fermi level. Then, we turned to non-spin-polarized calculations to avoid this unphysical behavior. By employing two plausible starting hybridization functions, it is observed that the characteristics of the resonance are crucially dependent on the starting point. It appears that only one of these starting hybridizations could result in an orbital Kondo resonance in the presence of a strong magnetic field like in the Cr(001) surface. It is for a future investigation to first resolve the unphysical behavior within the spin-polarized noncrossing approximation and then check for an orbital Kondo resonance.

SEDIDAT: A BASIC program for the collection and statistical analysis of particle settling velocity data

NASA Astrophysics Data System (ADS)

Wright, Robyn; Thornberg, Steven M.

SEDIDAT is a series of compiled IBM-BASIC (version 2.0) programs that direct the collection, statistical calculation, and graphic presentation of particle settling velocity and equivalent spherical diameter for samples analyzed using the settling tube technique. The programs follow a menu-driven format that is understood easily by students and scientists with little previous computer experience. Settling velocity is measured directly (cm,sec) and also converted into Chi units. Equivalent spherical diameter (reported in Phi units) is calculated using a modified Gibbs equation for different particle densities. Input parameters, such as water temperature, settling distance, particle density, run time, and Phi;Chi interval are changed easily at operator discretion. Optional output to a dot-matrix printer includes a summary of moment and graphic statistical parameters, a tabulation of individual and cumulative weight percents, a listing of major distribution modes, and cumulative and histogram plots of a raw time, settling velocity. Chi and Phi data.

Stress fluctuations in fracture networks from theoretical and numerical models

NASA Astrophysics Data System (ADS)

Davy, P.; Darcel, C.; Mas Ivars, D.; Le Goc, R.

2017-12-01

We analyze the spatial fluctuations of stress in a simple tridimensional model constituted by a population of disc-shaped fractures embedded in an elastic matrix with uniform and isotropic properties. The fluctuations arise from the classical stress enhancement at fracture tips and stress shadowing around fracture centers that are amplified or decreased by the interactions between close-by fractures. The distribution of local stresses is calculated at the elementary mesh scale with the 3DEC numerical program based on the distinct element method. As expected, the stress distributions vary with fracture density, the larger is the density, the wider is the distribution. For freely slipping fractures, it is mainly controlled by the percolation parameter p (i.e., the total volume of spheres surrounding fractures). For stresses smaller than the remote deviatoric stress, the distribution depends only on for the range of density that has been studied. For large stresses, the distribution decreases exponentially when increasing stress, with a characteristic stress that increases with entailing a widening of the stress distribution. We extend the analysis to fractures with plane resistance defined by an elastic shear stiffness ks and a slip Coulomb threshold. A consequence of the fracture plane resistance is to lower the stress perturbation in the surrounding matrix by a factor that depends on the ratio between ks and a fracture-matrix stiffness km mainly dependent on the ratio between Young modulus and fracture size. km is also the ratio between the remote shear stress and the displacement across the fracture plane in the case of freely slipping fractures. A complete analytical derivation of the expressions of the stress perturbations and of the fracture displacements is obtained and checked with numerical simulations. In the limit ks >> km, the stress perturbation tends to 0 and the stress state is spatially uniform. The analysis allows us to quantify the intensity of the stress fluctuations in fractured rocks as a function of both the fracture network characteristics (density and size distribution), and the mechanical properties (fracture shear stiffness vs matrix elastic properties).

Synthesis and Characterisation of ETS-10/Acetate-based Ionic Liquid/Chitosan Mixed Matrix Membranes for CO2/N2 Permeation.

PubMed

Casado-Coterillo, Clara; Del Mar López-Guerrero, María; Irabien, Angel

2014-06-19

Mixed matrix membranes (MMMs) were prepared by incorporating organic surfactant-free hydrothermally synthesised ETS-10 and 1-ethyl-3-methylimidazolium acetate ionic liquid (IL) to chitosan (CS) polymer matrix. The membrane material characteristics and permselectivity performance of the two-component membranes were compared with the three-component membrane and the pure CS membrane. The addition of IL increased CO2 solubility of the polymer, and, thus, the CO2 affinity was maintained for the MMMs, which can be correlated with the crystallinity, measured by FT-IR, and void fraction calculations from differences between theoretical and experimental densities. The mechanical resistance was enhanced by the ETS-10 nanoparticles, and flexibility decreased in the two-component ETS-10/CS MMMs, but the flexibility imparted by the IL remained in three-component ETS-10/IL/CS MMMs. The results of this work provide insight into another way of facing the adhesion challenge in MMMs and obtain CO2 selective MMMs from renewable or green chemistry materials.

Superfluidity, Bose-Einstein condensation, and structure in one-dimensional Luttinger liquids

NASA Astrophysics Data System (ADS)

Vranješ Markić, L.; Vrcan, H.; Zuhrianda, Z.; Glyde, H. R.

2018-01-01

We report diffusion Monte Carlo (DMC) and path integral Monte Carlo (PIMC) calculations of the properties of a one-dimensional (1D) Bose quantum fluid. The equation of state, the superfluid fraction ρS/ρ0 , the one-body density matrix n (x ) , the pair distribution function g (x ) , and the static structure factor S (q ) are evaluated. The aim is to test Luttinger liquid (LL) predictions for 1D fluids over a wide range of fluid density and LL parameter K . The 1D Bose fluid examined is a single chain of 4He atoms confined to a line in the center of a narrow nanopore. The atoms cannot exchange positions in the nanopore, the criterion for 1D. The fluid density is varied from the spinodal density where the 1D liquid is unstable to droplet formation to the density of bulk liquid 4He. In this range, K varies from K >2 at low density, where a robust superfluid is predicted, to K <0.5 , where fragile 1D superflow and solidlike peaks in S (q ) are predicted. For uniform pore walls, the ρS/ρ0 scales as predicted by LL theory. The n (x ) and g (x ) show long range oscillations and decay with x as predicted by LL theory. The amplitude of the oscillations is large at high density (small K ) and small at low density (large K ). The K values obtained from different properties agree well verifying the internal structure of LL theory. In the presence of disorder, the ρS/ρ0 does not scale as predicted by LL theory. A single vJ parameter in the LL theory that recovers LL scaling was not found. The one body density matrix (OBDM) in disorder is well predicted by LL theory. The "dynamical" superfluid fraction, ρSD/ρ0 , is determined. The physics of the deviation from LL theory in disorder and the "dynamical" ρSD/ρ0 are discussed.

Symbolic computation of the Hartree-Fock energy from a chiral EFT three-nucleon interaction at N 2LO

NASA Astrophysics Data System (ADS)

Gebremariam, B.; Bogner, S. K.; Duguet, T.

2010-06-01

We present the first of a two-part Mathematica notebook collection that implements a symbolic approach for the application of the density matrix expansion (DME) to the Hartree-Fock (HF) energy from a chiral effective field theory (EFT) three-nucleon interaction at N 2LO. The final output from the notebooks is a Skyrme-like energy density functional that provides a quasi-local approximation to the non-local HF energy. In this paper, we discuss the derivation of the HF energy and its simplification in terms of the scalar/vector-isoscalar/isovector parts of the one-body density matrix. Furthermore, a set of steps is described and illustrated on how to extend the approach to other three-nucleon interactions. Program summaryProgram title: SymbHFNNN Catalogue identifier: AEGC_v1_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEGC_v1_0.html Program obtainable from: CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions: Standard CPC licence, http://cpc.cs.qub.ac.uk/licence/licence.html No. of lines in distributed program, including test data, etc.: 96 666 No. of bytes in distributed program, including test data, etc.: 378 083 Distribution format: tar.gz Programming language: Mathematica 7.1 Computer: Any computer running Mathematica 6.0 and later versions Operating system: Windows Xp, Linux/Unix RAM: 256 Mb Classification: 5, 17.16, 17.22 Nature of problem: The calculation of the HF energy from the chiral EFT three-nucleon interaction at N 2LO involves tremendous spin-isospin algebra. The problem is compounded by the need to eventually obtain a quasi-local approximation to the HF energy, which requires the HF energy to be expressed in terms of scalar/vector-isoscalar/isovector parts of the one-body density matrix. The Mathematica notebooks discussed in this paper solve the latter issue. Solution method: The HF energy from the chiral EFT three-nucleon interaction at N 2LO is cast into a form suitable for an automatic simplification of the spin-isospin traces. Several Mathematica functions and symbolic manipulation techniques are used to obtain the result in terms of the scalar/vector-isoscalar/isovector parts of the one-body density matrix. Running time: Several hours

Partially coherent electron transport in terahertz quantum cascade lasers based on a Markovian master equation for the density matrix

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jonasson, O.; Karimi, F.; Knezevic, I.

2016-08-01

We derive a Markovian master equation for the single-electron density matrix, applicable to quantum cascade lasers (QCLs). The equation conserves the positivity of the density matrix, includes off-diagonal elements (coherences) as well as in-plane dynamics, and accounts for electron scattering with phonons and impurities. We use the model to simulate a terahertz-frequency QCL, and compare the results with both experiment and simulation via nonequilibrium Green's functions (NEGF). We obtain very good agreement with both experiment and NEGF when the QCL is biased for optimal lasing. For the considered device, we show that the magnitude of coherences can be a significantmore » fraction of the diagonal matrix elements, which demonstrates their importance when describing THz QCLs. We show that the in-plane energy distribution can deviate far from a heated Maxwellian distribution, which suggests that the assumption of thermalized subbands in simplified density-matrix models is inadequate. As a result, we also show that the current density and subband occupations relax towards their steady-state values on very different time scales.« less

Effect of competing amines on the removal of tetramethylammonium hydroxide from solution using ion exchange.

PubMed

Citraningrum, H M; Liu, Jhy-Chern

Tetramethylammonium hydroxide (TMAH, TMA(+)) has been widely used as the photoresist developer in semiconductor and thin film transistor liquid crystal display manufacturing. In this study, TMAH-containing wastewater was treated by ion exchange method. Strong acid cation exchange resin was used. A kinetics study revealed that the ion exchange reaction reached equilibrium within 20 min and it could be described by a pseudo-second-order model. To assess the effects of competing ions, wastewater was spiked with three different amines, namely ethylamine (EA(+)), diethylamine (DEA(+)), and triethylamine (TEA(+)). TMAH uptake decreased when in the presence of amines, and it decreased in the order EA(+) < DEA(+) < TEA(+). It could be attributed to different proton affinity (PA) and the strength of affinity between amine molecules and resin matrix, as found from the ab initio calculation values and Langmuir isotherm parameters. However, the interaction energy between sulphonic acid groups and interfering amines in solution using density functional theory (DFT) calculation resulted in a different trend compared with that of PA. The difference might be caused by stabilization of amines by resin matrix and different molecular structures.

Towards a multiconfigurational method of increments

NASA Astrophysics Data System (ADS)

Fertitta, E.; Koch, D.; Paulus, B.; Barcza, G.; Legeza, Ö.

2018-06-01

The method of increments (MoI) allows one to successfully calculate cohesive energies of bulk materials with high accuracy, but it encounters difficulties when calculating dissociation curves. The reason is that its standard formalism is based on a single Hartree-Fock (HF) configuration whose orbitals are localised and used for the many-body expansion. In situations where HF does not allow a size-consistent description of the dissociation, the MoI cannot be guaranteed to yield proper results either. Herein, we address the problem by employing a size-consistent multiconfigurational reference for the MoI formalism. This leads to a matrix equation where a coupling derived by the reference itself is employed. In principle, such an approach allows one to evaluate approximate values for the ground as well as excited states energies. While the latter are accurate close to the avoided crossing only, the ground state results are very promising for the whole dissociation curve, as shown by the comparison with density matrix renormalisation group benchmarks. We tested this two-state constant-coupling MoI on beryllium rings of different sizes and studied the error introduced by the constant coupling.

On the formation of the ·CH 2CH 2CH=NH 2+ distonic radical cation upon ionization of cyclopropylamine and allylamine

NASA Astrophysics Data System (ADS)

Nguyen, Minh Tho; Creve, Steven; Ha, Tae-Kyu

1998-08-01

Ab initio molecular orbital and density functional theory calculations have been applied to determine the relative stability of the cyclopropylamine 1 and allylamine (CH 2=CHCH 2NH 2+·2) radical cations and their isomers. It is confirmed that, upon ionization, 1 undergoes barrier-free ring-opening giving the distonic species ·CH 2CH 2CH=NH 2+3. 2 also rearranges by a 1,2-H-shift to the more stable 3 (by 70 kJ/mol) which is, however, less stable than the 1-aminopropene ion (CH 3-CH=CH-NH 2+·4) by 60 kJ/mol. The transition structure TS 2/3 lies 40 kJ/mol higher in energy than TS 3/4. Although QCISD and B3LYP calculations of isotropic hyperfine coupling constants agree reasonably with observed values, supporting the presence of the distonic 3 in ESR matrix experiments, the exclusive observation of 3, but not 4, is intriguing. This emphasizes the role of the matrix in stabilizing 3.

Optimization of ISOCS Parameters for Quantitative Non-Destructive Analysis of Uranium in Bulk Form

NASA Astrophysics Data System (ADS)

Kutniy, D.; Vanzha, S.; Mikhaylov, V.; Belkin, F.

2011-12-01

Quantitative calculation of the isotopic masses of fissionable U and Pu is important for forensic analysis of nuclear materials. γ-spectrometry is the most commonly applied tool for qualitative detection and analysis of key radionuclides in nuclear materials. Relative isotopic measurement of U and Pu may be obtained from γ-spectra through application of special software such as MGAU (Multi-Group Analysis for Uranium, LLNL) or FRAM (Fixed-Energy Response Function Analysis with Multiple Efficiency, LANL). If the concentration of U/Pu in the matrix is unknown, however, isotopic masses cannot be calculated. At present, active neutron interrogation is the only practical alternative for non-destructive quantification of fissionable isotopes of U and Pu. An active well coincidence counter (AWCC), an alternative for analyses of uranium materials, has the following disadvantages: 1) The detection of small quantities (≤100 g) of 235U is not possible in many models; 2) Representative standards that capture the geometry, density and chemical composition of the analyzed unknown are required for precise analysis; and 3) Specimen size is severely restricted by the size of the measuring chamber. These problems may be addressed using modified γ-spectrometry techniques based on a coaxial HPGe-detector and ISOCS software (In Situ Object Counting System software, Canberra). We present data testing a new gamma-spectrometry method uniting actinide detection with commonly utilized software, modified for application in determining the masses of the fissionable isotopes in unknown samples of nuclear materials. The ISOCS software, widely used in radiation monitoring, calculates the detector efficiency curve in a specified geometry and range of photon energies. In describing the geometry of the source-detector, it is necessary to clearly describe the distance between the source and the detector, the material and the thickness of the walls of the container, as well as material, density and chemical composition of the matrix of the specimen. Obviously, not all parameters can be characterized when measuring samples of unknown composition or uranium in bulk form. Because of this, and especially for uranium materials, the IAEA developed an ISOCS optimization procedure. The target values for the optimization are Μmatrixfixed, the matrix mass determined by weighing with a known mass container, and Εfixed, the 235U enrichment, determined by MGAU. Target values are fitted by varying the matrix density (ρ), and the concentration of uranium in the matrix of the unknown (w). For each (ρi, wi), an efficiency curve is generated, and the masses of uranium isotopes, Μ235Ui and Μ238Ui, determined using spectral activity data and known specific activities for U. Finally, fitted parameters are obtained for Μmatrixi = Μmatrixfixed ± 1σ, Εi = Εfixed ± 1σ, as well as important parameters (ρi, wi, Μ235Ui, Μ238Ui, ΜUi). We examined multiple forms of uranium (powdered, pressed, and scrap UO2 and U3O8) to test this method for its utility in accurately identifying the mass and enrichment of uranium materials, and will present the results of this research.

Compressed Sensing for Chemistry

NASA Astrophysics Data System (ADS)

Sanders, Jacob Nathan

Many chemical applications, from spectroscopy to quantum chemistry, involve measuring or computing a large amount of data, and then compressing this data to retain the most chemically-relevant information. In contrast, compressed sensing is an emergent technique that makes it possible to measure or compute an amount of data that is roughly proportional to its information content. In particular, compressed sensing enables the recovery of a sparse quantity of information from significantly undersampled data by solving an ℓ 1-optimization problem. This thesis represents the application of compressed sensing to problems in chemistry. The first half of this thesis is about spectroscopy. Compressed sensing is used to accelerate the computation of vibrational and electronic spectra from real-time time-dependent density functional theory simulations. Using compressed sensing as a drop-in replacement for the discrete Fourier transform, well-resolved frequency spectra are obtained at one-fifth the typical simulation time and computational cost. The technique is generalized to multiple dimensions and applied to two-dimensional absorption spectroscopy using experimental data collected on atomic rubidium vapor. Finally, a related technique known as super-resolution is applied to open quantum systems to obtain realistic models of a protein environment, in the form of atomistic spectral densities, at lower computational cost. The second half of this thesis deals with matrices in quantum chemistry. It presents a new use of compressed sensing for more efficient matrix recovery whenever the calculation of individual matrix elements is the computational bottleneck. The technique is applied to the computation of the second-derivative Hessian matrices in electronic structure calculations to obtain the vibrational modes and frequencies of molecules. When applied to anthracene, this technique results in a threefold speed-up, with greater speed-ups possible for larger molecules. The implementation of the method in the Q-Chem commercial software package is described. Moreover, the method provides a general framework for bootstrapping cheap low-accuracy calculations in order to reduce the required number of expensive high-accuracy calculations.

Band gap engineering in finite elongated graphene nanoribbon heterojunctions: Tight-binding model

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tayo, Benjamin O.

2015-08-15

A simple model based on the divide and conquer rule and tight-binding (TB) approximation is employed for studying the role of finite size effect on the electronic properties of elongated graphene nanoribbon (GNR) heterojunctions. In our model, the GNR heterojunction is divided into three parts: a left (L) part, middle (M) part, and right (R) part. The left part is a GNR of width W{sub L}, the middle part is a GNR of width W{sub M}, and the right part is a GNR of width W{sub R}. We assume that the left and right parts of the GNR heterojunction interactmore » with the middle part only. Under this approximation, the Hamiltonian of the system can be expressed as a block tridiagonal matrix. The matrix elements of the tridiagonal matrix are computed using real space nearest neighbor orthogonal TB approximation. The electronic structure of the GNR heterojunction is analyzed by computing the density of states. We demonstrate that for heterojunctions for which W{sub L} = W{sub R}, the band gap of the system can be tuned continuously by varying the length of the middle part, thus providing a new approach to band gap engineering in GNRs. Our TB results were compared with calculations employing divide and conquer rule in combination with density functional theory (DFT) and were found to agree nicely.« less

Symmetrized density matrix renormalization group algorithm for low-lying excited states of conjugated carbon systems: Application to 1,12-benzoperylene and polychrysene

NASA Astrophysics Data System (ADS)

Prodhan, Suryoday; Ramasesha, S.

2018-05-01

The symmetry adapted density matrix renormalization group (SDMRG) technique has been an efficient method for studying low-lying eigenstates in one- and quasi-one-dimensional electronic systems. However, the SDMRG method had bottlenecks involving the construction of linearly independent symmetry adapted basis states as the symmetry matrices in the DMRG basis were not sparse. We have developed a modified algorithm to overcome this bottleneck. The new method incorporates end-to-end interchange symmetry (C2) , electron-hole symmetry (J ) , and parity or spin-flip symmetry (P ) in these calculations. The one-to-one correspondence between direct-product basis states in the DMRG Hilbert space for these symmetry operations renders the symmetry matrices in the new basis with maximum sparseness, just one nonzero matrix element per row. Using methods similar to those employed in the exact diagonalization technique for Pariser-Parr-Pople (PPP) models, developed in the 1980s, it is possible to construct orthogonal SDMRG basis states while bypassing the slow step of the Gram-Schmidt orthonormalization procedure. The method together with the PPP model which incorporates long-range electronic correlations is employed to study the correlated excited-state spectra of 1,12-benzoperylene and a narrow mixed graphene nanoribbon with a chrysene molecule as the building unit, comprising both zigzag and cove-edge structures.

Identification of regional activation by factorization of high-density surface EMG signals: A comparison of Principal Component Analysis and Non-negative Matrix factorization.

PubMed

Gallina, Alessio; Garland, S Jayne; Wakeling, James M

2018-05-22

In this study, we investigated whether principal component analysis (PCA) and non-negative matrix factorization (NMF) perform similarly for the identification of regional activation within the human vastus medialis. EMG signals from 64 locations over the VM were collected from twelve participants while performing a low-force isometric knee extension. The envelope of the EMG signal of each channel was calculated by low-pass filtering (8 Hz) the monopolar EMG signal after rectification. The data matrix was factorized using PCA and NMF, and up to 5 factors were considered for each algorithm. Association between explained variance, spatial weights and temporal scores between the two algorithms were compared using Pearson correlation. For both PCA and NMF, a single factor explained approximately 70% of the variance of the signal, while two and three factors explained just over 85% or 90%. The variance explained by PCA and NMF was highly comparable (R > 0.99). Spatial weights and temporal scores extracted with non-negative reconstruction of PCA and NMF were highly associated (all p < 0.001, mean R > 0.97). Regional VM activation can be identified using high-density surface EMG and factorization algorithms. Regional activation explains up to 30% of the variance of the signal, as identified through both PCA and NMF. Copyright © 2018 Elsevier Ltd. All rights reserved.

Communication: Wigner functions in action-angle variables, Bohr-Sommerfeld quantization, the Heisenberg correspondence principle, and a symmetrical quasi-classical approach to the full electronic density matrix

DOE PAGES

Miller, William H.; Cotton, Stephen J.

2016-08-28

It is pointed out that the classical phase space distribution in action-angle (a-a) variables obtained from a Wigner function depends on how the calculation is carried out: if one computes the standard Wigner function in Cartesian variables (p, x), and then replaces p and x by their expressions in terms of a-a variables, one obtains a different result than if the Wigner function is computed directly in terms of the a-a variables. Furthermore, the latter procedure gives a result more consistent with classical and semiclassical theory - e.g., by incorporating the Bohr-Sommerfeld quantization condition (quantum states defined by integer valuesmore » of the action variable) as well as the Heisenberg correspondence principle for matrix elements of an operator between such states - and has also been shown to be more accurate when applied to electronically non-adiabatic applications as implemented within the recently developed symmetrical quasi-classical (SQC) Meyer-Miller (MM) approach. Moreover, use of the Wigner function (obtained directly) in a-a variables shows how our standard SQC/MM approach can be used to obtain off-diagonal elements of the electronic density matrix by processing in a different way the same set of trajectories already used (in the SQC/MM methodology) to obtain the diagonal elements.« less

Communication: Wigner functions in action-angle variables, Bohr-Sommerfeld quantization, the Heisenberg correspondence principle, and a symmetrical quasi-classical approach to the full electronic density matrix.

PubMed

Miller, William H; Cotton, Stephen J

2016-08-28

It is pointed out that the classical phase space distribution in action-angle (a-a) variables obtained from a Wigner function depends on how the calculation is carried out: if one computes the standard Wigner function in Cartesian variables (p, x), and then replaces p and x by their expressions in terms of a-a variables, one obtains a different result than if the Wigner function is computed directly in terms of the a-a variables. Furthermore, the latter procedure gives a result more consistent with classical and semiclassical theory-e.g., by incorporating the Bohr-Sommerfeld quantization condition (quantum states defined by integer values of the action variable) as well as the Heisenberg correspondence principle for matrix elements of an operator between such states-and has also been shown to be more accurate when applied to electronically non-adiabatic applications as implemented within the recently developed symmetrical quasi-classical (SQC) Meyer-Miller (MM) approach. Moreover, use of the Wigner function (obtained directly) in a-a variables shows how our standard SQC/MM approach can be used to obtain off-diagonal elements of the electronic density matrix by processing in a different way the same set of trajectories already used (in the SQC/MM methodology) to obtain the diagonal elements.

Effective-medium theory of elastic waves in random networks of rods.

PubMed

Katz, J I; Hoffman, J J; Conradi, M S; Miller, J G

2012-06-01

We formulate an effective medium (mean field) theory of a material consisting of randomly distributed nodes connected by straight slender rods, hinged at the nodes. Defining wavelength-dependent effective elastic moduli, we calculate both the static moduli and the dispersion relations of ultrasonic longitudinal and transverse elastic waves. At finite wave vector k the waves are dispersive, with phase and group velocities decreasing with increasing wave vector. These results are directly applicable to networks with empty pore space. They also describe the solid matrix in two-component (Biot) theories of fluid-filled porous media. We suggest the possibility of low density materials with higher ratios of stiffness and strength to density than those of foams, aerogels, or trabecular bone.

The ab-initio density matrix renormalization group in practice.

PubMed

Olivares-Amaya, Roberto; Hu, Weifeng; Nakatani, Naoki; Sharma, Sandeep; Yang, Jun; Chan, Garnet Kin-Lic

2015-01-21

The ab-initio density matrix renormalization group (DMRG) is a tool that can be applied to a wide variety of interesting problems in quantum chemistry. Here, we examine the density matrix renormalization group from the vantage point of the quantum chemistry user. What kinds of problems is the DMRG well-suited to? What are the largest systems that can be treated at practical cost? What sort of accuracies can be obtained, and how do we reason about the computational difficulty in different molecules? By examining a diverse benchmark set of molecules: π-electron systems, benchmark main-group and transition metal dimers, and the Mn-oxo-salen and Fe-porphine organometallic compounds, we provide some answers to these questions, and show how the density matrix renormalization group is used in practice.

Resonant-convergent PCM response theory for the calculation of second harmonic generation in makaluvamines A-V: pyrroloiminoquinone marine natural products from poriferans of genus Zyzzya.

PubMed

Milne, Bruce F; Norman, Patrick

2015-05-28

The first-order hyperpolarizability, β, has been calculated for a group of marine natural products, the makaluvamines. These compounds possess a common cationic pyrroloiminoquinone structure that is substituted to varying degrees. Calculations at the MP2 level indicate that makaluvamines possessing phenolic side chains conjugated with the pyrroloiminoquinone moiety display large β values, while breaking this conjugation leads to a dramatic decrease in the calculated hyperpolarizability. This is consistent with a charge-transfer donor-π-acceptor (D-π-A) structure type, characteristic of nonlinear optical chromophores. Dynamic hyperpolarizabilities calculated using resonance-convergent time-dependent density functional theory coupled to polarizable continuum model (PCM) solvation suggest that significant resonance enhancement effects can be expected for incident radiation with wavelengths around 800 nm. The results of the current work suggest that the pyrroloiminoquinone moiety represents a potentially useful new chromophore subunit, in particular for the development of molecular probes for biological imaging. The introduction of solvent-solute interactions in the theory is conventionally made in a density matrix formalism, and the present work will provide detailed account of the approximations that need to be introduced in wave function theory and our program implementation. The program implementation as such is achieved by a mere combination of existing modules from previous developments, and it is here only briefly reviewed.

Development of edge effects around experimental ecosystem hotspots is affected by edge density and matrix type

USDA-ARS?s Scientific Manuscript database

Ecological edge effects are sensitive to landscape context. In particular, edge effects can be altered by matrix type and by the presence of other nearby edges. We experimentally altered patch configurations in an African savanna to determine how edge density and matrix type influence edge effect de...

Effects of autoionising states on the single and double ionisation yields of neon with soft X-ray fields. JMO Series: Attosecond and Strong Field Science

NASA Astrophysics Data System (ADS)

Middleton, D. P. W.; Nikolopoulos, L. A. A.

2012-11-01

In this work, single and double ionisation yields of neon under extreme ultraviolet free-electron laser (FEL) radiation tuned in the vicinity of the autoionising states (AIS) of Ne+ were studied. Density matrix equations were developed and were used to calculate the dependence of the branching ratios of singly and doubly ionised neon on the field intensity and its duration. In addition, in response to a recent experiment [M. Martins et al., Phys. Rev. A 2011, 80, 023411], a quantitative analysis was undertaken in order to reproduce the magnitude of the branching ratios by varying the FEL photon frequency in the range 41.0-42.0 eV in accordance with the experimental report. While the reported variations of the species' branching ratios as a function of the FEL field's photon energy were found, their magnitude and shape differ. In general, the branching ratios are found to be heavily dependent on the given combination of the peak intensity and the pulse duration. Furthermore, the FEL's stochastic fluctuation has been modelled by solving the average density matrix equations and it was found that stochastic effects should also affect branching ratios, mainly due to the increase in the effective bandwidth of the pulse in comparison with the AIS's decay ionisation width. Our calculations suggest that field fluctuations generally diminish the resonance features of the branching ratios.

Atomically thin layers of B-N-C-O with tunable composition.

PubMed

Ozturk, Birol; de-Luna-Bugallo, Andres; Panaitescu, Eugen; Chiaramonti, Ann N; Liu, Fangze; Vargas, Anthony; Jiang, Xueping; Kharche, Neerav; Yavuzcetin, Ozgur; Alnaji, Majed; Ford, Matthew J; Lok, Jay; Zhao, Yongyi; King, Nicholas; Dhar, Nibir K; Dubey, Madan; Nayak, Saroj K; Sridhar, Srinivas; Kar, Swastik

2015-07-01

In recent times, atomically thin alloys of boron, nitrogen, and carbon have generated significant excitement as a composition-tunable two-dimensional (2D) material that demonstrates rich physics as well as application potentials. The possibility of tunably incorporating oxygen, a group VI element, into the honeycomb sp(2)-type 2D-BNC lattice is an intriguing idea from both fundamental and applied perspectives. We present the first report on an atomically thin quaternary alloy of boron, nitrogen, carbon, and oxygen (2D-BNCO). Our experiments suggest, and density functional theory (DFT) calculations corroborate, stable configurations of a honeycomb 2D-BNCO lattice. We observe micrometer-scale 2D-BNCO domains within a graphene-rich 2D-BNC matrix, and are able to control the area coverage and relative composition of these domains by varying the oxygen content in the growth setup. Macroscopic samples comprising 2D-BNCO domains in a graphene-rich 2D-BNC matrix show graphene-like gate-modulated electronic transport with mobility exceeding 500 cm(2) V(-1) s(-1), and Arrhenius-like activated temperature dependence. Spin-polarized DFT calculations for nanoscale 2D-BNCO patches predict magnetic ground states originating from the B atoms closest to the O atoms and sizable (0.6 eV < E g < 0.8 eV) band gaps in their density of states. These results suggest that 2D-BNCO with novel electronic and magnetic properties have great potential for nanoelectronics and spintronic applications in an atomically thin platform.

Density functional theory for molecular and periodic systems using density fitting and continuous fast multipole method: Analytical gradients.

PubMed

Łazarski, Roman; Burow, Asbjörn Manfred; Grajciar, Lukáš; Sierka, Marek

2016-10-30

A full implementation of analytical energy gradients for molecular and periodic systems is reported in the TURBOMOLE program package within the framework of Kohn-Sham density functional theory using Gaussian-type orbitals as basis functions. Its key component is a combination of density fitting (DF) approximation and continuous fast multipole method (CFMM) that allows for an efficient calculation of the Coulomb energy gradient. For exchange-correlation part the hierarchical numerical integration scheme (Burow and Sierka, Journal of Chemical Theory and Computation 2011, 7, 3097) is extended to energy gradients. Computational efficiency and asymptotic O(N) scaling behavior of the implementation is demonstrated for various molecular and periodic model systems, with the largest unit cell of hematite containing 640 atoms and 19,072 basis functions. The overall computational effort of energy gradient is comparable to that of the Kohn-Sham matrix formation. © 2016 Wiley Periodicals, Inc. © 2016 Wiley Periodicals, Inc.

Infrared matrix-isolation and theoretical studies of the reactions of ferrocene with ozone.

PubMed

Kugel, Roger W; Pinelo, Laura F; Ault, Bruce S

2015-03-19

The reactions between ferrocene (Cp2Fe) (2a) and ozone (O3) were studied using low-temperature matrix-isolation techniques coupled with theoretical density functional theory (DFT) calculations. Co-deposition of Ar/Cp2Fe and Ar/O3 gas mixtures onto a cryogenically cooled CsI window produced a dark-green charge-transfer complex, Cp2Fe-O3, that photodecomposed upon red (λ ≥ 600 nm) and infrared (λ ≥ 1000 nm) irradiation but was stable to green or blue irradiation. Products of photodecomposition were characterized by FT-IR, oxygen-18 labeling, and DFT calculations using the B3LYP functionals and the 6-311G++(d,2p) basis set. Likely, photochemical products included four structures having the molecular formula C10H10FeO, identified by DFT calculations based on their calculated infrared spectra and (18)O isotope shifts. Each of these calculated molecules had one intact and fully coordinated η(5)-C5H5 cyclopentadienyl (Cp) ring and (1) an η(5)-C5H5O cyclic ether (pyran ring) (2b), (2) an η(4)-C5H5O linear aldehyde (2c), (3) a bidentate cyclic aldehyde with a seven-membered ring including the iron atom (2d), or (4) an Fe-O bond and an η(2)-C5H5 (Cp) ring (2e). No conclusive evidence for a gas-phase thermal reaction between ferrocene and ozone was observed under the conditions of these experiments. However, strong evidence for a surface-catalyzed thermal reaction was observed in merged-jet experiments wherein the gases were premixed before deposition. Surface-catalyzed ferrocene-ozone reaction products included a thin film of Fe2O3 observed on the walls of the merged tube as well as cyclopentadiene (C5H6), cyclopentadienone (C5H4O), and further oxidation products observed in the matrix. Possible mechanisms for both the photochemical and the thermal reactions are discussed.

Density matrix renormalization group with efficient dynamical electron correlation through range separation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hedegård, Erik Donovan, E-mail: erik.hedegard@phys.chem.ethz.ch; Knecht, Stefan; Reiher, Markus, E-mail: markus.reiher@phys.chem.ethz.ch

2015-06-14

We present a new hybrid multiconfigurational method based on the concept of range-separation that combines the density matrix renormalization group approach with density functional theory. This new method is designed for the simultaneous description of dynamical and static electron-correlation effects in multiconfigurational electronic structure problems.

A matrix-based approach to solving the inverse Frobenius-Perron problem using sequences of density functions of stochastically perturbed dynamical systems

NASA Astrophysics Data System (ADS)

Nie, Xiaokai; Coca, Daniel

2018-01-01

The paper introduces a matrix-based approach to estimate the unique one-dimensional discrete-time dynamical system that generated a given sequence of probability density functions whilst subjected to an additive stochastic perturbation with known density.

A matrix-based approach to solving the inverse Frobenius-Perron problem using sequences of density functions of stochastically perturbed dynamical systems.

PubMed

Nie, Xiaokai; Coca, Daniel

2018-01-01

The paper introduces a matrix-based approach to estimate the unique one-dimensional discrete-time dynamical system that generated a given sequence of probability density functions whilst subjected to an additive stochastic perturbation with known density.

Vibrational and UV spectroscopic studies of 2-coumaranone by experimental and density functional theory calculations

NASA Astrophysics Data System (ADS)

Priya, Y. Sushma; Rao, K. Ramachandra; Chalapathi, P. V.; Satyavani, M.; Veeraiah, A.

2017-09-01

The vibrational and electronic properties of 2-coumaranone have been reported in the ground state using experimental techniques (FT-IR, FT-Raman, UV spectra and fluorescence microscopic imaging) and density functional theory (DFT) employing B3LYP correlation with the 6-31G(d, p) basis set. The theoretically reported optimized parameters, vibrational frequencies etc., were compared with the experimental values, which yielded good concurrence between the experimental and calculated values. The assignments of the vibrational spectra were done with the help of normal co-ordinate analysis (NCA) following the Scaled Quantum Mechanical Force Field(SQMFF) methodology. The whole assignments of fundamental modes were based on the potential energy distribution (PED) matrix. The electric dipole moment and the first order hyperpolarizability of the 2-coumaranone have been computed using quantum mechanical calculations. NBO and HOMO, LUMO analyses have been carried out. UV spectrum of 2-coumaranone was recorded in the region 100-300 nm and compared with the theoretical UV spectrum using TD-DFT and SAC-CI methods by which a good agreement is observed. Fluorescence microscopic imaging study reflects that the compound fluoresces in the green-yellow region.

Acceleration of intensity-modulated radiotherapy dose calculation by importance sampling of the calculation matrices.

PubMed

Thieke, Christian; Nill, Simeon; Oelfke, Uwe; Bortfeld, Thomas

2002-05-01

In inverse planning for intensity-modulated radiotherapy, the dose calculation is a crucial element limiting both the maximum achievable plan quality and the speed of the optimization process. One way to integrate accurate dose calculation algorithms into inverse planning is to precalculate the dose contribution of each beam element to each voxel for unit fluence. These precalculated values are stored in a big dose calculation matrix. Then the dose calculation during the iterative optimization process consists merely of matrix look-up and multiplication with the actual fluence values. However, because the dose calculation matrix can become very large, this ansatz requires a lot of computer memory and is still very time consuming, making it not practical for clinical routine without further modifications. In this work we present a new method to significantly reduce the number of entries in the dose calculation matrix. The method utilizes the fact that a photon pencil beam has a rapid radial dose falloff, and has very small dose values for the most part. In this low-dose part of the pencil beam, the dose contribution to a voxel is only integrated into the dose calculation matrix with a certain probability. Normalization with the reciprocal of this probability preserves the total energy, even though many matrix elements are omitted. Three probability distributions were tested to find the most accurate one for a given memory size. The sampling method is compared with the use of a fully filled matrix and with the well-known method of just cutting off the pencil beam at a certain lateral distance. A clinical example of a head and neck case is presented. It turns out that a sampled dose calculation matrix with only 1/3 of the entries of the fully filled matrix does not sacrifice the quality of the resulting plans, whereby the cutoff method results in a suboptimal treatment plan.

Extension of many-body theory and approximate density functionals to fractional charges and fractional spins.

PubMed

Yang, Weitao; Mori-Sánchez, Paula; Cohen, Aron J

2013-09-14

The exact conditions for density functionals and density matrix functionals in terms of fractional charges and fractional spins are known, and their violation in commonly used functionals has been shown to be the root of many major failures in practical applications. However, approximate functionals are designed for physical systems with integer charges and spins, not in terms of the fractional variables. Here we develop a general framework for extending approximate density functionals and many-electron theory to fractional-charge and fractional-spin systems. Our development allows for the fractional extension of any approximate theory that is a functional of G(0), the one-electron Green's function of the non-interacting reference system. The extension to fractional charge and fractional spin systems is based on the ensemble average of the basic variable, G(0). We demonstrate the fractional extension for the following theories: (1) any explicit functional of the one-electron density, such as the local density approximation and generalized gradient approximations; (2) any explicit functional of the one-electron density matrix of the non-interacting reference system, such as the exact exchange functional (or Hartree-Fock theory) and hybrid functionals; (3) many-body perturbation theory; and (4) random-phase approximations. A general rule for such an extension has also been derived through scaling the orbitals and should be useful for functionals where the link to the Green's function is not obvious. The development thus enables the examination of approximate theories against known exact conditions on the fractional variables and the analysis of their failures in chemical and physical applications in terms of violations of exact conditions of the energy functionals. The present work should facilitate the calculation of chemical potentials and fundamental bandgaps with approximate functionals and many-electron theories through the energy derivatives with respect to the fractional charge. It should play an important role in developing accurate approximate density functionals and many-body theory.

Theoretical Stark broadening parameters for spectral lines arising from the 2p5ns, 2p5np and 2p5nd electronic configurations of Mg III

NASA Astrophysics Data System (ADS)

Colón, C.; Moreno-Díaz, C.; Alonso-Medina, A.

2013-10-01

In the present work we report theoretical Stark widths and shifts calculated using the Griem semi-empirical approach, corresponding to 237 spectral lines of Mg III. Data are presented for an electron density of 1017 cm-3 and temperatures T = 0.5-10.0 (104K). The matrix elements used in these calculations have been determined from 23 configurations of Mg III: 2s22p6, 2s22p53p, 2s22p54p, 2s22p54f and 2s22p55f for even parity and 2s22p5ns (n = 3-6), 2s22p5nd (n = 3-9), 2s22p55g and 2s2p6np (n = 3-8) for odd parity. For the intermediate coupling (IC) calculations, we use the standard method of least-squares fitting from experimental energy levels by means of the Cowan computer code. Also, in order to test the matrix elements used in our calculations, we present calculated values of 70 transition probabilities of Mg III spectral lines and 14 calculated values of radiative lifetimes of Mg III levels. There is good agreement between our calculations and experimental radiative lifetimes. Spectral lines of Mg III are relevant in astrophysics and also play an important role in the spectral analysis of laboratory plasma. Theoretical trends of the Stark broadening parameter versus the temperature for relevant lines are presented. No values of Stark parameters can be found in the bibliography.

Metal matrix-metal nanoparticle composites with tunable melting temperature and high thermal conductivity for phase-change thermal storage.

PubMed

Liu, Minglu; Ma, Yuanyu; Wu, Hsinwei; Wang, Robert Y

2015-02-24

Phase-change materials (PCMs) are of broad interest for thermal storage and management applications. For energy-dense storage with fast thermal charging/discharging rates, a PCM should have a suitable melting temperature, large enthalpy of fusion, and high thermal conductivity. To simultaneously accomplish these traits, we custom design nanocomposites consisting of phase-change Bi nanoparticles embedded in an Ag matrix. We precisely control nanoparticle size, shape, and volume fraction in the composite by separating the nanoparticle synthesis and nanocomposite formation steps. We demonstrate a 50-100% thermal energy density improvement relative to common organic PCMs with equivalent volume fraction. We also tune the melting temperature from 236-252 °C by varying nanoparticle diameter from 8.1-14.9 nm. Importantly, the silver matrix successfully prevents nanoparticle coalescence, and no melting changes are observed during 100 melt-freeze cycles. The nanocomposite's Ag matrix also leads to very high thermal conductivities. For example, the thermal conductivity of a composite with a 10% volume fraction of 13 nm Bi nanoparticles is 128 ± 23 W/m-K, which is several orders of magnitude higher than typical thermal storage materials. We complement these measurements with calculations using a modified effective medium approximation for nanoscale thermal transport. These calculations predict that the thermal conductivity of composites with 13 nm Bi nanoparticles varies from 142 to 47 W/m-K as the nanoparticle volume fraction changes from 10 to 35%. Larger nanoparticle diameters and/or smaller nanoparticle volume fractions lead to larger thermal conductivities.

Entanglement entropy of the Q≥4 quantum Potts chain.

PubMed

Lajkó, Péter; Iglói, Ferenc

2017-01-01

The entanglement entropy S is an indicator of quantum correlations in the ground state of a many-body quantum system. At a second-order quantum phase-transition point in one dimension S generally has a logarithmic singularity. Here we consider quantum spin chains with a first-order quantum phase transition, the prototype being the Q-state quantum Potts chain for Q>4 and calculate S across the transition point. According to numerical, density matrix renormalization group results at the first-order quantum phase transition point S shows a jump, which is expected to vanish for Q→4^{+}. This jump is calculated in leading order as ΔS=lnQ[1-4/Q-2/(QlnQ)+O(1/Q^{2})].

Theoretical analysis for the specific heat and thermal parameters of solid C60

NASA Astrophysics Data System (ADS)

Soto, J. R.; Calles, A.; Castro, J. J.

1997-08-01

We present the results of a theoretical analysis for the thermal parameters and phonon contribution to the specific heat in solid C60. The phonon contribution to the specific heat is calculated through the solution of the corresponding dynamical matrix, for different points in the Brillouin zone, and the construccion of the partial and generalized phonon density of states. The force constants are obtained from a first principle calculation, using a SCF Hartree-Fock wave function from the Gaussian 92 program. The thermal parameters reported are the effective temperatures and vibrational amplitudes as a function of temperature. Using this model we present a parametization scheme in order to reproduce the general behaviour of the experimental specific heat for these materials.

Ramsey scheme for coherent population resonance detection in the optically dense medium

NASA Astrophysics Data System (ADS)

Barantsev, Konstantin; Litvinov, Andrey; Popov, Evgeniy

2018-04-01

This work is devoted to a theoretical investigation of the Ramsey method of detection of the coherent population trapping resonance in cold atomic clouds taking into account collective effects caused by finite optical depth of the considered clouds. The interaction of atoms with pulsed laser radiation is described in the formalism of density matrix by means of Maxwell-Bloch set of equations. The Ramsey signal of coherent population trapping resonance was calculated for the radiation passed through the medium and analyzed for different length of the atomic cloud. Also the population of excited level was calculated in dependence on the two-photon detuning and coordinate along the main optical axis. The light shift of sidebands and appearance of additional harmonics were discovered.

Site-occupation embedding theory using Bethe ansatz local density approximations

NASA Astrophysics Data System (ADS)

Senjean, Bruno; Nakatani, Naoki; Tsuchiizu, Masahisa; Fromager, Emmanuel

2018-06-01

Site-occupation embedding theory (SOET) is an alternative formulation of density functional theory (DFT) for model Hamiltonians where the fully interacting Hubbard problem is mapped, in principle exactly, onto an impurity-interacting (rather than a noninteracting) one. It provides a rigorous framework for combining wave-function (or Green function)-based methods with DFT. In this work, exact expressions for the per-site energy and double occupation of the uniform Hubbard model are derived in the context of SOET. As readily seen from these derivations, the so-called bath contribution to the per-site correlation energy is, in addition to the latter, the key density functional quantity to model in SOET. Various approximations based on Bethe ansatz and perturbative solutions to the Hubbard and single-impurity Anderson models are constructed and tested on a one-dimensional ring. The self-consistent calculation of the embedded impurity wave function has been performed with the density-matrix renormalization group method. It has been shown that promising results are obtained in specific regimes of correlation and density. Possible further developments have been proposed in order to provide reliable embedding functionals and potentials.

Vapor-liquid phase behavior of a size-asymmetric model of ionic fluids confined in a disordered matrix: The collective-variables-based approach

NASA Astrophysics Data System (ADS)

Patsahan, O. V.; Patsahan, T. M.; Holovko, M. F.

2018-02-01

We develop a theory based on the method of collective variables to study the vapor-liquid equilibrium of asymmetric ionic fluids confined in a disordered porous matrix. The approach allows us to formulate the perturbation theory using an extension of the scaled particle theory for a description of a reference system presented as a two-component hard-sphere fluid confined in a hard-sphere matrix. Treating an ionic fluid as a size- and charge-asymmetric primitive model (PM) we derive an explicit expression for the relevant chemical potential of a confined ionic system which takes into account the third-order correlations between ions. Using this expression, the phase diagrams for a size-asymmetric PM are calculated for different matrix porosities as well as for different sizes of matrix and fluid particles. It is observed that general trends of the coexistence curves with the matrix porosity are similar to those of simple fluids under disordered confinement, i.e., the coexistence region gets narrower with a decrease of porosity and, simultaneously, the reduced critical temperature Tc* and the critical density ρi,c * become lower. At the same time, our results suggest that an increase in size asymmetry of oppositely charged ions considerably affects the vapor-liquid diagrams leading to a faster decrease of Tc* and ρi,c * and even to a disappearance of the phase transition, especially for the case of small matrix particles.

Slepton pair production at the LHC in NLO+NLL with resummation-improved parton densities

NASA Astrophysics Data System (ADS)

Fiaschi, Juri; Klasen, Michael

2018-03-01

Novel PDFs taking into account resummation-improved matrix elements, albeit only in the fit of a reduced data set, allow for consistent NLO+NLL calculations of slepton pair production at the LHC. We apply a factorisation method to this process that minimises the effect of the data set reduction, avoids the problem of outlier replicas in the NNPDF method for PDF uncertainties and preserves the reduction of the scale uncertainty. For Run II of the LHC, left-handed selectron/smuon, right-handed and maximally mixed stau production, we confirm that the consistent use of threshold-improved PDFs partially compensates the resummation contributions in the matrix elements. Together with the reduction of the scale uncertainty at NLO+NLL, the described method further increases the reliability of slepton pair production cross sections at the LHC.

The Infrared Spectrum of Matrix Isolated Aminoacetonitrile: A Precursor to the Amino Acid Glycine

NASA Technical Reports Server (NTRS)

Bernstein, Max P.; Bauschlicher, Charles W., Jr.; Sandford, Scott A.

2003-01-01

We present infrared (IR) spectral data from matrix isolation experiments and density functional theory calculations on the pre-biologically interesting molecule aminoacetonitrile, a precursor to glycine. We find that this nitrile has an unusually weak nitrile (C=N) stretch in the infrared, in contrast to expectations based on measurements and models of other nitriles under astrophysical conditions. The absence of an observable nitrile absorption feature in the infrared will make the IR search for this molecule considerably more difficult, and will raise estimates of upper limits on nitriles in interstellar and outer Solar System ices. This is also of relevance to assessing the formation routes of the amino acid glycine, since aminoacetonitrile is the putative precursor to glycine via the Strecker synthesis, the mechanism postulated to have produced the amino acids in meteorites.

Topological Luttinger liquids from decorated domain walls

NASA Astrophysics Data System (ADS)

Parker, Daniel E.; Scaffidi, Thomas; Vasseur, Romain

2018-04-01

We introduce a systematic construction of a gapless symmetry-protected topological phase in one dimension by "decorating" the domain walls of Luttinger liquids. The resulting strongly interacting phases provide a concrete example of a gapless symmetry-protected topological (gSPT) phase with robust symmetry-protected edge modes. Using boundary conformal field theory arguments, we show that while the bulks of such gSPT phases are identical to conventional Luttinger liquids, their boundary critical behavior is controlled by a different, strongly coupled renormalization group fixed point. Our results are checked against extensive density matrix renormalization group calculations.

Effects of electromagnetic fields on the nonlinear optical properties of asymmetric double quantum well under intense laser field

NASA Astrophysics Data System (ADS)

Yesilgul, U.; Sari, H.; Ungan, F.; Martínez-Orozco, J. C.; Restrepo, R. L.; Mora-Ramos, M. E.; Duque, C. A.; Sökmen, I.

2017-03-01

In this study, the effects of electric and magnetic fields on the optical rectification and second and third harmonic generation in asymmetric double quantum well under the intense non-resonant laser field is theoretically investigated. We calculate the optical rectification and second and third harmonic generation within the compact density-matrix approach. The theoretical findings show that the influence of electric, magnetic, and intense laser fields leads to significant changes in the coefficients of nonlinear optical rectification, second and third harmonic generation.

Entanglement transitions induced by large deviations

NASA Astrophysics Data System (ADS)

Bhosale, Udaysinh T.

2017-12-01

The probability of large deviations of the smallest Schmidt eigenvalue for random pure states of bipartite systems, denoted as A and B , is computed analytically using a Coulomb gas method. It is shown that this probability, for large N , goes as exp[-β N2Φ (ζ ) ] , where the parameter β is the Dyson index of the ensemble, ζ is the large deviation parameter, while the rate function Φ (ζ ) is calculated exactly. Corresponding equilibrium Coulomb charge density is derived for its large deviations. Effects of the large deviations of the extreme (largest and smallest) Schmidt eigenvalues on the bipartite entanglement are studied using the von Neumann entropy. Effect of these deviations is also studied on the entanglement between subsystems 1 and 2, obtained by further partitioning the subsystem A , using the properties of the density matrix's partial transpose ρ12Γ. The density of states of ρ12Γ is found to be close to the Wigner's semicircle law with these large deviations. The entanglement properties are captured very well by a simple random matrix model for the partial transpose. The model predicts the entanglement transition across a critical large deviation parameter ζ . Log negativity is used to quantify the entanglement between subsystems 1 and 2. Analytical formulas for it are derived using the simple model. Numerical simulations are in excellent agreement with the analytical results.

Entanglement transitions induced by large deviations.

PubMed

Bhosale, Udaysinh T

2017-12-01

The probability of large deviations of the smallest Schmidt eigenvalue for random pure states of bipartite systems, denoted as A and B, is computed analytically using a Coulomb gas method. It is shown that this probability, for large N, goes as exp[-βN^{2}Φ(ζ)], where the parameter β is the Dyson index of the ensemble, ζ is the large deviation parameter, while the rate function Φ(ζ) is calculated exactly. Corresponding equilibrium Coulomb charge density is derived for its large deviations. Effects of the large deviations of the extreme (largest and smallest) Schmidt eigenvalues on the bipartite entanglement are studied using the von Neumann entropy. Effect of these deviations is also studied on the entanglement between subsystems 1 and 2, obtained by further partitioning the subsystem A, using the properties of the density matrix's partial transpose ρ_{12}^{Γ}. The density of states of ρ_{12}^{Γ} is found to be close to the Wigner's semicircle law with these large deviations. The entanglement properties are captured very well by a simple random matrix model for the partial transpose. The model predicts the entanglement transition across a critical large deviation parameter ζ. Log negativity is used to quantify the entanglement between subsystems 1 and 2. Analytical formulas for it are derived using the simple model. Numerical simulations are in excellent agreement with the analytical results.

C library for topological study of the electronic charge density.

PubMed

Vega, David; Aray, Yosslen; Rodríguez, Jesús

2012-12-05

The topological study of the electronic charge density is useful to obtain information about the kinds of bonds (ionic or covalent) and the atom charges on a molecule or crystal. For this study, it is necessary to calculate, at every space point, the electronic density and its electronic density derivatives values up to second order. In this work, a grid-based method for these calculations is described. The library, implemented for three dimensions, is based on a multidimensional Lagrange interpolation in a regular grid; by differentiating the resulting polynomial, the gradient vector, the Hessian matrix and the Laplacian formulas were obtained for every space point. More complex functions such as the Newton-Raphson method (to find the critical points, where the gradient is null) and the Cash-Karp Runge-Kutta method (used to make the gradient paths) were programmed. As in some crystals, the unit cell has angles different from 90°, the described library includes linear transformations to correct the gradient and Hessian when the grid is distorted (inclined). Functions were also developed to handle grid containing files (grd from DMol® program, CUBE from Gaussian® program and CHGCAR from VASP® program). Each one of these files contains the data for a molecular or crystal electronic property (such as charge density, spin density, electrostatic potential, and others) in a three-dimensional (3D) grid. The library can be adapted to make the topological study in any regular 3D grid by modifying the code of these functions. Copyright © 2012 Wiley Periodicals, Inc.

Interaction cross sections and matter radii of oxygen isotopes using the Glauber model

NASA Astrophysics Data System (ADS)

Ahmad, Suhel; Usmani, A. A.; Ahmad, Shakeb; Khan, Z. A.

2017-05-01

Using the Coulomb modified correlation expansion for the Glauber model S matrix, we calculate the interaction cross sections of oxygen isotopes (O-2616) on 12C at 1.0 GeV/nucleon. The densities of O-2616 are obtained using (i) the Slater determinants consisting of the harmonic oscillator single-particle wave functions (SDHO) and (ii) the relativistic mean-field approach (RMF). Retaining up to the two-body density term in the correlation expansion, the calculations are performed employing the free as well as the in-medium nucleon-nucleon (N N ) scattering amplitude. The in-medium N N amplitude considers the effects arising due to phase variation, higher momentum transfer components, and Pauli blocking. Our main focus in this work is to reveal how could one make the best use of SDHO densities with reference to the RMF one. The results demonstrate that the SDHO densities, along with the in-medium N N amplitude, are able to provide satisfactory explanation of the experimental data. It is found that, except for O,2423, the predicted SDHO matter rms radii of oxygen isotopes closely agree with those obtained using the RMF densities. However, for O,2423, our results require reasonably larger SDHO matter rms radii than the RMF values, thereby predicting thicker neutron skins in 23O and 24O as compared to RMF ones. In conclusion, the results of the present analysis establish the utility of SDHO densities in predicting fairly reliable estimates of the matter rms radii of neutron-rich nuclei.

Assessment of bone mineral density by DXA and the trabecular microarchitecture of the calcaneum by texture analysis in pre- and postmenopausal women in the evaluation of osteoporosis.

PubMed

Karunanithi, R; Ganesan, S; Panicker, T M R; Korath, M Paul; Jagadeesan, K

2007-10-01

The in vivo evaluation of trabecular bone structure could be useful in the diagnosis of osteoporosis for the characterization of therapeutic response and understanding the role of parameters other than bone mineral density (BMD) in defining skeletal status. This study was made to evaluate changes taking place in the trabecular architecture of bone with age and menopausal status in women. The findings are compared with the femoral neck bone as well as the trochantar bone mineral density determined by dual energy X-ray absorptiometry (DXA), which is a standard reference test for evaluation of osteoporosis. Seventy females were recruited for the study, 25 premenopausal (mean age ± SD: 39.4 ± 3.8) and 45 postmenopausal (mean age ± SD: 57.9 ± 7.9) women. The right femoral neck bone mineral density was measured for them by dual energy X-ray absorptiometry (DXA). For the same individuals, lateral view radiographs of the right calcaneum were taken as well. The radiographs were digitized and the region of interest (ROI) of 256 × 256 pixels was selected, the run length matrix was computed for calculating seven parameters [Table 1] and the two dimensional fast Fourier transform of the image was calculated. Using the FFT, the power spectral density (PSD) was derived and the root mean square (RMS) value was determined. Our results confirm that age has a significant influence on the texture of the trabecular bone and bone mineral density.

A density functional approach to ferrogels

NASA Astrophysics Data System (ADS)

Cremer, P.; Heinen, M.; Menzel, A. M.; Löwen, H.

2017-07-01

Ferrogels consist of magnetic colloidal particles embedded in an elastic polymer matrix. As a consequence, their structural and rheological properties are governed by a competition between magnetic particle-particle interactions and mechanical matrix elasticity. Typically, the particles are permanently fixed within the matrix, which makes them distinguishable by their positions. Over time, particle neighbors do not change due to the fixation by the matrix. Here we present a classical density functional approach for such ferrogels. We map the elastic matrix-induced interactions between neighboring colloidal particles distinguishable by their positions onto effective pairwise interactions between indistinguishable particles similar to a ‘pairwise pseudopotential’. Using Monte-Carlo computer simulations, we demonstrate for one-dimensional dipole-spring models of ferrogels that this mapping is justified. We then use the pseudopotential as an input into classical density functional theory of inhomogeneous fluids and predict the bulk elastic modulus of the ferrogel under various conditions. In addition, we propose the use of an ‘external pseudopotential’ when one switches from the viewpoint of a one-dimensional dipole-spring object to a one-dimensional chain embedded in an infinitely extended bulk matrix. Our mapping approach paves the way to describe various inhomogeneous situations of ferrogels using classical density functional concepts of inhomogeneous fluids.

GOCE gravity gradient data for lithospheric modeling - From well surveyed to frontier areas

NASA Astrophysics Data System (ADS)

Bouman, J.; Ebbing, J.; Gradmann, S.; Fuchs, M.; Fattah, R. Abdul; Meekes, S.; Schmidt, M.; Lieb, V.; Haagmans, R.

2012-04-01

We explore how GOCE gravity gradient data can improve modeling of the Earth's lithosphere and thereby contribute to a better understanding of the Earth's dynamic processes. The idea is to invert satellite gravity gradients and terrestrial gravity data in the well explored and understood North-East Atlantic Margin and to compare the results of this inversion, providing improved information about the lithosphere and upper mantle, with results obtained by means of models based upon other sources like seismics and magnetic field information. Transfer of the obtained knowledge to the less explored Rub' al Khali desert is foreseen. We present a case study for the North-East Atlantic margin, where we analyze the use of satellite gravity gradients by comparison with a well-constrained 3D density model that provides a detailed picture from the upper mantle to the top basement (base of sediments). The latter horizon is well resolved from gravity and especially magnetic data, whereas sedimentary layers are mainly constrained from seismic studies, but do in general not show a prominent effect in the gravity and magnetic field. We analyze how gravity gradients can increase confidence in the modeled structures by calculating a sensitivity matrix for the existing 3D model. This sensitivity matrix describes the relation between calculated gravity gradient data and geological structures with respect to their depth, extent and relative density contrast. As the sensitivity of the modeled bodies varies for different tensor components, we can use this matrix for a weighted inversion of gradient data to optimize the model. This sensitivity analysis will be used as input to study the Rub' al Khali desert in Saudi Arabia. In terms of modeling and data availability this is a frontier area. Here gravity gradient data will be used to better identify the extent of anomalous structures within the basin, with the goal to improve the modeling for hydrocarbon exploration purposes.

Computing the Density Matrix in Electronic Structure Theory on Graphics Processing Units.

PubMed

Cawkwell, M J; Sanville, E J; Mniszewski, S M; Niklasson, Anders M N

2012-11-13

The self-consistent solution of a Schrödinger-like equation for the density matrix is a critical and computationally demanding step in quantum-based models of interatomic bonding. This step was tackled historically via the diagonalization of the Hamiltonian. We have investigated the performance and accuracy of the second-order spectral projection (SP2) algorithm for the computation of the density matrix via a recursive expansion of the Fermi operator in a series of generalized matrix-matrix multiplications. We demonstrate that owing to its simplicity, the SP2 algorithm [Niklasson, A. M. N. Phys. Rev. B2002, 66, 155115] is exceptionally well suited to implementation on graphics processing units (GPUs). The performance in double and single precision arithmetic of a hybrid GPU/central processing unit (CPU) and full GPU implementation of the SP2 algorithm exceed those of a CPU-only implementation of the SP2 algorithm and traditional matrix diagonalization when the dimensions of the matrices exceed about 2000 × 2000. Padding schemes for arrays allocated in the GPU memory that optimize the performance of the CUBLAS implementations of the level 3 BLAS DGEMM and SGEMM subroutines for generalized matrix-matrix multiplications are described in detail. The analysis of the relative performance of the hybrid CPU/GPU and full GPU implementations indicate that the transfer of arrays between the GPU and CPU constitutes only a small fraction of the total computation time. The errors measured in the self-consistent density matrices computed using the SP2 algorithm are generally smaller than those measured in matrices computed via diagonalization. Furthermore, the errors in the density matrices computed using the SP2 algorithm do not exhibit any dependence of system size, whereas the errors increase linearly with the number of orbitals when diagonalization is employed.

Unsteady combustion of solid propellants

NASA Astrophysics Data System (ADS)

Chung, T. J.; Kim, P. K.

The oscillatory motions of all field variables (pressure, temperature, velocity, density, and fuel fractions) in the flame zone of solid propellant rocket motors are calculated using the finite element method. The Arrhenius law with a single step forward chemical reaction is used. Effects of radiative heat transfer, impressed arbitrary acoustic wave incidence, and idealized mean flow velocities are also investigated. Boundary conditions are derived at the solid-gas interfaces and at the flame edges which are implemented via Lagrange multipliers. Perturbation expansions of all governing conservation equations up to and including the second order are carried out so that nonlinear oscillations may be accommodated. All excited frequencies are calculated by means of eigenvalue analyses, and the combustion response functions corresponding to these frequencies are determined. It is shown that the use of isoparametric finite elements, Gaussian quadrature integration, and the Lagrange multiplier boundary matrix scheme offers a convenient approach to two-dimensional calculations.

Exact stochastic unraveling of an optical coherence dynamics by cumulant expansion

NASA Astrophysics Data System (ADS)

Olšina, Jan; Kramer, Tobias; Kreisbeck, Christoph; Mančal, Tomáš

2014-10-01

A numerically exact Monte Carlo scheme for calculation of open quantum system dynamics is proposed and implemented. The method consists of a Monte Carlo summation of a perturbation expansion in terms of trajectories in Liouville phase-space with respect to the coupling between the excited states of the molecule. The trajectories are weighted by a complex decoherence factor based on the second-order cumulant expansion of the environmental evolution. The method can be used with an arbitrary environment characterized by a general correlation function and arbitrary coupling strength. It is formally exact for harmonic environments, and it can be used with arbitrary temperature. Time evolution of an optically excited Frenkel exciton dimer representing a molecular exciton interacting with a charge transfer state is calculated by the proposed method. We calculate the evolution of the optical coherence elements of the density matrix and linear absorption spectrum, and compare them with the predictions of standard simulation methods.

Efficient and accurate treatment of electron correlations with correlation matrix renormalization theory

DOE PAGES

Yao, Y. X.; Liu, J.; Liu, C.; ...

2015-08-28

We present an efficient method for calculating the electronic structure and total energy of strongly correlated electron systems. The method extends the traditional Gutzwiller approximation for one-particle operators to the evaluation of the expectation values of two particle operators in the many-electron Hamiltonian. The method is free of adjustable Coulomb parameters, and has no double counting issues in the calculation of total energy, and has the correct atomic limit. We demonstrate that the method describes well the bonding and dissociation behaviors of the hydrogen and nitrogen clusters, as well as the ammonia composed of hydrogen and nitrogen atoms. We alsomore » show that the method can satisfactorily tackle great challenging problems faced by the density functional theory recently discussed in the literature. The computational workload of our method is similar to the Hartree-Fock approach while the results are comparable to high-level quantum chemistry calculations.« less

Plackett-Burman experimental design to facilitate syntactic foam development

DOE PAGES

Smith, Zachary D.; Keller, Jennie R.; Bello, Mollie; ...

2015-09-14

The use of an eight-experiment Plackett–Burman method can assess six experimental variables and eight responses in a polysiloxane-glass microsphere syntactic foam. The approach aims to decrease the time required to develop a tunable polymer composite by identifying a reduced set of variables and responses suitable for future predictive modeling. The statistical design assesses the main effects of mixing process parameters, polymer matrix composition, microsphere density and volume loading, and the blending of two grades of microspheres, using a dummy factor in statistical calculations. Responses cover rheological, physical, thermal, and mechanical properties. The cure accelerator content of the polymer matrix andmore » the volume loading of the microspheres have the largest effects on foam properties. These factors are the most suitable for controlling the gel point of the curing foam, and the density of the cured foam. The mixing parameters introduce widespread variability and therefore should be fixed at effective levels during follow-up testing. Some responses may require greater contrast in microsphere-related factors. As a result, compared to other possible statistical approaches, the run economy of the Plackett–Burman method makes it a valuable tool for rapidly characterizing new foams.« less

The impact of non-Gaussianity upon cosmological forecasts

NASA Astrophysics Data System (ADS)

Repp, A.; Szapudi, I.; Carron, J.; Wolk, M.

2015-12-01

The primary science driver for 3D galaxy surveys is their potential to constrain cosmological parameters. Forecasts of these surveys' effectiveness typically assume Gaussian statistics for the underlying matter density, despite the fact that the actual distribution is decidedly non-Gaussian. To quantify the effect of this assumption, we employ an analytic expression for the power spectrum covariance matrix to calculate the Fisher information for Baryon Acoustic Oscillation (BAO)-type model surveys. We find that for typical number densities, at kmax = 0.5h Mpc-1, Gaussian assumptions significantly overestimate the information on all parameters considered, in some cases by up to an order of magnitude. However, after marginalizing over a six-parameter set, the form of the covariance matrix (dictated by N-body simulations) causes the majority of the effect to shift to the `amplitude-like' parameters, leaving the others virtually unaffected. We find that Gaussian assumptions at such wavenumbers can underestimate the dark energy parameter errors by well over 50 per cent, producing dark energy figures of merit almost three times too large. Thus, for 3D galaxy surveys probing the non-linear regime, proper consideration of non-Gaussian effects is essential.

Quantitative (31)P NMR spectroscopy and (1)H MRI measurements of bone mineral and matrix density differentiate metabolic bone diseases in rat models.

PubMed

Cao, Haihui; Nazarian, Ara; Ackerman, Jerome L; Snyder, Brian D; Rosenberg, Andrew E; Nazarian, Rosalynn M; Hrovat, Mirko I; Dai, Guangping; Mintzopoulos, Dionyssios; Wu, Yaotang

2010-06-01

In this study, bone mineral density (BMD) of normal (CON), ovariectomized (OVX), and partially nephrectomized (NFR) rats was measured by (31)P NMR spectroscopy; bone matrix density was measured by (1)H water- and fat-suppressed projection imaging (WASPI); and the extent of bone mineralization (EBM) was obtained by the ratio of BMD/bone matrix density. The capability of these MR methods to distinguish the bone composition of the CON, OVX, and NFR groups was evaluated against chemical analysis (gravimetry). For cortical bone specimens, BMD of the CON and OVX groups was not significantly different; BMD of the NFR group was 22.1% (by (31)P NMR) and 17.5% (by gravimetry) lower than CON. For trabecular bone specimens, BMD of the OVX group was 40.5% (by (31)P NMR) and 24.6% (by gravimetry) lower than CON; BMD of the NFR group was 26.8% (by (31)P NMR) and 21.5% (by gravimetry) lower than CON. No significant change of cortical bone matrix density between CON and OVX was observed by WASPI or gravimetry; NFR cortical bone matrix density was 10.3% (by WASPI) and 13.9% (by gravimetry) lower than CON. OVX trabecular bone matrix density was 38.0% (by WASPI) and 30.8% (by gravimetry) lower than CON, while no significant change in NFR trabecular bone matrix density was observed by either method. The EBMs of OVX cortical and trabecular specimens were slightly higher than CON but not significantly different from CON. Importantly, EBMs of NFR cortical and trabecular specimens were 12.4% and 26.3% lower than CON by (31)P NMR/WASPI, respectively, and 4.0% and 11.9% lower by gravimetry. Histopathology showed evidence of osteoporosis in the OVX group and severe secondary hyperparathyroidism (renal osteodystrophy) in the NFR group. These results demonstrate that the combined (31)P NMR/WASPI method is capable of discerning the difference in EBM between animals with osteoporosis and those with impaired bone mineralization. Copyright 2010 Elsevier Inc. All rights reserved.

Use of density functional theory orbitals in the GVVPT2 variant of second-order multistate multireference perturbation theory.

PubMed

Hoffmann, Mark R; Helgaker, Trygve

2015-03-05

A new variation of the second-order generalized van Vleck perturbation theory (GVVPT2) for molecular electronic structure is suggested. In contrast to the established procedure, in which CASSCF or MCSCF orbitals are first obtained and subsequently used to define a many-electron model (or reference) space, the use of an orbital space obtained from the local density approximation (LDA) variant of density functional theory is considered. Through a final, noniterative diagonalization of an average Fock matrix within orbital subspaces, quasicanonical orbitals that are otherwise indistinguishable from quasicanonical orbitals obtained from a CASSCF or MCSCF calculation are obtained. Consequently, all advantages of the GVVPT2 method are retained, including use of macroconfigurations to define incomplete active spaces and rigorous avoidance of intruder states. The suggested variant is vetted on three well-known model problems: the symmetric stretching of the O-H bonds in water, the dissociation of N2, and the stretching of ground and excited states C2 to more than twice the equilibrium bond length of the ground state. It is observed that the LDA-based GVVPT2 calculations yield good results, of comparable quality to conventional CASSCF-based calculations. This is true even for the C2 model problem, in which the orbital space for each state was defined by the LDA orbitals. These results suggest that GVVPT2 can be applied to much larger problems than previously accessible.

Stark widths and shifts for spectral lines of Sn IV

NASA Astrophysics Data System (ADS)

de Andrés-García, I.; Alonso-Medina, A.; Colón, C.

2016-01-01

In this paper, we present theoretical Stark widths and shifts calculated corresponding to 66 spectral lines of Sn IV. We use the Griem semi-empirical approach and the COWAN computer code. For the intermediate coupling calculations, the standard method of least-squares fitting from experimental energy levels was used. Data are presented for an electron density of 1017 cm-3 and temperatures T = 1.1-5.0 (104 K). The matrix elements used in these calculations have been determined from 34 configurations of Sn IV: 4d10ns(n = 5-10), 4d10nd(n = 5-8), 4d95s2, 4d95p2, 4d95s5d, 4d85s5p2 and 4d105g for even parity and 4d10np(n = 5-8), 4d10nf (n = 4-6), 4d95snp(n = 5-8), 4d85s25p and 4d95snf (n = 4-10) for odd parity. Also, in order to test the matrix elements used in our calculations, we present calculated values of radiative lifetimes of 14 levels of Sn IV. There is good agreement between our calculations and the experimental radiative lifetimes obtained from the bibliography. The spectral lines of Sn IV are observed in UV spectra of HD 149499 B obtained with the Far Ultraviolet Spectroscopic Explorer, the Goddard High Resolution Spectrograph and the International Ultraviolet Explorer. Theoretical trends of the Stark broadening parameter versus the temperature for relevant lines are presented. Also our values of Stark broadening parameters have been compared with the data available in the bibliography.

IOL calculation using paraxial matrix optics.

PubMed

Haigis, Wolfgang

2009-07-01

Matrix methods have a long tradition in paraxial physiological optics. They are especially suited to describe and handle optical systems in a simple and intuitive manner. While these methods are more and more applied to calculate the refractive power(s) of toric intraocular lenses (IOL), they are hardly used in routine IOL power calculations for cataract and refractive surgery, where analytical formulae are commonly utilized. Since these algorithms are also based on paraxial optics, matrix optics can offer rewarding approaches to standard IOL calculation tasks, as will be shown here. Some basic concepts of matrix optics are introduced and the system matrix for the eye is defined, and its application in typical IOL calculation problems is illustrated. Explicit expressions are derived to determine: predicted refraction for a given IOL power; necessary IOL power for a given target refraction; refractive power for a phakic IOL (PIOL); predicted refraction for a thick lens system. Numerical examples with typical clinical values are given for each of these expressions. It is shown that matrix optics can be applied in a straightforward and intuitive way to most problems of modern routine IOL calculation, in thick or thin lens approximation, for aphakic or phakic eyes.

Detecting Damage in Ceramic Matrix Composites Using Electrical Resistance

NASA Technical Reports Server (NTRS)

Smith, Craig E.; Gyekenyesi, Andrew

2011-01-01

The majority of damage in SiC/SiC ceramic matrix composites subjected to monotonic tensile loads is in the form of distributed matrix cracks. These cracks initiate near stress concentrations, such as 90 deg fiber tows or large matrix pores and continue to accumulate with additional stress until matrix crack saturation is achieved. Such damage is difficult to detect with conventional nondestructive evaluation techniques (immersion ultrasonics, x-ray, etc.). Monitoring a specimen.s electrical resistance change provides an indirect approach for monitoring matrix crack density. Sylramic-iBN fiber- reinforced SiC composites with a melt infiltrated (MI) matrix were tensile tested at room temperature. Results showed an increase in resistance of more than 500% prior to fracture, which can be detected either in situ or post-damage. A relationship between resistance change and matrix crack density was also determined.

Detecting Cracks in Ceramic Matrix Composites by Electrical Resistance

NASA Technical Reports Server (NTRS)

Smith, Craig; Gyekenyesi, Andrew

2011-01-01

The majority of damage in SiC/SiC ceramic matrix composites subjected to monotonic tensile loads is in the form of distributed matrix cracks. These cracks initiate near stress concentrations, such as 90o fiber tows or large matrix pores and continue to accumulate with additional stress until matrix crack saturation is achieved. Such damage is difficult to detect with conventional nondestructive evaluation techniques (immersion ultrasonics, x-ray, etc.). Monitoring a specimen.s electrical resistance change provides an indirect approach for monitoring matrix crack density. Sylramic-iBN fiber- reinforced SiC composites with a melt infiltrated (MI) matrix were tensile tested at room temperature. Results showed an increase in resistance of more than 500% prior to fracture, which can be detected either in situ or post-damage. A relationship between resistance change and matrix crack density was also determined.

Embedded random matrix ensembles from nuclear structure and their recent applications

NASA Astrophysics Data System (ADS)

Kota, V. K. B.; Chavda, N. D.

Embedded random matrix ensembles generated by random interactions (of low body rank and usually two-body) in the presence of a one-body mean field, introduced in nuclear structure physics, are now established to be indispensable in describing statistical properties of a large number of isolated finite quantum many-particle systems. Lie algebra symmetries of the interactions, as identified from nuclear shell model and the interacting boson model, led to the introduction of a variety of embedded ensembles (EEs). These ensembles with a mean field and chaos generating two-body interaction generate in three different stages, delocalization of wave functions in the Fock space of the mean-field basis states. The last stage corresponds to what one may call thermalization and complex nuclei, as seen from many shell model calculations, lie in this region. Besides briefly describing them, their recent applications to nuclear structure are presented and they are (i) nuclear level densities with interactions; (ii) orbit occupancies; (iii) neutrinoless double beta decay nuclear transition matrix elements as transition strengths. In addition, their applications are also presented briefly that go beyond nuclear structure and they are (i) fidelity, decoherence, entanglement and thermalization in isolated finite quantum systems with interactions; (ii) quantum transport in disordered networks connected by many-body interactions with centrosymmetry; (iii) semicircle to Gaussian transition in eigenvalue densities with k-body random interactions and its relation to the Sachdev-Ye-Kitaev (SYK) model for majorana fermions.

Connection between the regular approximation and the normalized elimination of the small component in relativistic quantum theory

NASA Astrophysics Data System (ADS)

Filatov, Michael; Cremer, Dieter

2005-02-01

The regular approximation to the normalized elimination of the small component (NESC) in the modified Dirac equation has been developed and presented in matrix form. The matrix form of the infinite-order regular approximation (IORA) expressions, obtained in [Filatov and Cremer, J. Chem. Phys. 118, 6741 (2003)] using the resolution of the identity, is the exact matrix representation and corresponds to the zeroth-order regular approximation to NESC (NESC-ZORA). Because IORA (=NESC-ZORA) is a variationally stable method, it was used as a suitable starting point for the development of the second-order regular approximation to NESC (NESC-SORA). As shown for hydrogenlike ions, NESC-SORA energies are closer to the exact Dirac energies than the energies from the fifth-order Douglas-Kroll approximation, which is much more computationally demanding than NESC-SORA. For the application of IORA (=NESC-ZORA) and NESC-SORA to many-electron systems, the number of the two-electron integrals that need to be evaluated (identical to the number of the two-electron integrals of a full Dirac-Hartree-Fock calculation) was drastically reduced by using the resolution of the identity technique. An approximation was derived, which requires only the two-electron integrals of a nonrelativistic calculation. The accuracy of this approach was demonstrated for heliumlike ions. The total energy based on the approximate integrals deviates from the energy calculated with the exact integrals by less than 5×10-9hartree units. NESC-ZORA and NESC-SORA can easily be implemented in any nonrelativistic quantum chemical program. Their application is comparable in cost with that of nonrelativistic methods. The methods can be run with density functional theory and any wave function method. NESC-SORA has the advantage that it does not imply a picture change.

Exact and approximate many-body dynamics with stochastic one-body density matrix evolution

NASA Astrophysics Data System (ADS)

Lacroix, Denis

2005-06-01

We show that the dynamics of interacting fermions can be exactly replaced by a quantum jump theory in the many-body density matrix space. In this theory, jumps occur between densities formed of pairs of Slater determinants, Dab=|Φa><Φb|, where each state evolves according to the stochastic Schrödinger equation given by O. Juillet and Ph. Chomaz [Phys. Rev. Lett. 88, 142503 (2002)]. A stochastic Liouville-von Neumann equation is derived as well as the associated. Bogolyubov-Born-Green-Kirwood-Yvon hierarchy. Due to the specific form of the many-body density along the path, the presented theory is equivalent to a stochastic theory in one-body density matrix space, in which each density matrix evolves according to its own mean-field augmented by a one-body noise. Guided by the exact reformulation, a stochastic mean-field dynamics valid in the weak coupling approximation is proposed. This theory leads to an approximate treatment of two-body effects similar to the extended time-dependent Hartree-Fock scheme. In this stochastic mean-field dynamics, statistical mixing can be directly considered and jumps occur on a coarse-grained time scale. Accordingly, numerical effort is expected to be significantly reduced for applications.

Fine structure of the entanglement entropy in the O(2) model.

PubMed

Yang, Li-Ping; Liu, Yuzhi; Zou, Haiyuan; Xie, Z Y; Meurice, Y

2016-01-01

We compare two calculations of the particle density in the superfluid phase of the O(2) model with a chemical potential μ in 1+1 dimensions. The first relies on exact blocking formulas from the Tensor Renormalization Group (TRG) formulation of the transfer matrix. The second is a worm algorithm. We show that the particle number distributions obtained with the two methods agree well. We use the TRG method to calculate the thermal entropy and the entanglement entropy. We describe the particle density, the two entropies and the topology of the world lines as we increase μ to go across the superfluid phase between the first two Mott insulating phases. For a sufficiently large temporal size, this process reveals an interesting fine structure: the average particle number and the winding number of most of the world lines in the Euclidean time direction increase by one unit at a time. At each step, the thermal entropy develops a peak and the entanglement entropy increases until we reach half-filling and then decreases in a way that approximately mirrors the ascent. This suggests an approximate fermionic picture.

Quantitative determination of the lateral density and intermolecular correlation between proteins anchored on the membrane surfaces using grazing incidence small-angle X-ray scattering and grazing incidence X-ray fluorescence.

PubMed

Abuillan, Wasim; Vorobiev, Alexei; Hartel, Andreas; Jones, Nicola G; Engstler, Markus; Tanaka, Motomu

2012-11-28

As a physical model of the surface of cells coated with densely packed, non-crystalline proteins coupled to lipid anchors, we functionalized the surface of phospholipid membranes by coupling of neutravidin to biotinylated lipid anchors. After the characterization of fine structures perpendicular to the plane of membrane using specular X-ray reflectivity, the same membrane was characterized by grazing incidence small angle X-ray scattering (GISAXS). Within the framework of distorted wave Born approximation and two-dimensional Percus-Yevick function, we can analyze the form and structure factors of the non-crystalline, membrane-anchored proteins for the first time. As a new experimental technique to quantify the surface density of proteins on the membrane surface, we utilized grazing incidence X-ray fluorescence (GIXF). Here, the mean intermolecular distance between proteins from the sulfur peak intensities can be calculated by applying Abelé's matrix formalism. The characteristic correlation distance between non-crystalline neutravidin obtained by the GISAXS analysis agrees well with the intermolecular distance calculated by GIXF, suggesting a large potential of the combination of GISAXS and GIXF in probing the lateral density and correlation of non-crystalline proteins displayed on the membrane surface.

Low-Density Parity-Check Code Design Techniques to Simplify Encoding

NASA Astrophysics Data System (ADS)

Perez, J. M.; Andrews, K.

2007-11-01

This work describes a method for encoding low-density parity-check (LDPC) codes based on the accumulate-repeat-4-jagged-accumulate (AR4JA) scheme, using the low-density parity-check matrix H instead of the dense generator matrix G. The use of the H matrix to encode allows a significant reduction in memory consumption and provides the encoder design a great flexibility. Also described are new hardware-efficient codes, based on the same kind of protographs, which require less memory storage and area, allowing at the same time a reduction in the encoding delay.

Block matrix based LU decomposition to analyze kinetic damping in active plasma resonance spectroscopy

NASA Astrophysics Data System (ADS)

Roehl, Jan Hendrik; Oberrath, Jens

2016-09-01

``Active plasma resonance spectroscopy'' (APRS) is a widely used diagnostic method to measure plasma parameter like electron density. Measurements with APRS probes in plasmas of a few Pa typically show a broadening of the spectrum due to kinetic effects. To analyze the broadening a general kinetic model in electrostatic approximation based on functional analytic methods has been presented [ 1 ] . One of the main results is, that the system response function Y(ω) is given in terms of the matrix elements of the resolvent of the dynamic operator evaluated for values on the imaginary axis. To determine the response function of a specific probe the resolvent has to be approximated by a huge matrix which is given by a banded block structure. Due to this structure a block based LU decomposition can be implemented. It leads to a solution of Y(ω) which is given only by products of matrices of the inner block size. This LU decomposition allows to analyze the influence of kinetic effects on the broadening and saves memory and calculation time. Gratitude is expressed to the internal funding of Leuphana University.

Synthesis and Characterisation of ETS-10/Acetate-based Ionic Liquid/Chitosan Mixed Matrix Membranes for CO2/N2 Permeation

PubMed Central

Casado-Coterillo, Clara; López-Guerrero, María del Mar; Irabien, Ángel

2014-01-01

Mixed matrix membranes (MMMs) were prepared by incorporating organic surfactant-free hydrothermally synthesised ETS-10 and 1-ethyl-3-methylimidazolium acetate ionic liquid (IL) to chitosan (CS) polymer matrix. The membrane material characteristics and permselectivity performance of the two-component membranes were compared with the three-component membrane and the pure CS membrane. The addition of IL increased CO2 solubility of the polymer, and, thus, the CO2 affinity was maintained for the MMMs, which can be correlated with the crystallinity, measured by FT-IR, and void fraction calculations from differences between theoretical and experimental densities. The mechanical resistance was enhanced by the ETS-10 nanoparticles, and flexibility decreased in the two-component ETS-10/CS MMMs, but the flexibility imparted by the IL remained in three-component ETS-10/IL/CS MMMs. The results of this work provide insight into another way of facing the adhesion challenge in MMMs and obtain CO2 selective MMMs from renewable or green chemistry materials. PMID:24957178

Double Gamow-Teller Transitions and its Relation to Neutrinoless β β Decay

NASA Astrophysics Data System (ADS)

Shimizu, Noritaka; Menéndez, Javier; Yako, Kentaro

2018-04-01

We study the double Gamow-Teller (DGT) strength distribution of 48Ca with state-of-the-art large-scale nuclear shell model calculations. Our analysis shows that the centroid energy of the DGT giant resonance depends mostly on the isovector pairing interaction, while the resonance width is more sensitive to isoscalar pairing. Pairing correlations are also key in neutrinoless β β (0 ν β β ) decay. We find a simple relation between the centroid energy of the 48Ca DGT giant resonance and the 0 ν β β decay nuclear matrix element. More generally, we observe a very good linear correlation between the DGT transition to the ground state of the final nucleus and the 0 ν β β decay matrix element. The correlation, which originates on the dominant short-range character of both transitions, extends to heavier systems including several β β emitters and also holds in energy-density functional results. Our findings suggest that DGT experiments can be a very valuable tool to obtain information on the value of 0 ν β β decay nuclear matrix elements.

Variational optimization algorithms for uniform matrix product states

NASA Astrophysics Data System (ADS)

Zauner-Stauber, V.; Vanderstraeten, L.; Fishman, M. T.; Verstraete, F.; Haegeman, J.

2018-01-01

We combine the density matrix renormalization group (DMRG) with matrix product state tangent space concepts to construct a variational algorithm for finding ground states of one-dimensional quantum lattices in the thermodynamic limit. A careful comparison of this variational uniform matrix product state algorithm (VUMPS) with infinite density matrix renormalization group (IDMRG) and with infinite time evolving block decimation (ITEBD) reveals substantial gains in convergence speed and precision. We also demonstrate that VUMPS works very efficiently for Hamiltonians with long-range interactions and also for the simulation of two-dimensional models on infinite cylinders. The new algorithm can be conveniently implemented as an extension of an already existing DMRG implementation.

Intense laser field effects on a Woods-Saxon potential quantum well

NASA Astrophysics Data System (ADS)

Restrepo, R. L.; Morales, A. L.; Akimov, V.; Tulupenko, V.; Kasapoglu, E.; Ungan, F.; Duque, C. A.

2015-11-01

This paper presents the results of the theoretical study of the effects of non-resonant intense laser field and electric and magnetic fields on the optical properties in an quantum well (QW) make with Woods-Saxon potential profile. The electric field and intense laser field are applied along the growth direction of the Woods-Saxon quantum well and the magnetic field is oriented perpendicularly. To calculate the energy and the wave functions of the electron in the Woods-Saxon quantum well, the effective mass approximation and the method of envelope wave function are used. The confinement in the Woods-Saxon quantum well is changed drastically by the application of intense laser field or either the effect of electric and magnetic fields. The optical properties are calculated using the compact density matrix.

Breaking the theoretical scaling limit for predicting quasiparticle energies: the stochastic GW approach.

PubMed

Neuhauser, Daniel; Gao, Yi; Arntsen, Christopher; Karshenas, Cyrus; Rabani, Eran; Baer, Roi

2014-08-15

We develop a formalism to calculate the quasiparticle energy within the GW many-body perturbation correction to the density functional theory. The occupied and virtual orbitals of the Kohn-Sham Hamiltonian are replaced by stochastic orbitals used to evaluate the Green function G, the polarization potential W, and, thereby, the GW self-energy. The stochastic GW (sGW) formalism relies on novel theoretical concepts such as stochastic time-dependent Hartree propagation, stochastic matrix compression, and spatial or temporal stochastic decoupling techniques. Beyond the theoretical interest, the formalism enables linear scaling GW calculations breaking the theoretical scaling limit for GW as well as circumventing the need for energy cutoff approximations. We illustrate the method for silicon nanocrystals of varying sizes with N_{e}>3000 electrons.

Matrix- and tensor-based recommender systems for the discovery of currently unknown inorganic compounds

NASA Astrophysics Data System (ADS)

Seko, Atsuto; Hayashi, Hiroyuki; Kashima, Hisashi; Tanaka, Isao

2018-01-01

Chemically relevant compositions (CRCs) and atomic arrangements of inorganic compounds have been collected as inorganic crystal structure databases. Machine learning is a unique approach to search for currently unknown CRCs from vast candidates. Herein we propose matrix- and tensor-based recommender system approaches to predict currently unknown CRCs from database entries of CRCs. Firstly, the performance of the recommender system approaches to discover currently unknown CRCs is examined. A Tucker decomposition recommender system shows the best discovery rate of CRCs as the majority of the top 100 recommended ternary and quaternary compositions correspond to CRCs. Secondly, systematic density functional theory (DFT) calculations are performed to investigate the phase stability of the recommended compositions. The phase stability of the 27 compositions reveals that 23 currently unknown compounds are newly found to be stable. These results indicate that the recommender system has great potential to accelerate the discovery of new compounds.

Bivariate- distribution for transition matrix elements in Breit-Wigner to Gaussian domains of interacting particle systems.

PubMed

Kota, V K B; Chavda, N D; Sahu, R

2006-04-01

Interacting many-particle systems with a mean-field one-body part plus a chaos generating random two-body interaction having strength lambda exhibit Poisson to Gaussian orthogonal ensemble and Breit-Wigner (BW) to Gaussian transitions in level fluctuations and strength functions with transition points marked by lambda = lambda c and lambda = lambda F, respectively; lambda F > lambda c. For these systems a theory for the matrix elements of one-body transition operators is available, as valid in the Gaussian domain, with lambda > lambda F, in terms of orbital occupation numbers, level densities, and an integral involving a bivariate Gaussian in the initial and final energies. Here we show that, using a bivariate-t distribution, the theory extends below from the Gaussian regime to the BW regime up to lambda = lambda c. This is well tested in numerical calculations for 6 spinless fermions in 12 single-particle states.

Numerical homogenization of elastic and thermal material properties for metal matrix composites (MMC)

NASA Astrophysics Data System (ADS)

Schindler, Stefan; Mergheim, Julia; Zimmermann, Marco; Aurich, Jan C.; Steinmann, Paul

2017-01-01

A two-scale material modeling approach is adopted in order to determine macroscopic thermal and elastic constitutive laws and the respective parameters for metal matrix composite (MMC). Since the common homogenization framework violates the thermodynamical consistency for non-constant temperature fields, i.e., the dissipation is not conserved through the scale transition, the respective error is calculated numerically in order to prove the applicability of the homogenization method. The thermomechanical homogenization is applied to compute the macroscopic mass density, thermal expansion, elasticity, heat capacity and thermal conductivity for two specific MMCs, i.e., aluminum alloy Al2024 reinforced with 17 or 30 % silicon carbide particles. The temperature dependency of the material properties has been considered in the range from 0 to 500°C, the melting temperature of the alloy. The numerically determined material properties are validated with experimental data from the literature as far as possible.

UV absorption spectrum of allene radical cations in solid argon

NASA Astrophysics Data System (ADS)

Chin, Chih-Hao; Lin, Meng-Yeh; Huang, Tzu-Ping; Wu, Yu-Jong

2018-05-01

Electron bombardment during deposition of an Ar matrix containing a small proportion of allene generated allene cations. Further irradiation of the matrix sample at 385 nm destroyed the allene cations and formed propyne cations in solid Ar. Both cations were identified according to previously reported IR absorption bands. Using a similar technique, we recorded the ultraviolet absorption spectrum of allene cations in solid Ar. The vibrationally resolved progression recorded in the range of 266-237 nm with intervals of about 800 cm-1 was assigned to the A2E ← X2E transition of allene cations, and the broad continuum absorption recorded in the region of 229-214 nm was assigned to their B2A1 ← X2E transition. These assignments were made based on the observed photolytic behavior of the progressions and the vertical excitation energies and oscillator strengths calculated using time-dependent density functional theory.

Coupled Cluster Method with Single and Double Excitations Tailored by Matrix Product State Wave Functions.

PubMed

Veis, Libor; Antalík, Andrej; Brabec, Jiří; Neese, Frank; Legeza, Örs; Pittner, Jiří

2016-10-03

In the past decade, the quantum chemical version of the density matrix renormalization group (DMRG) method has established itself as the method of choice for calculations of strongly correlated molecular systems. Despite its favorable scaling, it is in practice not suitable for computations of dynamic correlation. We present a novel method for accurate "post-DMRG" treatment of dynamic correlation based on the tailored coupled cluster (CC) theory in which the DMRG method is responsible for the proper description of nondynamic correlation, whereas dynamic correlation is incorporated through the framework of the CC theory. We illustrate the potential of this method on prominent multireference systems, in particular, N 2 and Cr 2 molecules and also oxo-Mn(Salen), for which we have performed the first post-DMRG computations in order to shed light on the energy ordering of the lowest spin states.

Finite-temperature dynamic structure factor of the spin-1 XXZ chain with single-ion anisotropy

NASA Astrophysics Data System (ADS)

Lange, Florian; Ejima, Satoshi; Fehske, Holger

2018-02-01

Improving matrix-product state techniques based on the purification of the density matrix, we are able to accurately calculate the finite-temperature dynamic response of the infinite spin-1 XXZ chain with single-ion anisotropy in the Haldane, large-D , and antiferromagnetic phases. Distinct thermally activated scattering processes make a significant contribution to the spectral weight in all cases. In the Haldane phase, intraband magnon scattering is prominent, and the on-site anisotropy causes the magnon to split into singlet and doublet branches. In the large-D phase response, the intraband signal is separated from an exciton-antiexciton continuum. In the antiferromagnetic phase, holons are the lowest-lying excitations, with a gap that closes at the transition to the Haldane state. At finite temperatures, scattering between domain-wall excitations becomes especially important and strongly enhances the spectral weight for momentum transfer π .

Analyzing the propagation behavior of coherence and polarization degrees of a phase-locked partially coherent radial flat-topped array laser beam in underwater turbulence.

PubMed

Kashani, Fatemeh Dabbagh; Yousefi, Masoud

2016-08-10

In this research, based on an analytical expression for cross-spectral density (CSD) matrix elements, coherence and polarization properties of phase-locked partially coherent flat-topped (PCFT) radial array laser beams propagating through weak oceanic turbulence are analyzed. Spectral degrees of coherence and polarization are analytically calculated using CSD matrix elements. Also, the effective width of spatial degree of coherence (EWSDC) is calculated numerically. The simulation is done by considering the effects of source parameters (such as radius of the array setup's circle, effective width of the spectral degree of coherence, and wavelength) and turbulent ocean factors (such as the rate of dissipation of the turbulent kinetic energy per unit mass of fluid and relative strength of temperature and salinity fluctuations, Kolmogorov micro-scale, and rate of dissipation of the mean squared temperature) in detail. Results indicate that any change in the amount of turbulence factors that increase the turbulence power reduces the EWSDC significantly and causes the reduction in the degree of polarization, and occurs at shorter propagation distances but with smaller magnitudes. In addition, being valid for all conditions, the degradation rate of the EWSDC of Gaussian array beams are more in comparison with the PCFT ones. The simulation and calculation results are shown by graphs.

Distribution of dopant ions around poly(3,4-ethylenedioxythiophene) chains: a theoretical study.

PubMed

Casanovas, Jordi; Zanuy, David; Alemán, Carlos

2017-04-12

The effect of counterions and multiple polymer chains on the properties and structure of poly(3,4-ethylenedioxythiophene) (PEDOT) doped with ClO 4 - has been examined using density functional theory (DFT) calculations with periodic boundary conditions (PBCs). Calculations on a one-dimensional periodic model with four explicit polymer repeat units and two ClO 4 - molecules indicate that the latter are separated as much as possible, with the salt structure and band gap obtained from such ClO 4 - distribution being in excellent agreement with those determined experimentally. On the other hand, DFT calculations on periodic models that include two chains indicate that neighboring PEDOT chains are shifted along the molecular axis by a half of the repeat unit length, with dopant ions intercalated between the polymer molecules acting as cement. In order to support these structural features, classical molecular dynamics (MD) simulations have been performed on a multiphasic system consisting of 69 explicit PEDOT chains anchored onto a steel surface, explicit ClO 4 - anions embedded in the polymer matrix, and an acetonitrile phase layer onto the polymer matrix. Analyses of the radial distribution functions indicate that the all-anti conformation, the relative disposition of adjacent PEDOT chains and the distribution of ClO 4 - dopant ions are fully consistent with periodic DFT predictions. The agreement between two such different methodologies allows reinforcing the microscopic understanding of the PEDOT film structure.

Efficient calculation of the energy of a molecule in an arbitrary electric field

NASA Astrophysics Data System (ADS)

Pulay, Peter; Janowski, Tomasz

In thermodynamic (e.g., Monte Carlo) simulations with electronic embedding, the energy of the active site or solute must be calculated for millions of configurations of the environment (solvent or protein matrix) to obtain reliable statistics. This precludes the use of accurate but expensive ab initio and density functional techniques. Except for the immediate neighbors, the effect of the environment is electrostatic. We show that the energy of a molecule in the irregular field of the environment can be determined very efficiently by expanding the electric potential in known functions, and precalculating the first and second order response of the molecule to the components of the potential. These generalized multipole moments and polarizabilities allow the calculation of the energy of the system without further ab initio calculations. Several expansion functions were explored: polynomials, distributed inverse powers, and sine functions. The latter provide the numerically most stable fit but require new types of integrals. Distributed inverse powers can be simulated using dummy atoms, and energies calculated this way provide a very good approximation to the actual energies in the field of the environment.

Low-density resin impregnated ceramic article and method for making the same

NASA Technical Reports Server (NTRS)

Tran, Huy K. (Inventor); Henline, William D. (Inventor); Hsu, Ming-ta S. (Inventor); Rasky, Daniel J. (Inventor); Riccitiello, Salvatore R. (Inventor)

1997-01-01

A low-density resin impregnated ceramic article advantageously employed as a structural ceramic ablator comprising a matrix of ceramic fibers. The fibers of the ceramic matrix are coated with an organic resin film. The organic resin can be a thermoplastic resin or a cured thermosetting resin. In one embodiment, the resin is uniformly distributed within the ceramic article. In a second embodiment, the resin is distributed so as to provide a density gradient along at least one direction of the ceramic article. The resin impregnated ceramic article is prepared by providing a matrix of ceramic fibers; immersing the matrix of ceramic fibers in a solution of a solvent and an organic resin infiltrant; and removing the solvent to form a resin film on the ceramic fibers.

Polymer-mediated tunneling transport between carbon nanotubes in nanocomposites.

PubMed

Derosa, Pedro A; Michalak, Tyler

2014-05-01

Electron transport in nanocomposites has attracted a good deal of attention for some time now; furthermore, the ability to control its characteristics is a necessary step in the design of multifunctional materials. When conductive nanostructures (for example carbon nanotubes) are inserted in a non-conductive matrix, electron transport below the percolation threshold is dominated by tunneling and thus the conductive characteristics of the composite depends heavily on the characteristics of the tunneling currents between nanoinserts. A parameter-free approach to study tunneling transport between carbon nanotubes across a polymer matrix is presented. The calculation is done with a combination of Density Functional Theory and Green functions (an approach heavily used in molecular electronics) which is shown here to be effective in this non-resonant transport condition. The results show that the method can effectively capture the effect of a dielectric layer in tunneling transport. The current is found to exponentially decrease with the size of the gap for both vacuum and polymer, and that the polymer layer lowers the tunneling barrier enhancing tunneling conduction. For a polyacrylonitrile matrix, a four-fold decrease in the tunneling constant, compared to tunneling in vacuum, is observed, a result that is consistent with available information. The method is very versatile as any DFT functional (or any other quantum mechanics method) can be used and thus the most accurate method for each particular system can be chosen. Furthermore as more methods become available, the calculations can be revised and improved. This approach can be used to design functional materials for fine-tunning the tunneling transport, for instance, the effect of modifying the nanoinsert-matrix interface (for example, by adding functional groups to carbon nanotubes) can be captured and the comparative performance of each interface predicted by simulation.

Resonant scattering due to adatoms in graphene: Top, bridge, and hollow positions

NASA Astrophysics Data System (ADS)

Irmer, Susanne; Kochan, Denis; Lee, Jeongsu; Fabian, Jaroslav

2018-02-01

We present a theoretical study of resonance characteristics in graphene from adatoms with s or pz character binding in top, bridge, and hollow positions. The adatoms are described by two tight-binding parameters: on-site energy and hybridization strength. We explore a wide range of different magnitudes of these parameters by employing T -matrix calculations in the single adatom limit and by tight-binding supercell calculations for dilute adatom coverage. We calculate the density of states and the momentum relaxation rate and extract the resonance level and resonance width. The top position with a large hybridization strength or, equivalently, small on-site energy, induces resonances close to zero energy. The bridge position, compared to top, is more sensitive to variation in the orbital tight-binding parameters. Resonances within the experimentally relevant energy window are found mainly for bridge adatoms with negative on-site energies. The effect of resonances from the top and bridge positions on the density of states and momentum relaxation rate is comparable and both positions give rise to a power-law decay of the resonant state in graphene. The hollow position with s orbital character is affected from destructive interference, which is seen from the very narrow resonance peaks in the density of states and momentum relaxation rate. The resonant state shows no clear tendency to a power-law decay around the impurity and its magnitude decreases strongly with lowering the adatom content in the supercell calculations. This is in contrast to the top and bridge positions. We conclude our study with a comparison to models of pointlike vacancies and strong midgap scatterers. The latter model gives rise to significantly higher momentum relaxation rates than caused by single adatoms.

Finite amplitude method applied to the giant dipole resonance in heavy rare-earth nuclei

NASA Astrophysics Data System (ADS)

Oishi, Tomohiro; Kortelainen, Markus; Hinohara, Nobuo

2016-03-01

Background: The quasiparticle random phase approximation (QRPA), within the framework of nuclear density functional theory (DFT), has been a standard tool to access the collective excitations of atomic nuclei. Recently, the finite amplitude method (FAM) was developed in order to perform the QRPA calculations efficiently without any truncation on the two-quasiparticle model space. Purpose: We discuss the nuclear giant dipole resonance (GDR) in heavy rare-earth isotopes, for which the conventional matrix diagonalization of the QRPA is numerically demanding. A role of the Thomas-Reiche-Kuhn (TRK) sum rule enhancement factor, connected to the isovector effective mass, is also investigated. Methods: The electric dipole photoabsorption cross section was calculated within a parallelized FAM-QRPA scheme. We employed the Skyrme energy density functional self-consistently in the DFT calculation for the ground states and FAM-QRPA calculation for the excitations. Results: The mean GDR frequency and width are mostly reproduced with the FAM-QRPA, when compared to experimental data, although some deficiency is observed with isotopes heavier than erbium. A role of the TRK enhancement factor in actual GDR strength is clearly shown: its increment leads to a shift of the GDR strength to higher-energy region, without a significant change in the transition amplitudes. Conclusions: The newly developed FAM-QRPA scheme shows remarkable efficiency, which enables one to perform systematic analysis of GDR for heavy rare-earth nuclei. The theoretical deficiency of the photoabsorption cross section could not be improved by only adjusting the TRK enhancement factor, suggesting the necessity of an approach beyond self-consistent QRPA and/or a more systematic optimization of the energy density functional (EDF) parameters.

Extracting electron transfer coupling elements from constrained density functional theory

NASA Astrophysics Data System (ADS)

Wu, Qin; Van Voorhis, Troy

2006-10-01

Constrained density functional theory (DFT) is a useful tool for studying electron transfer (ET) reactions. It can straightforwardly construct the charge-localized diabatic states and give a direct measure of the inner-sphere reorganization energy. In this work, a method is presented for calculating the electronic coupling matrix element (Hab) based on constrained DFT. This method completely avoids the use of ground-state DFT energies because they are known to irrationally predict fractional electron transfer in many cases. Instead it makes use of the constrained DFT energies and the Kohn-Sham wave functions for the diabatic states in a careful way. Test calculations on the Zn2+ and the benzene-Cl atom systems show that the new prescription yields reasonable agreement with the standard generalized Mulliken-Hush method. We then proceed to produce the diabatic and adiabatic potential energy curves along the reaction pathway for intervalence ET in the tetrathiafulvalene-diquinone (Q-TTF-Q) anion. While the unconstrained DFT curve has no reaction barrier and gives Hab≈17kcal /mol, which qualitatively disagrees with experimental results, the Hab calculated from constrained DFT is about 3kcal /mol and the generated ground state has a barrier height of 1.70kcal/mol, successfully predicting (Q-TTF-Q)- to be a class II mixed-valence compound.

Broken Time-Reversal Symmetry in Strongly Correlated Ladder Structures

NASA Astrophysics Data System (ADS)

Troyer, Matthias

2004-03-01

A decade after the first detailed numerical investigations of strongly correlated ladder models, exotic and interesting phases are still being discovered. Besides charge and spin density wave states with broken translational symmetry, and resonating valence bond (RVB) type superconductivity, a time reversal symmetry borken phase was recently found at half filling [J.B. Marston et al., Phys. Rev. Lett 89, 056404 (2002)]. In this talk I will present our recent results of density matrix renormalization group (DMRG) calculations [Phys. Rev. Lett. 90, 186401 (2003)], where we provide, for the first time, in a doped strongly correlated system (two-leg ladder), a controlled theoretical demonstration of the existence of this state in which long-range ordered orbital currents are arranged in a staggered pattern. This phase, which we found to coexist with a charge density wave, is known in the literature under the names ``staggered flux phase'', ``orbital antiferromagnetism'' or ``d-density wave (DDW)''. This brings us closer to recent proposals that this order might be realized in the enigmatic pseudogap phase of the cuprate high temperature superconductors.

Development of a poly(dimethylacrylamide) based matrix material for solid phase high density peptide array synthesis employing a laser based material transfer

NASA Astrophysics Data System (ADS)

Ridder, Barbara; Foertsch, Tobias C.; Welle, Alexander; Mattes, Daniela S.; von Bojnicic-Kninski, Clemens M.; Loeffler, Felix F.; Nesterov-Mueller, Alexander; Meier, Michael A. R.; Breitling, Frank

2016-12-01

Poly(dimethylacrylamide) (PDMA) based matrix materials were developed for laser-based in situ solid phase peptide synthesis to produce high density arrays. In this specific array synthesis approach, amino acid derivatives are embedded into a matrix material, serving as a ;solid; solvent material at room temperature. Then, a laser pulse transfers this mixture to the target position on a synthesis slide, where the peptide array is synthesized. Upon heating above the glass transition temperature of the matrix material, it softens, allowing diffusion of the amino acid derivatives to the synthesis surface and serving as a solvent for peptide bond formation. Here, we synthesized PDMA six-arm star polymers, offering the desired matrix material properties, using atom transfer radical polymerization. With the synthesized polymers as matrix material, we structured and synthesized arrays with combinatorial laser transfer. With densities of up to 20,000 peptide spots per cm2, the resolution could be increased compared to the commercially available standard matrix material. Time-of-Flight Secondary Ion Mass Spectrometry experiments revealed the penetration behavior of an amino acid derivative into the prepared acceptor synthesis surface and the effectiveness of the washing protocols.

Joint refinement model for the spin resolved one-electron reduced density matrix of YTiO3 using magnetic structure factors and magnetic Compton profiles data.

PubMed

Gueddida, Saber; Yan, Zeyin; Kibalin, Iurii; Voufack, Ariste Bolivard; Claiser, Nicolas; Souhassou, Mohamed; Lecomte, Claude; Gillon, Béatrice; Gillet, Jean-Michel

2018-04-28

In this paper, we propose a simple cluster model with limited basis sets to reproduce the unpaired electron distributions in a YTiO 3 ferromagnetic crystal. The spin-resolved one-electron-reduced density matrix is reconstructed simultaneously from theoretical magnetic structure factors and directional magnetic Compton profiles using our joint refinement algorithm. This algorithm is guided by the rescaling of basis functions and the adjustment of the spin population matrix. The resulting spin electron density in both position and momentum spaces from the joint refinement model is in agreement with theoretical and experimental results. Benefits brought from magnetic Compton profiles to the entire spin density matrix are illustrated. We studied the magnetic properties of the YTiO 3 crystal along the Ti-O 1 -Ti bonding. We found that the basis functions are mostly rescaled by means of magnetic Compton profiles, while the molecular occupation numbers are mainly modified by the magnetic structure factors.

Dart model for irradiation-induced swelling of dispersion fuel elements including aluminum-fuel interaction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rest, J.; Hofman, G.L.

1997-06-01

The Dispersion Analysis Research Tool (DART) contains models for fission-gas induced fuel swelling, interaction of fuel with the matrix aluminum, resultant reaction-product swelling, and calculation of the stress gradient within the fuel particle. The effects of an aluminide shell on fuel particle swelling are evaluated. Validation of the model is demonstrated by a comparison of DART calculations of fuel swelling of U{sub 3}SiAl-Al and U{sub 3}Si{sub 2}-Al for various dispersion fuel element designs with the data. DART results are compared with data for fuel swelling Of U{sub 3}SiAl-Al in plate, tube, and rod configurations as a function of fission density.more » Plate and tube calculations were performed at a constant fuel temperature of 373 K and 518 K, respectively. An irradiation temperature of 518 K results in a calculated aluminide layer thickness for the Russian tube that is in the center of the measured range (16 {mu}m). Rod calculations were performed with a temperature gradient across the rod characterized by surface and central temperatures of 373 K and 423 K, respectively. The effective yield stress of irradiated Al matrix material and the aluminide was determined by comparing the results of DART calculations with postirradiation immersion volume measurement of U{sub 3}SiAl plates. The values for the effective yield stress were used in all subsequent simulations. The lower calculated fuel swelling in the rod-type element is due to an assumed biaxial stress state. Fuel swelling in plates results in plate thickness increase only. Likewise, in tubes, only the wall thickness increases. Irradiation experiments have shown that plate-type dispersion fuel elements can develop blisters or pillows at high U-235 burnup when fuel compounds exhibiting breakaway swelling are used at moderate to high fuel volume fractions. DART-calculated interaction layer thickness and fuel swelling follows the trends of the observations. 3 refs., 2 figs.« less

Gauge invariance of excitonic linear and nonlinear optical response

NASA Astrophysics Data System (ADS)

Taghizadeh, Alireza; Pedersen, T. G.

2018-05-01

We study the equivalence of four different approaches to calculate the excitonic linear and nonlinear optical response of multiband semiconductors. These four methods derive from two choices of gauge, i.e., length and velocity gauges, and two ways of computing the current density, i.e., direct evaluation and evaluation via the time-derivative of the polarization density. The linear and quadratic response functions are obtained for all methods by employing a perturbative density-matrix approach within the mean-field approximation. The equivalence of all four methods is shown rigorously, when a correct interaction Hamiltonian is employed for the velocity gauge approaches. The correct interaction is written as a series of commutators containing the unperturbed Hamiltonian and position operators, which becomes equivalent to the conventional velocity gauge interaction in the limit of infinite Coulomb screening and infinitely many bands. As a case study, the theory is applied to hexagonal boron nitride monolayers, and the linear and nonlinear optical response found in different approaches are compared.

Atomic Cholesky decompositions: a route to unbiased auxiliary basis sets for density fitting approximation with tunable accuracy and efficiency.

PubMed

Aquilante, Francesco; Gagliardi, Laura; Pedersen, Thomas Bondo; Lindh, Roland

2009-04-21

Cholesky decomposition of the atomic two-electron integral matrix has recently been proposed as a procedure for automated generation of auxiliary basis sets for the density fitting approximation [F. Aquilante et al., J. Chem. Phys. 127, 114107 (2007)]. In order to increase computational performance while maintaining accuracy, we propose here to reduce the number of primitive Gaussian functions of the contracted auxiliary basis functions by means of a second Cholesky decomposition. Test calculations show that this procedure is most beneficial in conjunction with highly contracted atomic orbital basis sets such as atomic natural orbitals, and that the error resulting from the second decomposition is negligible. We also demonstrate theoretically as well as computationally that the locality of the fitting coefficients can be controlled by means of the decomposition threshold even with the long-ranged Coulomb metric. Cholesky decomposition-based auxiliary basis sets are thus ideally suited for local density fitting approximations.

Atomic Cholesky decompositions: A route to unbiased auxiliary basis sets for density fitting approximation with tunable accuracy and efficiency

NASA Astrophysics Data System (ADS)

Aquilante, Francesco; Gagliardi, Laura; Pedersen, Thomas Bondo; Lindh, Roland

2009-04-01

Cholesky decomposition of the atomic two-electron integral matrix has recently been proposed as a procedure for automated generation of auxiliary basis sets for the density fitting approximation [F. Aquilante et al., J. Chem. Phys. 127, 114107 (2007)]. In order to increase computational performance while maintaining accuracy, we propose here to reduce the number of primitive Gaussian functions of the contracted auxiliary basis functions by means of a second Cholesky decomposition. Test calculations show that this procedure is most beneficial in conjunction with highly contracted atomic orbital basis sets such as atomic natural orbitals, and that the error resulting from the second decomposition is negligible. We also demonstrate theoretically as well as computationally that the locality of the fitting coefficients can be controlled by means of the decomposition threshold even with the long-ranged Coulomb metric. Cholesky decomposition-based auxiliary basis sets are thus ideally suited for local density fitting approximations.

A general non-Abelian density matrix renormalization group algorithm with application to the C2 dimer.

PubMed

Sharma, Sandeep

2015-01-14

We extend our previous work [S. Sharma and G. K.-L. Chan, J. Chem. Phys. 136, 124121 (2012)], which described a spin-adapted (SU(2) symmetry) density matrix renormalization group algorithm, to additionally utilize general non-Abelian point group symmetries. A key strength of the present formulation is that the requisite tensor operators are not hard-coded for each symmetry group, but are instead generated on the fly using the appropriate Clebsch-Gordan coefficients. This allows our single implementation to easily enable (or disable) any non-Abelian point group symmetry (including SU(2) spin symmetry). We use our implementation to compute the ground state potential energy curve of the C2 dimer in the cc-pVQZ basis set (with a frozen-core), corresponding to a Hilbert space dimension of 10(12) many-body states. While our calculated energy lies within the 0.3 mEh error bound of previous initiator full configuration interaction quantum Monte Carlo and correlation energy extrapolation by intrinsic scaling calculations, our estimated residual error is only 0.01 mEh, much more accurate than these previous estimates. Due to the additional efficiency afforded by the algorithm, the excitation energies (Te) of eight lowest lying excited states: a(3)Πu, b(3)Σg (-), A(1)Πu, c(3)Σu (+), B(1)Δg, B(') (1)Σg (+), d(3)Πg, and C(1)Πg are calculated, which agree with experimentally derived values to better than 0.06 eV. In addition, we also compute the potential energy curves of twelve states: the three lowest levels for each of the irreducible representations (1)Σg (+), (1)Σu (+), (1)Σg (-), and (1)Σu (-), to an estimated accuracy of 0.1 mEh of the exact result in this basis.

A general non-Abelian density matrix renormalization group algorithm with application to the C2 dimer

NASA Astrophysics Data System (ADS)

Sharma, Sandeep

2015-01-01

We extend our previous work [S. Sharma and G. K.-L. Chan, J. Chem. Phys. 136, 124121 (2012)], which described a spin-adapted (SU(2) symmetry) density matrix renormalization group algorithm, to additionally utilize general non-Abelian point group symmetries. A key strength of the present formulation is that the requisite tensor operators are not hard-coded for each symmetry group, but are instead generated on the fly using the appropriate Clebsch-Gordan coefficients. This allows our single implementation to easily enable (or disable) any non-Abelian point group symmetry (including SU(2) spin symmetry). We use our implementation to compute the ground state potential energy curve of the C2 dimer in the cc-pVQZ basis set (with a frozen-core), corresponding to a Hilbert space dimension of 1012 many-body states. While our calculated energy lies within the 0.3 mEh error bound of previous initiator full configuration interaction quantum Monte Carlo and correlation energy extrapolation by intrinsic scaling calculations, our estimated residual error is only 0.01 mEh, much more accurate than these previous estimates. Due to the additional efficiency afforded by the algorithm, the excitation energies (Te) of eight lowest lying excited states: a3Πu, b 3 Σg - , A1Πu, c 3 Σu + , B1Δg, B ' 1 Σg + , d3Πg, and C1Πg are calculated, which agree with experimentally derived values to better than 0.06 eV. In addition, we also compute the potential energy curves of twelve states: the three lowest levels for each of the irreducible representations 1 Σg + , 1 Σu + , 1 Σg - , and 1 Σu - , to an estimated accuracy of 0.1 mEh of the exact result in this basis.

Electric field induced optical gain of a hydrogenic impurity in a Cd{sub 0.8}Zn{sub 0.2}Se/ZnSe parabolic quantum dot

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jasmine, P. Christina Lily; Peter, A. John, E-mail: a.john.peter@gmail.com

The dependence of electric field on the electronic and optical properties is investigated in a Cd{sub 0.8}Zn{sub 0.2}Se/ZnSe quantum dot. The hydrogenic binding energy, in the presence of electric field, is calculated with the spatial confinement effect. The electric field dependent optical gain with the photon energy is found using compact density matrix method. The results show that the electric field has a great influence on the optical properties of II-VI semiconductor quantum dot.

Effect of Long-Period Ordering of the Structure of a Plant on the Initial Stages of Photosynthesis

NASA Astrophysics Data System (ADS)

Korshunov, M. A.; Shabanov, A. V.; Bukhanov, E. R.; Shabanov, V. F.

2018-01-01

Using data on the structure of plant leaves, specific features of light propagation in biophotoniccrystal structures have been established by the transfer matrix method. Splitting of the stopband in two bands has been found. The density of photonic states and the electromagnetic field value have been calculated. The occurrence of two photosystems (splitting of the stopband in two bands), the peculiarity of the long-wavelength quantum yield and its enhancement (Emerson effect), and water dissociation in the soft mode due to an increase in the electromagnetic field on the layers are explained.

Charge and Spin Dynamics of the Hubbard Chains

NASA Technical Reports Server (NTRS)

Park, Youngho; Liang, Shoudan

1999-01-01

We calculate the local correlation functions of charge and spin for the one-chain and two-chain Hubbard model using density matrix renormalization group method and the recursion technique. Keeping only finite number of states we get good accuracy for the low energy excitations. We study the charge and spin gaps, bandwidths and weights of the spectra for various values of the on-site Coulomb interaction U and the electron filling. In the low energy part, the local correlation functions are different for the charge and spin. The bandwidths are proportional to t for the charge and J for the spin respectively.

Investigating decoherence in a simple system

NASA Technical Reports Server (NTRS)

Albrecht, Andreas

1991-01-01

The results of some simple calculations designed to study quantum decoherence are presented. The physics of quantum decoherence are briefly reviewed, and a very simple 'toy' model is analyzed. Exact solutions are found using numerical techniques. The type of incoherence exhibited by the model can be changed by varying a coupling strength. The author explains why the conventional approach to studying decoherence by checking the diagonality of the density matrix is not always adequate. Two other approaches, the decoherence functional and the Schmidt paths approach, are applied to the toy model and contrasted to each other. Possible problems with each are discussed.

Study on spin filtering and switching action in a double-triangular network chain

NASA Astrophysics Data System (ADS)

Zhang, Yongmei

2018-04-01

Spin transport properties of a double-triangular quantum network with local magnetic moment on backbones and magnetic flux penetrating the network plane are studied. Numerical simulation results show that such a quantum network will be a good candidate for spin filter and spin switch. Local dispersion and density of states are considered in the framework of tight-binding approximation. Transmission coefficients are calculated by the method of transfer matrix. Spin transmission is regulated by substrate magnetic moment and magnetic flux piercing those triangles. Experimental realization of such theoretical research will be conducive to designing of new spintronic devices.

Photon Localization and Dicke Superradiance in Atomic Gases

NASA Astrophysics Data System (ADS)

Akkermans, E.; Gero, A.; Kaiser, R.

2008-09-01

Photon propagation in a gas of N atoms is studied using an effective Hamiltonian describing photon-mediated atomic dipolar interactions. The density P(Γ) of photon escape rates is determined from the spectrum of the N×N random matrix Γij=sin⁡(xij)/xij, where xij is the dimensionless random distance between any two atoms. Varying disorder and system size, a scaling behavior is observed for the escape rates. It is explained using microscopic calculations and a stochastic model which emphasizes the role of cooperative effects in photon localization and provides an interesting relation with statistical properties of “small world networks.”

Collision-induced stimulated photon echoes in ‘strong’ magnetic field

NASA Astrophysics Data System (ADS)

Reshetov, V. A.

2018-05-01

Collision-induced stimulated photon echoes formed in a gaseous medium on the transition with the angular momentum change Ja=0 → Jb=1 under the action of ‘strong’ longitudinal magnetic field, when the echo pulse becomes unpolarized, are considered with an account of elastic depolarizing collisions. In the case of narrow spectral line the explicit expressions for the echo polarization density matrix and the degree of polarization are obtained. In the case of broad spectral line the results of the numeric calculations reproduce qualitatively the curve obtained in the experiments with ytterbium vapor.

The time-dependent density matrix renormalisation group method

NASA Astrophysics Data System (ADS)

Ma, Haibo; Luo, Zhen; Yao, Yao

2018-04-01

Substantial progress of the time-dependent density matrix renormalisation group (t-DMRG) method in the recent 15 years is reviewed in this paper. By integrating the time evolution with the sweep procedures in density matrix renormalisation group (DMRG), t-DMRG provides an efficient tool for real-time simulations of the quantum dynamics for one-dimensional (1D) or quasi-1D strongly correlated systems with a large number of degrees of freedom. In the illustrative applications, the t-DMRG approach is applied to investigate the nonadiabatic processes in realistic chemical systems, including exciton dissociation and triplet fission in polymers and molecular aggregates as well as internal conversion in pyrazine molecule.

Development and application of a 2-electron reduced density matrix approach to electron transport via molecular junctions

NASA Astrophysics Data System (ADS)

Hoy, Erik P.; Mazziotti, David A.; Seideman, Tamar

2017-11-01

Can an electronic device be constructed using only a single molecule? Since this question was first asked by Aviram and Ratner in the 1970s [Chem. Phys. Lett. 29, 277 (1974)], the field of molecular electronics has exploded with significant experimental advancements in the understanding of the charge transport properties of single molecule devices. Efforts to explain the results of these experiments and identify promising new candidate molecules for molecular devices have led to the development of numerous new theoretical methods including the current standard theoretical approach for studying single molecule charge transport, i.e., the non-equilibrium Green's function formalism (NEGF). By pairing this formalism with density functional theory (DFT), a wide variety of transport problems in molecular junctions have been successfully treated. For some systems though, the conductance and current-voltage curves predicted by common DFT functionals can be several orders of magnitude above experimental results. In addition, since density functional theory relies on approximations to the exact exchange-correlation functional, the predicted transport properties can show significant variation depending on the functional chosen. As a first step to addressing this issue, the authors have replaced density functional theory in the NEGF formalism with a 2-electron reduced density matrix (2-RDM) method, creating a new approach known as the NEGF-RDM method. 2-RDM methods provide a more accurate description of electron correlation compared to density functional theory, and they have lower computational scaling compared to wavefunction based methods of similar accuracy. Additionally, 2-RDM methods are capable of capturing static electron correlation which is untreatable by existing NEGF-DFT methods. When studying dithiol alkane chains and dithiol benzene in model junctions, the authors found that the NEGF-RDM predicts conductances and currents that are 1-2 orders of magnitude below those of B3LYP and M06 DFT functionals. This suggests that the NEGF-RDM method could be a viable alternative to NEGF-DFT for molecular junction calculations.

Long-range corrected density functional through the density matrix expansion based semilocal exchange hole.

PubMed

Patra, Bikash; Jana, Subrata; Samal, Prasanjit

2018-03-28

The exchange hole, which is one of the principal constituents of the density functional formalism, can be used to design accurate range-separated hybrid functionals in association with appropriate correlation. In this regard, the exchange hole derived from the density matrix expansion has gained attention due to its fulfillment of some of the desired exact constraints. Thus, the new long-range corrected density functional proposed here combines the meta generalized gradient approximation level exchange functional designed from the density matrix expansion based exchange hole coupled with the ab initio Hartree-Fock exchange through the range separation of the Coulomb interaction operator using the standard error function technique. Then, in association with the Lee-Yang-Parr correlation functional, the assessment and benchmarking of the above newly constructed range-separated functional with various well-known test sets shows its reasonable performance for a broad range of molecular properties, such as thermochemistry, non-covalent interaction and barrier heights of the chemical reactions.

Turbidimetric method for the determination of particle sizes in polypropylene/clay-composites during extrusion.

PubMed

Becker, Wolfgang; Guschin, Viktor; Mikonsaari, Irma; Teipel, Ulrich; Kölle, Sabine; Weiss, Patrick

2017-01-01

Nanocomposites with polypropylene as matrix material and nanoclay as filler were produced in a double twin screw extruder. The extrusion was monitored with a spectrometer in the visible and near-infrared spectral region with a diode array spectrometer. Two probes were installed at the end at the extruder die and the transmission spectra were measured during the extrusion. After measuring the transmission spectra and converting into turbidity units, the particle distribution density was calculated via numerical linear equation system. The distribution density function shows either a bimodal or mono modal shape in dependence of the processing parameters like screw speed, dosage, and concentration of the nanoclays. The method was verified with SEM measurements which yield comparable results. The method is suitable for industrial in-line processing monitoring of particle radii and dispersion process, respectively.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pratap, Surender; Sarkar, Niladri, E-mail: niladri@pilani.bits-pilani.ac.in

Self-Consistent Quantum Method using Schrodinger-Poisson equations have been used for determining the Channel electron density of Nano-Scale MOSFETs for 6nm and 9nm thick channels. The 6nm thick MOSFET show the peak of the electron density at the middle where as the 9nm thick MOSFET shows the accumulation of the electrons at the oxide/semiconductor interface. The electron density in the channel is obtained from the diagonal elements of the density matrix; [ρ]=[1/(1+exp(β(H − μ)))] A Tridiagonal Hamiltonian Matrix [H] is constructed for the oxide/channel/oxide 1D structure for the dual gate MOSFET. This structure is discretized and Finite-Difference method is used formore » constructing the matrix equation. The comparison of these results which are obtained by Quantum methods are done with Semi-Classical methods.« less

Ab initio R-matrix calculations of e+-molecule scattering

NASA Technical Reports Server (NTRS)

Danby, Grahame; Tennyson, Jonathan

1990-01-01

The adaptation of the molecular R-matrix method, originally developed for electron-molecule collision studies, to positron scattering is discussed. Ab initio R-matrix calculations are presented for collisions of low energy positrons with a number of diatomic systems including H2, HF and N2. Differential elastic cross sections for positron-H2 show a minimum at about 45 deg for collision energies between 0.3 and 0.5 Ryd. The calculations predict a bound state of positronHF. Calculations on inelastic processes in N2 and O2 are also discussed.

Simple expression for the quantum Fisher information matrix

NASA Astrophysics Data System (ADS)

Šafránek, Dominik

2018-04-01

Quantum Fisher information matrix (QFIM) is a cornerstone of modern quantum metrology and quantum information geometry. Apart from optimal estimation, it finds applications in description of quantum speed limits, quantum criticality, quantum phase transitions, coherence, entanglement, and irreversibility. We derive a surprisingly simple formula for this quantity, which, unlike previously known general expression, does not require diagonalization of the density matrix, and is provably at least as efficient. With a minor modification, this formula can be used to compute QFIM for any finite-dimensional density matrix. Because of its simplicity, it could also shed more light on the quantum information geometry in general.

Processing and properties of SiC whisker reinforced Si sub 3 N sub 4 ceramic matrix composites

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nunn, S.D.

1991-01-01

Silicon carbide whiskers reinforced silicon nitride ceramic matrix composites were pressureless sintered to high density by liquid phase sintering. Important processing parameters included: whisker dispersion by ultrasonic shear homogenization, particle refinement by attrition milling, pressure slip casting to obtain high greed densities, and sintering in a protective powder bed to limit decomposition. Composites with a {beta}20-Si{sub 3}N{sub 4} solid solution matrix containing 20 vol.% SiC whiskers were sintered to 98-100% theoretical density; composites having a Si{sub 3}N{sub 4} matrix containing YAG sintering aid were sintered to 98% of the theoretical density with 20 vol.% SiC whiskers, and 94% density withmore » 30 vol.% SiC whiskers. Analysis of the pressureless sintered composites revealed orientation of the SiC whiskers and the Si{sub 3}N{sub 4} matrix grains. The mechanical properties of hot pressed Si{sub 3}N{sub 4} composites reinforced with 20 vol.% SiC whiskers were shown to depend on the characteristics of the intergranular phase. Variations in the properties of the composites were analyzed in terms of the amount and morphology of the secondary phase, and the development of internal residual stresses due to the thermal expansion mismatch between the sintering aid phase at the grain boundaries.« less

Adhesion and Interphase Properties of Reinforced Polymeric Composites

NASA Astrophysics Data System (ADS)

Caldwell, Kyle Bernd

Reinforced polymeric composites are an increasingly utilized material with a wide range of applications. Fiber reinforced polymeric composites, in particular, possess impressive mechanical properties at a fraction of the weight of many other building materials. There will always, however, be a demand for producing lighter, stiffer, and stronger materials. Understanding the mechanism of adhesion and ways to engineer the reinforcement-matrix interphase can lead to the development of new materials with improved mechanical properties, and even impart additional functionality such as electrical conductivity. The performance of reinforced polymeric composites is critically dependent upon the adhesion between the reinforcement and the surrounding polymer. The relative adhesion between a filler and a thermoplastic matrix can be predicted using calculable thermodynamic quantities such as the Gibbs free energy of mixing. A recent model, COSMO-SAC, is capable of predicting the adhesion between organo-silane treated glass surfaces and several thermoplastic materials. COSMO-SAC uses information based on the charge distribution of a molecule's surface to calculate many thermodynamic properties. Density functional theory calculations, which are relative inexpensive computations, generate the information necessary to perform the COSMO-SAC analysis and can be performed on any given molecule. The flexibility of the COSMO-SAC model is one of the main advantages it possesses over other methods for calculating thermodynamic quantities. In many cases the adhesion between a reinforcing fiber and the surrounding matrix may be improved by incorporating interphase modifiers in the vicinity of the fiber surface. The modifiers can improve the fracture toughness and modulus of the interphase, which may improve the stress transfer from the matrix to the fiber. In addition, the interphase modifiers may improve the mechanical interlock between the fiber surface and the bulk polymer, leading to improved adhesion. In recent years, the use of so called "migrating agents" have been used to self-assemble nanoparticle reinforced fiber-matrix interphases in thermosetting resin systems. The inclusion of a modest amount of thermoplastic migrating agent can lead to the formation of a self-assembled interphase, without causing aggregation of nanoparticles in the bulk phase. Formulations containing excess migrating agent, however, can induce aggregation in the bulk of increasing severity with increasing migrating agent concentration. Several techniques were used to study the mechanism by which the migrating agents operate including, scanning electron microscopy, and in situ fluorescence microscopy. The self-assembly mechanism by which migrating agents operate is described well by depletion forces, which are depend on the geometry of the approaching objects, as well as the migrating agent molecular weight and concentration.

Hypergraph partitioning implementation for parallelizing matrix-vector multiplication using CUDA GPU-based parallel computing

NASA Astrophysics Data System (ADS)

Murni, Bustamam, A.; Ernastuti, Handhika, T.; Kerami, D.

2017-07-01

Calculation of the matrix-vector multiplication in the real-world problems often involves large matrix with arbitrary size. Therefore, parallelization is needed to speed up the calculation process that usually takes a long time. Graph partitioning techniques that have been discussed in the previous studies cannot be used to complete the parallelized calculation of matrix-vector multiplication with arbitrary size. This is due to the assumption of graph partitioning techniques that can only solve the square and symmetric matrix. Hypergraph partitioning techniques will overcome the shortcomings of the graph partitioning technique. This paper addresses the efficient parallelization of matrix-vector multiplication through hypergraph partitioning techniques using CUDA GPU-based parallel computing. CUDA (compute unified device architecture) is a parallel computing platform and programming model that was created by NVIDIA and implemented by the GPU (graphics processing unit).

Simple Derivation of the Lindblad Equation

ERIC Educational Resources Information Center

Pearle, Philip

2012-01-01

The Lindblad equation is an evolution equation for the density matrix in quantum theory. It is the general linear, Markovian, form which ensures that the density matrix is Hermitian, trace 1, positive and completely positive. Some elementary examples of the Lindblad equation are given. The derivation of the Lindblad equation presented here is…

Properties of Cerium Hydroxides from Matrix Infrared Spectra and Electronic Structure Calculations.

PubMed

Fang, Zongtang; Thanthiriwatte, K Sahan; Dixon, David A; Andrews, Lester; Wang, Xuefeng

2016-02-15

Reactions of laser ablated cerium atoms with hydrogen peroxide or hydrogen and oxygen mixtures diluted in argon and condensed at 4 K produced the Ce(OH)3 and Ce(OH)2 molecules and Ce(OH)2(+) cation as major products. Additional minor products were identified as the Ce(OH)4, HCeO, and OCeOH molecules. These new species were identified from their matrix infrared spectra with D2O2, D2, and (18)O2 isotopic substitution and correlating observed frequencies with values calculated by density functional theory. We find that the amounts of Ce(OH)3 and of the Ce(OH)2(+) cation increase on UV (λ > 220 nm) photolysis, while Ce(OH)2, Ce(OH)4, and HCeO are photosensitive. The observed major species for Ce are in the +III or +II oxidation state, and the minor product, Ce(OH)4, is in the +IV oxidation state. The calculations for the vibrational frequencies with the B3LYP functional agree well with the experiment. The NBO analysis shows significant backbonding to the metal 4f and 5d orbitals for the closed shell species. Most open shell species have the excess spin in the 4f with paired spin in the 5d due to backbonding. The heats of formation of the observed species were derived from the available data from experiment and the calculated reaction energies. The major products in this study are different from similar reactions for Th where the tetrahydroxide was the major species.

Quantum-mechanical approach to predissociation of water dimers in the vibrational adiabatic representation: Importance of channel interactions.

PubMed

Mineo, H; Niu, Y L; Kuo, J L; Lin, S H; Fujimura, Y

2015-08-28

The results of application of the quantum-mechanical adiabatic theory to vibrational predissociation (VPD) of water dimers, (H2O)2 and (D2O)2, are presented. We consider the VPD processes including the totally symmetric OH mode of the dimer and the bending mode of the fragment. The VPD in the adiabatic representation is induced by breakdown of the vibrational adiabatic approximation, and two types of nonadiabatic coupling matrix elements are involved: one provides the VPD induced by the low-frequency dissociation mode and the other provides the VPD through channel interactions induced by the low-frequency modes. The VPD rate constants were calculated using the Fermi golden rule expression. A closed form for the nonadiabatic transition matrix element between the discrete and continuum states was derived in the Morse potential model. All of the parameters used were obtained from the potential surfaces of the water dimers, which were calculated by the density functional theory procedures. The VPD rate constants for the two processes were calculated in the non-Condon scheme beyond the so-called Condon approximation. The channel interactions in and between the initial and final states were taken into account, and those are found to increase the VPD rates by 3(1) orders of magnitude for the VPD processes in (H2O)2 ((D2O)2). The fraction of the bending-excited donor fragments is larger than that of the bending-excited acceptor fragments. The results obtained by quantum-mechanical approach are compared with both experimental and quasi-classical trajectory calculation results.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mineo, H.; Kuo, J. L.; Niu, Y. L.

The results of application of the quantum-mechanical adiabatic theory to vibrational predissociation (VPD) of water dimers, (H{sub 2}O){sub 2} and (D{sub 2}O){sub 2}, are presented. We consider the VPD processes including the totally symmetric OH mode of the dimer and the bending mode of the fragment. The VPD in the adiabatic representation is induced by breakdown of the vibrational adiabatic approximation, and two types of nonadiabatic coupling matrix elements are involved: one provides the VPD induced by the low-frequency dissociation mode and the other provides the VPD through channel interactions induced by the low-frequency modes. The VPD rate constants weremore » calculated using the Fermi golden rule expression. A closed form for the nonadiabatic transition matrix element between the discrete and continuum states was derived in the Morse potential model. All of the parameters used were obtained from the potential surfaces of the water dimers, which were calculated by the density functional theory procedures. The VPD rate constants for the two processes were calculated in the non-Condon scheme beyond the so-called Condon approximation. The channel interactions in and between the initial and final states were taken into account, and those are found to increase the VPD rates by 3(1) orders of magnitude for the VPD processes in (H{sub 2}O){sub 2} ((D{sub 2}O){sub 2}). The fraction of the bending-excited donor fragments is larger than that of the bending-excited acceptor fragments. The results obtained by quantum-mechanical approach are compared with both experimental and quasi-classical trajectory calculation results.« less

Computing the full spectrum of large sparse palindromic quadratic eigenvalue problems arising from surface Green's function calculations

NASA Astrophysics Data System (ADS)

Huang, Tsung-Ming; Lin, Wen-Wei; Tian, Heng; Chen, Guan-Hua

2018-03-01

Full spectrum of a large sparse ⊤-palindromic quadratic eigenvalue problem (⊤-PQEP) is considered arguably for the first time in this article. Such a problem is posed by calculation of surface Green's functions (SGFs) of mesoscopic transistors with a tremendous non-periodic cross-section. For this problem, general purpose eigensolvers are not efficient, nor is advisable to resort to the decimation method etc. to obtain the Wiener-Hopf factorization. After reviewing some rigorous understanding of SGF calculation from the perspective of ⊤-PQEP and nonlinear matrix equation, we present our new approach to this problem. In a nutshell, the unit disk where the spectrum of interest lies is broken down adaptively into pieces small enough that they each can be locally tackled by the generalized ⊤-skew-Hamiltonian implicitly restarted shift-and-invert Arnoldi (G⊤SHIRA) algorithm with suitable shifts and other parameters, and the eigenvalues missed by this divide-and-conquer strategy can be recovered thanks to the accurate estimation provided by our newly developed scheme. Notably the novel non-equivalence deflation is proposed to avoid as much as possible duplication of nearby known eigenvalues when a new shift of G⊤SHIRA is determined. We demonstrate our new approach by calculating the SGF of a realistic nanowire whose unit cell is described by a matrix of size 4000 × 4000 at the density functional tight binding level, corresponding to a 8 × 8nm2 cross-section. We believe that quantum transport simulation of realistic nano-devices in the mesoscopic regime will greatly benefit from this work.

Polymer-grafted gold nanorods in polymer thin films: Dispersion and plasmonic coupling

NASA Astrophysics Data System (ADS)

Hore, Michael-Jon Ainsley

This dissertation describes complementary experimental and theoretical studies to deter- mine the thermodynamic factors that affect the dispersion of polymer-grafted Au nanorods within polymer thin films. Au nanorods exhibit a uniform dispersion with a regular spacing for favorable brush / matrix interactions, such as poly(ethylene glycol) (PEG)-Au / poly(methyl methacrylate) (PMMA) and polystyrene (PS)-Au / poly(2,6-dimethyl-p-phenylene oxide) (PPO). For PEG-Au / PMMA, the nanorods are locally oriented and their dispersion is independent of the ratio of the degree of polymerization of the matrix (P) to that of the brush (N), α = P/N, whereas for chemically similar brush / matrix combinations, such as PS-Au / PS and PEG-Au / poly(ethylene oxide) (PEO), nanorods are randomly dispersed for α 2. For aggregated systems (α > 2), nanorods are found primarily within aggregates containing side-by-side aligned nanorods with a spacing that scales with N. UV-visible spectroscopy and discrete dipole approximation (DDA) calculations demonstrate that coupling between surface plasmons within the aggregates leads to a blue shift in the optical absorption as α increases, indicating the sensitivity of spectroscopy for determining nanorod dispersion in polymer nanocomposite films. Self-consistent field theory (SCFT) calculations and Monte Carlo (MC) simulations show that the aggregation of nanorods for α > 2 can be attributed to depletion-attraction forces caused by autophobic dewetting of the brush and matrix. Finally, miscible blends of PS and PPO are investigated as a route to control depletion-attraction interactions between PS-Au nanorods. Initially, nanorods aggregate in matrices having 50 vol. % PPO and then gradually disperse as PPO becomes the majority component. The brush and matrix density profiles, determined by SCFT, show that PPO segregates into the PS brush, and acts as a compatibilizer, which improves dispersion. As dispersion improves, coupling between surface plasmons is reduced, leading to a red shift in the optical absorption. The outcome of these systematic structure-property-modeling studies is the ability to control nanorod dispersion, orientation, and optical absorption by manipulating brush/matrix interactions and entropic depletion-attraction forces.

Matrix product operators, matrix product states, and ab initio density matrix renormalization group algorithms

NASA Astrophysics Data System (ADS)

Chan, Garnet Kin-Lic; Keselman, Anna; Nakatani, Naoki; Li, Zhendong; White, Steven R.

2016-07-01

Current descriptions of the ab initio density matrix renormalization group (DMRG) algorithm use two superficially different languages: an older language of the renormalization group and renormalized operators, and a more recent language of matrix product states and matrix product operators. The same algorithm can appear dramatically different when written in the two different vocabularies. In this work, we carefully describe the translation between the two languages in several contexts. First, we describe how to efficiently implement the ab initio DMRG sweep using a matrix product operator based code, and the equivalence to the original renormalized operator implementation. Next we describe how to implement the general matrix product operator/matrix product state algebra within a pure renormalized operator-based DMRG code. Finally, we discuss two improvements of the ab initio DMRG sweep algorithm motivated by matrix product operator language: Hamiltonian compression, and a sum over operators representation that allows for perfect computational parallelism. The connections and correspondences described here serve to link the future developments with the past and are important in the efficient implementation of continuing advances in ab initio DMRG and related algorithms.

Matrix product operators, matrix product states, and ab initio density matrix renormalization group algorithms.

PubMed

Chan, Garnet Kin-Lic; Keselman, Anna; Nakatani, Naoki; Li, Zhendong; White, Steven R

2016-07-07

Current descriptions of the ab initio density matrix renormalization group (DMRG) algorithm use two superficially different languages: an older language of the renormalization group and renormalized operators, and a more recent language of matrix product states and matrix product operators. The same algorithm can appear dramatically different when written in the two different vocabularies. In this work, we carefully describe the translation between the two languages in several contexts. First, we describe how to efficiently implement the ab initio DMRG sweep using a matrix product operator based code, and the equivalence to the original renormalized operator implementation. Next we describe how to implement the general matrix product operator/matrix product state algebra within a pure renormalized operator-based DMRG code. Finally, we discuss two improvements of the ab initio DMRG sweep algorithm motivated by matrix product operator language: Hamiltonian compression, and a sum over operators representation that allows for perfect computational parallelism. The connections and correspondences described here serve to link the future developments with the past and are important in the efficient implementation of continuing advances in ab initio DMRG and related algorithms.

One-dimensional continuum electronic structure with the density-matrix renormalization group and its implications for density-functional theory.

PubMed

Stoudenmire, E M; Wagner, Lucas O; White, Steven R; Burke, Kieron

2012-08-03

We extend the density matrix renormalization group to compute exact ground states of continuum many-electron systems in one dimension with long-range interactions. We find the exact ground state of a chain of 100 strongly correlated artificial hydrogen atoms. The method can be used to simulate 1D cold atom systems and to study density-functional theory in an exact setting. To illustrate, we find an interacting, extended system which is an insulator but whose Kohn-Sham system is metallic.

Experimental artefacts occurring during atom probe tomography analysis of oxide nanoparticles in metallic matrix: Quantification and correction

NASA Astrophysics Data System (ADS)

Hatzoglou, C.; Radiguet, B.; Pareige, P.

2017-08-01

Oxide Dispersion Strengthened (ODS) steels are promising candidates for future nuclear reactors, partly due to the fine dispersion of the nanoparticles they contain. Until now, there was no consensus as to the nature of the nanoparticles because their analysis pushed the techniques to their limits and in consequence, introduced some artefacts. In this study, the artefacts that occur during atom probe tomography analysis are quantified. The artefacts quantification reveals that the particles morphology, chemical composition and atomic density are biased. A model is suggested to correct these artefacts in order to obtain a fine and accurate characterization of the nanoparticles. This model is based on volume fraction calculation and an analytical expression of the atomic density. Then, the studied ODS steel reveals nanoparticles, pure in Y, Ti and O, with a core/shell structure. The shell is rich in Cr. The Cr content of the shell is dependent on that of the matrix by a factor of 1.5. This study also shows that 15% of the atoms that were initially in the particles are not detected during the analysis. This only affects O atoms. The particle stoichiometry evolves from YTiO2 for the smallest observed (<2 nm) to Y2TiO5 for the biggest (>8 nm).

Optical and vibrational properties of PbSe nanoparticles synthesized in clinoptilolite

NASA Astrophysics Data System (ADS)

Flores-Valenzuela, J.; Cortez-Valadez, M.; Ramírez-Bon, R.; Arizpe-Chavez, H.; Román-Zamorano, J. F.; Flores-Acosta, M.

2015-08-01

In this work, the optical and vibrational properties of composites based on PbSe semiconductor immersed in a zeolite matrix are reported. The natural zeolite, (clinoptilolite) was used as the host material of PbSe nanoparticles. The method for obtaining these particles is also reported here, which is based on ion exchange processes inside the natural zeolite in alkaline aqueous solution that contains the precursor ions Pb2+ and Se2-. The process of synthesis was conducted temperature, volume, concentration and reaction time of the precursors. The samples were studied by powder X-ray diffraction, TEM (transmission electron microscopy), diffuse reflectance and Raman spectroscopy. The experimental results demonstrate that with this method, the particles with nanometric PbSe sizes were synthesized in the zeolite matrix. Vibrational Raman bands at low wave numbers were detected in these particles by the presence of a shoulder located at 135 cm-1 and a band at around 149 cm-1. The vibrational calculations for small clusters of PbSe at LSDA (Local Spin Density Approximation) level combined with the basis set LANDL2DZ (Los Alamos National Laboratory 2 double ζ), were considered through DFT (Density Functionl Theory). The "breathing" Raman modes located at 119-152 cm-1 were detected for this level of theory.

Neural network based feed-forward high density associative memory

NASA Technical Reports Server (NTRS)

Daud, T.; Moopenn, A.; Lamb, J. L.; Ramesham, R.; Thakoor, A. P.

1987-01-01

A novel thin film approach to neural-network-based high-density associative memory is described. The information is stored locally in a memory matrix of passive, nonvolatile, binary connection elements with a potential to achieve a storage density of 10 to the 9th bits/sq cm. Microswitches based on memory switching in thin film hydrogenated amorphous silicon, and alternatively in manganese oxide, have been used as programmable read-only memory elements. Low-energy switching has been ascertained in both these materials. Fabrication and testing of memory matrix is described. High-speed associative recall approaching 10 to the 7th bits/sec and high storage capacity in such a connection matrix memory system is also described.

Effects of lattice morphology upon reaction dynamics in matrix-isolated systems

NASA Astrophysics Data System (ADS)

Raff, Lionel M.

1992-11-01

The dynamics of the cis-d2-ethylene+F2 addition reaction and the subsequent reaction dynamics of the products isolated in vapor-deposited Ar matrices at 12 K are investigated using trajectory methods that incorporate nonstatistical sampling to enhance the reaction probabilities. The matrix-isolated cis-d2-ethylene+F2 system is generated using a combination of Monte Carlo, damped trajectory, and volume contraction methods. Transport effects of the bulk are simulated using the velocity reset procedure developed by Riley et al. [J. Chem. Phys. 88, 5934 (1988)]. The potential-energy hypersurface is the same as that employed in our previous investigations of the matrix-isolated, decomposition dynamics of 1,2-difluoroethane-d4 and the bimolecular cis-d2-ethylene+F2 system in face-centered-cubic (fcc) matrices [J. Chem. Phys. 93, 3160 (1990); 95, 8901 (1991)]. It is found that matrices generated by these methods are amorphous with numerous vacancies and other imperfections. On the average, there are approximately three vacancies about each lattice atom compared to the fcc crystal. The calculated lattice density is about 82% that for a bulk fcc Ar solid. Computed radial distribution functions resemble those expected for a liquid which exhibits some short-range order. The imperfections of the lattice remain even after substantial annealing at 50 K. The calculated energy relaxation rate to the lattice phonon modes in these amorphous matrices is about a factor of 4 less than that for a close-packed fcc lattice. The 1,2-difluoroethane product is formed primarily via an αβ-addition process, as is the case for fcc matrices. However, the prominence of this pathway is greatly reduced. The major process leading to a fluoroethylene elimination product in amorphous matrices involves an atomic addition mechanism. Such a reaction path accounts for 94% of the elimination reactions. The probability of internal rotation about the C■C double bond in the fluoroethylene product is increased fivefold over that for fcc lattices. The calculated stabilization/elimination product ratio, the cis/trans ratios of fluoroethylene products, and the HF/DF elimination ratio are all found to be in fair to good accord with the reported experimental data. It is concluded that accurate simulation of matrix-isolation experiments requires a matrix model that properly represents the lattice structure present in the experiments.

Noise suppression for dual-energy CT via penalized weighted least-square optimization with similarity-based regularization

DOE Office of Scientific and Technical Information (OSTI.GOV)

Harms, Joseph; Wang, Tonghe; Petrongolo, Michael

Purpose: Dual-energy CT (DECT) expands applications of CT imaging in its capability to decompose CT images into material images. However, decomposition via direct matrix inversion leads to large noise amplification and limits quantitative use of DECT. Their group has previously developed a noise suppression algorithm via penalized weighted least-square optimization with edge-preservation regularization (PWLS-EPR). In this paper, the authors improve method performance using the same framework of penalized weighted least-square optimization but with similarity-based regularization (PWLS-SBR), which substantially enhances the quality of decomposed images by retaining a more uniform noise power spectrum (NPS). Methods: The design of PWLS-SBR is basedmore » on the fact that averaging pixels of similar materials gives a low-noise image. For each pixel, the authors calculate the similarity to other pixels in its neighborhood by comparing CT values. Using an empirical Gaussian model, the authors assign high/low similarity value to one neighboring pixel if its CT value is close/far to the CT value of the pixel of interest. These similarity values are organized in matrix form, such that multiplication of the similarity matrix to the image vector reduces image noise. The similarity matrices are calculated on both high- and low-energy CT images and averaged. In PWLS-SBR, the authors include a regularization term to minimize the L-2 norm of the difference between the images without and with noise suppression via similarity matrix multiplication. By using all pixel information of the initial CT images rather than just those lying on or near edges, PWLS-SBR is superior to the previously developed PWLS-EPR, as supported by comparison studies on phantoms and a head-and-neck patient. Results: On the line-pair slice of the Catphan{sup ©}600 phantom, PWLS-SBR outperforms PWLS-EPR and retains spatial resolution of 8 lp/cm, comparable to the original CT images, even at 90% reduction in noise standard deviation (STD). Similar performance on spatial resolution is observed on an anthropomorphic head phantom. In addition, results of PWLS-SBR show substantially improved image quality due to preservation of image NPS. On the Catphan{sup ©}600 phantom, NPS using PWLS-SBR has a correlation of 93% with that via direct matrix inversion, while the correlation drops to −52% for PWLS-EPR. Electron density measurement studies indicate high accuracy of PWLS-SBR. On seven different materials, the measured electron densities calculated from the decomposed material images using PWLS-SBR have a root-mean-square error (RMSE) of 1.20%, while the results of PWLS-EPR have a RMSE of 2.21%. In the study on a head-and-neck patient, PWLS-SBR is shown to reduce noise STD by a factor of 3 on material images with image qualities comparable to CT images, whereas fine structures are lost in the PWLS-EPR result. Additionally, PWLS-SBR better preserves low contrast on the tissue image. Conclusions: The authors propose improvements to the regularization term of an optimization framework which performs iterative image-domain decomposition for DECT with noise suppression. The regularization term avoids calculation of image gradient and is based on pixel similarity. The proposed method not only achieves a high decomposition accuracy, but also improves over the previous algorithm on NPS as well as spatial resolution.« less

Noise suppression for dual-energy CT via penalized weighted least-square optimization with similarity-based regularization

PubMed Central

Harms, Joseph; Wang, Tonghe; Petrongolo, Michael; Niu, Tianye; Zhu, Lei

2016-01-01

Purpose: Dual-energy CT (DECT) expands applications of CT imaging in its capability to decompose CT images into material images. However, decomposition via direct matrix inversion leads to large noise amplification and limits quantitative use of DECT. Their group has previously developed a noise suppression algorithm via penalized weighted least-square optimization with edge-preservation regularization (PWLS-EPR). In this paper, the authors improve method performance using the same framework of penalized weighted least-square optimization but with similarity-based regularization (PWLS-SBR), which substantially enhances the quality of decomposed images by retaining a more uniform noise power spectrum (NPS). Methods: The design of PWLS-SBR is based on the fact that averaging pixels of similar materials gives a low-noise image. For each pixel, the authors calculate the similarity to other pixels in its neighborhood by comparing CT values. Using an empirical Gaussian model, the authors assign high/low similarity value to one neighboring pixel if its CT value is close/far to the CT value of the pixel of interest. These similarity values are organized in matrix form, such that multiplication of the similarity matrix to the image vector reduces image noise. The similarity matrices are calculated on both high- and low-energy CT images and averaged. In PWLS-SBR, the authors include a regularization term to minimize the L-2 norm of the difference between the images without and with noise suppression via similarity matrix multiplication. By using all pixel information of the initial CT images rather than just those lying on or near edges, PWLS-SBR is superior to the previously developed PWLS-EPR, as supported by comparison studies on phantoms and a head-and-neck patient. Results: On the line-pair slice of the Catphan©600 phantom, PWLS-SBR outperforms PWLS-EPR and retains spatial resolution of 8 lp/cm, comparable to the original CT images, even at 90% reduction in noise standard deviation (STD). Similar performance on spatial resolution is observed on an anthropomorphic head phantom. In addition, results of PWLS-SBR show substantially improved image quality due to preservation of image NPS. On the Catphan©600 phantom, NPS using PWLS-SBR has a correlation of 93% with that via direct matrix inversion, while the correlation drops to −52% for PWLS-EPR. Electron density measurement studies indicate high accuracy of PWLS-SBR. On seven different materials, the measured electron densities calculated from the decomposed material images using PWLS-SBR have a root-mean-square error (RMSE) of 1.20%, while the results of PWLS-EPR have a RMSE of 2.21%. In the study on a head-and-neck patient, PWLS-SBR is shown to reduce noise STD by a factor of 3 on material images with image qualities comparable to CT images, whereas fine structures are lost in the PWLS-EPR result. Additionally, PWLS-SBR better preserves low contrast on the tissue image. Conclusions: The authors propose improvements to the regularization term of an optimization framework which performs iterative image-domain decomposition for DECT with noise suppression. The regularization term avoids calculation of image gradient and is based on pixel similarity. The proposed method not only achieves a high decomposition accuracy, but also improves over the previous algorithm on NPS as well as spatial resolution. PMID:27147376

Massively parallel sparse matrix function calculations with NTPoly

NASA Astrophysics Data System (ADS)

Dawson, William; Nakajima, Takahito

2018-04-01

We present NTPoly, a massively parallel library for computing the functions of sparse, symmetric matrices. The theory of matrix functions is a well developed framework with a wide range of applications including differential equations, graph theory, and electronic structure calculations. One particularly important application area is diagonalization free methods in quantum chemistry. When the input and output of the matrix function are sparse, methods based on polynomial expansions can be used to compute matrix functions in linear time. We present a library based on these methods that can compute a variety of matrix functions. Distributed memory parallelization is based on a communication avoiding sparse matrix multiplication algorithm. OpenMP task parallellization is utilized to implement hybrid parallelization. We describe NTPoly's interface and show how it can be integrated with programs written in many different programming languages. We demonstrate the merits of NTPoly by performing large scale calculations on the K computer.

Stress and Damage in Polymer Matrix Composite Materials Due to Material Degradation at High Temperatures

NASA Technical Reports Server (NTRS)

McManus, Hugh L.; Chamis, Christos C.

1996-01-01

This report describes analytical methods for calculating stresses and damage caused by degradation of the matrix constituent in polymer matrix composite materials. Laminate geometry, material properties, and matrix degradation states are specified as functions of position and time. Matrix shrinkage and property changes are modeled as functions of the degradation states. The model is incorporated into an existing composite mechanics computer code. Stresses, strains, and deformations at the laminate, ply, and micro levels are calculated, and from these calculations it is determined if there is failure of any kind. The rationale for the model (based on published experimental work) is presented, its integration into the laminate analysis code is outlined, and example results are given, with comparisons to existing material and structural data. The mechanisms behind the changes in properties and in surface cracking during long-term aging of polyimide matrix composites are clarified. High-temperature-material test methods are also evaluated.

Exchange Coupling Interactions from the Density Matrix Renormalization Group and N-Electron Valence Perturbation Theory: Application to a Biomimetic Mixed-Valence Manganese Complex.

PubMed

Roemelt, Michael; Krewald, Vera; Pantazis, Dimitrios A

2018-01-09

The accurate description of magnetic level energetics in oligonuclear exchange-coupled transition-metal complexes remains a formidable challenge for quantum chemistry. The density matrix renormalization group (DMRG) brings such systems for the first time easily within reach of multireference wave function methods by enabling the use of unprecedentedly large active spaces. But does this guarantee systematic improvement in predictive ability and, if so, under which conditions? We identify operational parameters in the use of DMRG using as a test system an experimentally characterized mixed-valence bis-μ-oxo/μ-acetato Mn(III,IV) dimer, a model for the oxygen-evolving complex of photosystem II. A complete active space of all metal 3d and bridge 2p orbitals proved to be the smallest meaningful starting point; this is readily accessible with DMRG and greatly improves on the unrealistic metal-only configuration interaction or complete active space self-consistent field (CASSCF) values. Orbital optimization is critical for stabilizing the antiferromagnetic state, while a state-averaged approach over all spin states involved is required to avoid artificial deviations from isotropic behavior that are associated with state-specific calculations. Selective inclusion of localized orbital subspaces enables probing the relative contributions of different ligands and distinct superexchange pathways. Overall, however, full-valence DMRG-CASSCF calculations fall short of providing a quantitative description of the exchange coupling owing to insufficient recovery of dynamic correlation. Quantitatively accurate results can be achieved through a DMRG implementation of second order N-electron valence perturbation theory (NEVPT2) in conjunction with a full-valence metal and ligand active space. Perspectives for future applications of DMRG-CASSCF/NEVPT2 to exchange coupling in oligonuclear clusters are discussed.

Gauge invariance of phenomenological models of the interaction of quantum dissipative systems with electromagnetic fields

NASA Astrophysics Data System (ADS)

Tokman, M. D.

2009-05-01

We discuss specific features of the electrodynamic characteristics of quantum systems within the framework of models that include a phenomenological description of the relaxation processes. As is shown by W. E. Lamb, Jr., R. R. Schlicher, and M. O. Scully [Phys. Rev. A 36, 2763 (1987)], the use of phenomenological relaxation operators, which adequately describe the attenuation of eigenvibrations of a quantum system, may lead to incorrect solutions in the presence of external electromagnetic fields determined by the vector potential for different resonance processes. This incorrectness can be eliminated by giving a gauge-invariant form to the relaxation operator. Lamb, Jr., proposed the corresponding gauge-invariant modification for the Weisskopf-Wigner relaxation operator, which is introduced directly into the Schrödinger equation within the framework of the two-level approximation. In the present paper, this problem is studied for the von Neumann equation supplemented by a relaxation operator. First, we show that the solution of the equation for the density matrix with the relaxation operator correctly obtained “from the first principles” has properties that ensure gauge invariance for the observables. Second, we propose a common recipe for transformation of the phenomenological relaxation operator into the correct (gauge-invariant) form in the density-matrix equations for a multilevel system. Also, we discuss the methods of elimination of other inaccuracies (not related to the gauge-invariance problem) which arise if the electrodynamic response of a dissipative quantum system is calculated within the framework of simplified relaxation models (first of all, the model corresponding to constant relaxation rates of coherences in quantum transitions). Examples illustrating the correctness of the results obtained within the framework of the proposed methods in contrast to inaccuracy of the results of the standard calculation techniques are given.

Ply cracking in composite laminates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Han, Youngmyong.

1989-01-01

Ply cracking behavior and accompanying stiffness changes in thermoset as well as thermoplastic matrix composites under various loading conditions are investigated. Specific topics addressed are: analytical model development for property degradations due to ply cracking under general in-plane loading; crack initiation and multiplication under static loading; and crack multiplication under cyclic loading. A model was developed to calculate the energy released due to ply cracking in a composite laminate subjected to general in-plane loading. The method is based on the use of a second order polynomial to represent the crack opening displacement and the concept of a through-the-thickness inherent flaw.more » The model is then used in conjunction with linear elastic fracture mechanics to predict the progressive ply cracking as well as first ply cracking. A resistance curve for crack multiplication is proposed as a means of characterizing the resistance to ply cracking in composite laminates. A methodology of utilizing the resistance curve to assess the crack density or overloading is also discussed. The method was applied to the graphite/thermoplastic polyimide composite to predict progressive ply cracking. However, unlike the thermoset matrix composites, a strength model is found to fit the experimental results better than the fracture mechanics based model. A set of closed form equations is also developed to calculate the accompanying stiffness changes due to the ply cracking. The effect of thermal residual stress is included in the analysis. A new method is proposed to characterize transverse ply cracking of symmetric balanced laminates under cyclic loading. The method is based on the concept of a through-the-thickness inherent flaw, the Paris law, and the resistance curve. Only two constants are needed to predict the crack density as a function of fatigue cycles.« less

Polarimetric signatures of a canopy of dielectric cylinders based on first and second order vector radiative transfer theory

NASA Technical Reports Server (NTRS)

Tsang, Leung; Chan, Chi Hou; Kong, Jin AU; Joseph, James

1992-01-01

Complete polarimetric signatures of a canopy of dielectric cylinders overlying a homogeneous half space are studied with the first and second order solutions of the vector radiative transfer theory. The vector radiative transfer equations contain a general nondiagonal extinction matrix and a phase matrix. The energy conservation issue is addressed by calculating the elements of the extinction matrix and the elements of the phase matrix in a manner that is consistent with energy conservation. Two methods are used. In the first method, the surface fields and the internal fields of the dielectric cylinder are calculated by using the fields of an infinite cylinder. The phase matrix is calculated and the extinction matrix is calculated by summing the absorption and scattering to ensure energy conservation. In the second method, the method of moments is used to calculate the elements of the extinction and phase matrices. The Mueller matrix based on the first order and second order multiple scattering solutions of the vector radiative transfer equation are calculated. Results from the two methods are compared. The vector radiative transfer equations, combined with the solution based on method of moments, obey both energy conservation and reciprocity. The polarimetric signatures, copolarized and depolarized return, degree of polarization, and phase differences are studied as a function of the orientation, sizes, and dielectric properties of the cylinders. It is shown that second order scattering is generally important for vegetation canopy at C band and can be important at L band for some cases.

Microstructural study and densification analysis of hot work tool steel matrix composites reinforced with TiB{sub 2} particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fedrizzi, A., E-mail: anna.fedrizzi@ing.unitn.it; Pellizzari, M.; Zadra, M.

2013-12-15

Hot work tool steels are characterized by good toughness and high hot hardness but are less wear resistant than other tooling materials, such as high speed steel. Metal matrix composites show improved tribological behavior, but not much work has been done in the field of hot work tool steels. In this paper TiB{sub 2}-reinforced hot work tool steel matrix composites were produced by spark plasma sintering (SPS). Mechanical alloying (MA) was proposed as a suited process to improve the composite microstructure. Density measurements and microstructure confirmed that MA promotes sintering and produces a fine and homogeneous dispersion of reinforcing particles.more » X-ray diffraction patterns of the sintered composites highlighted the formation of equilibrium Fe{sub 2}B and TiC, as predicted by thermodynamic calculations using Thermo-Calc® software. Scanning electron microscopy as well as scanning Kelvin probe force microscopy highlighted the reaction of the steel matrix with TiB{sub 2} particles, showing the formation of a reaction layer at the TiB{sub 2}-steel interface. Phase investigations pointed out that TiB{sub 2} is not chemically stable in steel matrix because of the presence of carbon even during short time SPS. - Highlights: • TiB{sub 2} reinforced steel matrix composites were produced by spark plasma sintering. • TiB{sub 2} was successfully dispersed in the steel matrix by mechanical alloying. • Steel and TiB{sub 2} react during sintering forming equilibrium Fe{sub 2}B and TiC. • The new phases were investigated by means of AFM, Volta potential and XRD analyses.« less

Contaminant transport in fractured rocks with significant matrix permeability, using natural fracture geometries

NASA Astrophysics Data System (ADS)

Odling, Noelle E.; Roden, Julie E.

1997-09-01

Some results from numerical models of flow and contaminant transport in fractured permeable rocks, where fractures are more conductive than rock matrix, are described. The 2D flow field in the fractured and permeable rock matrix is calculated using a finite difference, 'conductance mesh' method, and the contaminant transport is simulated by particle tracking methods using an advection-biased, random walk technique. The model is applied to simulated and naturally occurring fracture patterns. The simulated pattern is an en echelon array of unconnected fractures, as an example of a common, naturally occurring fracture geometry. Two natural fracture patterns are used: one of unconnected, sub-parallel fractures and one with oblique fracture sets which is well connected. Commonly occurring matrix permeability and fracture aperture values are chosen. The simulations show that the presence of fractures creates complex and heterogeneous flow fields and contaminant distribution in the permeable rock matrix. The modelling results have shown that some effects are non-intuitive and therefore difficult to foresee without the help of a model. With respect to contaminant transport rates and plume heterogeneity, it was found that fracture connectivity (crucial when the matrix is impermeable) can play a secondary role to fracture orientation and density. Connected fracture systems can produce smooth break-through curves of contaminants summed over, for example, a bore-hole length, whereas in detail the contaminant plume is spatially highly heterogeneous. Close to a constant-pressure boundary (e.g. an extraction bore-hole), flow and contaminants can be channelled by fractures. Thus observations at a bore-hole may suggest that contaminants are largely confined to the fracture system, when, in fact, significant contamination resides in the matrix.

Entanglement between atomic thermal states and coherent or squeezed photons in a damping cavity

NASA Astrophysics Data System (ADS)

Yadollahi, F.; Safaiee, R.; Golshan, M. M.

2018-02-01

In the present study, the standard Jaynes-Cummings model, in a lossy cavity, is employed to characterize the entanglement between atoms and photons when the former is initially in a thermal state (mixed ensemble) while the latter is described by either coherent or squeezed distributions. The whole system is thus assumed to be in equilibrium with a heat reservoir at a finite temperature T, and the measure of negativity is used to determine the time evolution of atom-photon entanglement. To this end, the master equation for the density matrix, in the secular approximation, is solved and a partial transposition of the result is made. The degree of atom-photon entanglement is then numerically computed, through the negativity, as a function of time and temperature. To justify the behavior of atom-photon entanglement, moreover, we employ the so obtained total density matrix to compute and analyze the time evolution of the initial photonic coherent or squeezed probability distributions and the squeezing parameters. On more practical points, our results demonstrate that as the initial photon mean number increases, the atom-photon entanglement decays at a faster pace for the coherent distribution compared to the squeezed one. Moreover, it is shown that the degree of atom-photon entanglement is much higher and more stable for the squeezed distribution than that for the coherent one. Consequently, we conclude that the time intervals during which the atom-photon entanglement is distillable is longer for the squeezed distribution. It is also illustrated that as the temperature increases the rate of approaching separability is faster for the coherent initial distribution. The novel point of the present report is the calculation of dynamical density matrix (containing all physical information) for the combined system of atom-photon in a lossy cavity, as well as the corresponding negativity, at a finite temperature.

Engine materials characterization and damage monitoring by using x ray technologies

NASA Technical Reports Server (NTRS)

Baaklini, George Y.

1993-01-01

X ray attenuation measurement systems that are capable of characterizing density variations in monolithic ceramics and damage due to processing and/or mechanical testing in ceramic and intermetallic matrix composites are developed and applied. Noninvasive monitoring of damage accumulation and failure sequences in ceramic matrix composites is used during room-temperature tensile testing. This work resulted in the development of a point-scan digital radiography system and an in situ x ray material testing system. The former is used to characterize silicon carbide and silicon nitride specimens, and the latter is used to image the failure behavior of silicon-carbide-fiber-reinforced, reaction-bonded silicon nitride matrix composites. State-of-the-art x ray computed tomography is investigated to determine its capabilities and limitations in characterizing density variations of subscale engine components (e.g., a silicon carbide rotor, a silicon nitride blade, and a silicon-carbide-fiber-reinforced beta titanium matrix rod, rotor, and ring). Microfocus radiography, conventional radiography, scanning acoustic microscopy, and metallography are used to substantiate the x ray computed tomography findings. Point-scan digital radiography is a viable technique for characterizing density variations in monolithic ceramic specimens. But it is very limited and time consuming in characterizing ceramic matrix composites. Precise x ray attenuation measurements, reflecting minute density variations, are achieved by photon counting and by using microcollimators at the source and the detector. X ray computed tomography is found to be a unique x ray attenuation measurement technique capable of providing cross-sectional spatial density information in monolithic ceramics and metal matrix composites. X ray computed tomography is proven to accelerate generic composite component development. Radiographic evaluation before, during, and after loading shows the effect of preexisting volume flaws on the fracture behavior of composites. Results from one-, three-, five-, and eight-ply ceramic composite specimens show that x ray film radiography can monitor damage accumulation during tensile loading. Matrix cracking, fiber-matrix debonding, fiber bridging, and fiber pullout are imaged throughout the tensile loading of the specimens. In situ film radiography is found to be a practical technique for estimating interfacial shear strength between the silicon carbide fibers and the reaction-bonded silicon nitride matrix. It is concluded that pretest, in situ, and post-test x ray imaging can provide greater understanding of ceramic matrix composite mechanical behavior.

Three-dimensional matrix fiber alignment modulates cell migration and MT1-MMP utility by spatially and temporally directing protrusions

NASA Astrophysics Data System (ADS)

Fraley, Stephanie I.; Wu, Pei-Hsun; He, Lijuan; Feng, Yunfeng; Krisnamurthy, Ranjini; Longmore, Gregory D.; Wirtz, Denis

2015-10-01

Multiple attributes of the three-dimensional (3D) extracellular matrix (ECM) have been independently implicated as regulators of cell motility, including pore size, crosslink density, structural organization, and stiffness. However, these parameters cannot be independently varied within a complex 3D ECM protein network. We present an integrated, quantitative study of these parameters across a broad range of complex matrix configurations using self-assembling 3D collagen and show how each parameter relates to the others and to cell motility. Increasing collagen density resulted in a decrease and then an increase in both pore size and fiber alignment, which both correlated significantly with cell motility but not bulk matrix stiffness within the range tested. However, using the crosslinking enzyme Transglutaminase II to alter microstructure independently of density revealed that motility is most significantly predicted by fiber alignment. Cellular protrusion rate, protrusion orientation, speed of migration, and invasion distance showed coupled biphasic responses to increasing collagen density not predicted by 2D models or by stiffness, but instead by fiber alignment. The requirement of matrix metalloproteinase (MMP) activity was also observed to depend on microstructure, and a threshold of MMP utility was identified. Our results suggest that fiber topography guides protrusions and thereby MMP activity and motility.

Collagen Matrix Density Drives the Metabolic Shift in Breast Cancer Cells.

PubMed

Morris, Brett A; Burkel, Brian; Ponik, Suzanne M; Fan, Jing; Condeelis, John S; Aguirre-Ghiso, Julio A; Castracane, James; Denu, John M; Keely, Patricia J

2016-11-01

Increased breast density attributed to collagen I deposition is associated with a 4-6 fold increased risk of developing breast cancer. Here, we assessed cellular metabolic reprogramming of mammary carcinoma cells in response to increased collagen matrix density using an in vitro 3D model. Our initial observations demonstrated changes in functional metabolism in both normal mammary epithelial cells and mammary carcinoma cells in response to changes in matrix density. Further, mammary carcinoma cells grown in high density collagen matrices displayed decreased oxygen consumption and glucose metabolism via the tricarboxylic acid (TCA) cycle compared to cells cultured in low density matrices. Despite decreased glucose entry into the TCA cycle, levels of glucose uptake, cell viability, and ROS were not different between high and low density matrices. Interestingly, under high density conditions the contribution of glutamine as a fuel source to drive the TCA cycle was significantly enhanced. These alterations in functional metabolism mirrored significant changes in the expression of metabolic genes involved in glycolysis, oxidative phosphorylation, and the serine synthesis pathway. This study highlights the broad importance of the collagen microenvironment to cellular expression profiles, and shows that changes in density of the collagen microenvironment can modulate metabolic shifts of cancer cells. Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.

Inelastic scattering of neutron-rich Ni and Zn isotopes off a proton target

NASA Astrophysics Data System (ADS)

Cortés, M. L.; Doornenbal, P.; Dupuis, M.; Lenzi, S. M.; Nowacki, F.; Obertelli, A.; Péru, S.; Pietralla, N.; Werner, V.; Wimmer, K.; Authelet, G.; Baba, H.; Calvet, D.; Château, F.; Corsi, A.; Delbart, A.; Gheller, J.-M.; Gillibert, A.; Isobe, T.; Lapoux, V.; Louchart, C.; Matsushita, M.; Momiyama, S.; Motobayashi, T.; Niikura, M.; Otsu, H.; Péron, C.; Peyaud, A.; Pollacco, E. C.; Roussé, J.-Y.; Sakurai, H.; Santamaria, C.; Sasano, M.; Shiga, Y.; Takeuchi, S.; Taniuchi, R.; Uesaka, T.; Wang, H.; Yoneda, K.; Browne, F.; Chung, L. X.; Dombradi, Zs.; Franchoo, S.; Giacoppo, F.; Gottardo, A.; Hadynska-Klek, K.; Korkulu, Z.; Koyama, S.; Kubota, Y.; Lee, J.; Lettmann, M.; Lozeva, R.; Matsui, K.; Miyazaki, T.; Nishimura, S.; Olivier, L.; Ota, S.; Patel, Z.; Sahin, E.; Shand, C. M.; Söderström, P.-A.; Stefan, I.; Steppenbeck, D.; Sumikama, T.; Suzuki, D.; Vajta, Zs.; Wu, J.; Xu, Z.

2018-04-01

Proton inelastic scattering of Ni,7472 and Zn,8076 ions at energies around 235 MeV/nucleon was performed at the Radioactive Isotope Beam Factory and studied using γ -ray spectroscopy. Angular integrated cross sections for direct inelastic scattering to the 21+ and 41+ states were measured. The Jeukenne-Lejeune-Mahaux folding model, extended beyond 200 MeV, was used together with neutron and proton densities stemming from quasiparticle random-phase approximation (QRPA) calculations to interpret the experimental cross sections and to infer neutron to proton matrix element ratios. In addition, coupled-channels calculations with a phenomenological potential were used to determine deformation lengths. For the Ni isotopes, correlations favor neutron excitations, thus conserving the Z =28 gap. A dominance of proton excitation, on the other hand, is observed in the Zn isotopes, pointing to the conservation of the N =50 gap approaching 78Ni. These results are in agreement with QRPA and large-scale shell-model calculations.

Cross Sections for Electron Impact Excitation of Astrophysically Abundant Atoms and Ions

NASA Technical Reports Server (NTRS)

Tayal, S. S.

2006-01-01

Electron collisional excitation rates and transition probabilities are important for computing electron temperatures and densities, ionization equilibria, and for deriving elemental abundances from emission lines formed in the collisional and photoionized astrophysical plasmas. Accurate representation of target wave functions that properly account for the important correlation and relaxation effects and inclusion of coupling effects including coupling to the continuum are essential components of a reliable collision calculation. Non-orthogonal orbitals technique in multiconfiguration Hartree-Fock approach is used to calculate oscillator strengths and transition probabilities. The effect of coupling to the continuum spectrum is included through the use of pseudostates which are chosen to account for most of the dipole polarizabilities of target states. The B-spline basis is used in the R-matrix approach to calculate electron excitation collision strengths and rates. Results for oscillator strengths and electron excitation collision strengths for transitions in N I, O I, O II, O IV, S X and Fe XIV have been produced

Axial-Current Matrix Elements in Light Nuclei from Lattice QCD

NASA Astrophysics Data System (ADS)

Savage, M.; Beane, S.; Chang, E.; Davoudi, Z.; Detmold, W.; Orginos, K.; Shanahan, P.; Tiburzi, B.; Wagman, M.; Winter, F.; Nplqcd Collaboration

I present results from the first lattice QCD calculations of axial-current matrix elements in light nuclei, performed by the NPLQCD collaboration. Precision calculations of these matrix elements, and the subsequent extraction of multi-nucleon axial-current operators, are essential in refining theoretical predictions of the proton-proton fusion cross section, neutrino-nucleus cross sections and $\\beta\\beta$-decay rates of nuclei. In addition, they are expected to shed light on the phenomenological quenching of $g_A$ that is required in nuclear many-body calculations.

Landscape attributes as drivers of the geographical variation in density of Sapajus nigritus Kerr, 1792, a primate endemic to the Atlantic Forest

NASA Astrophysics Data System (ADS)

Hendges, Carla D.; Melo, Geruza L.; Gonçalves, Alberto S.; Cerezer, Felipe O.; Cáceres, Nilton C.

2017-10-01

Neotropical primates are among the most well studied forest mammals concerning their population densities. However, few studies have evaluated the factors that influence the spatial variation in the population density of primates, which limits the possibility of inferences towards this animal group, especially at the landscape-level. Here, we compiled density data of Sapajus nigritus from 21 forest patches of the Brazilian Atlantic Forest. We tested the effects of climatic variables (temperature, precipitation), landscape attributes (number of patches, mean inter-patch isolation distance, matrix modification index) and patch size on the population density using linear models and the Akaike information criterion. Our findings showed that the density of S. nigritus is influenced by landscape attributes, particularly by fragmentation and matrix modification. Overall, moderately fragmented landscapes and those surrounded by matrices with intermediate indexes of temporal modification (i.e., crop plantations, forestry) are related to high densities of this species. These results support the assumptions that ecologically flexible species respond positively to forest fragmentation. However, the non-linear relationship between S. nigritus density and number of patches suggests that even the species that are most tolerant to forest cover changes seem to respond positively only at an intermediate level of habitat fragmentation, being dependent of both a moderate degree of forest cover and a high quality matrix. The results we found here can be a common response to fragmentation for those forest dweller species that are able to use the matrix as complementary foraging sites.

Photoinduced dynamics to photoluminescence in Ln3+ (Ln = Ce, Pr) doped β-NaYF4 nanocrystals computed in basis of non-collinear spin DFT with spin-orbit coupling

NASA Astrophysics Data System (ADS)

Han, Yulun; Vogel, Dayton J.; Inerbaev, Talgat M.; May, P. Stanley; Berry, Mary T.; Kilin, Dmitri S.

2018-03-01

In this work, non-collinear spin DFT + U approaches with spin-orbit coupling (SOC) are applied to Ln3+ doped β-NaYF4 (Ln = Ce, Pr) nanocrystals in Vienna ab initio Simulation Package taking into account unpaired spin configurations using the Perdew-Burke-Ernzerhof functional in a plane wave basis set. The calculated absorption spectra from non-collinear spin DFT + U approaches are compared with that from spin-polarised DFT + U approaches. The spectral difference indicates the importance of spin-flip transitions of Ln3+ ions. Suite of codes for nonadiabatic dynamics has been developed for 2-component spinor orbitals. On-the-fly nonadiabatic coupling calculations provide transition probabilities facilitated by nuclear motion. Relaxation rates of electrons and holes are calculated using Redfield theory in the reduced density matrix formalism cast in the basis of non-collinear spin DFT + U with SOC. The emission spectra are calculated using the time-integrated method along the excited state trajectories based on nonadiabatic couplings.

Approximate solution of the mode-mode coupling integral: Application to cytosine and its deuterated derivative.

PubMed

Rasheed, Tabish; Ahmad, Shabbir

2010-10-01

Ab initio Hartree-Fock (HF), density functional theory (DFT) and second-order Møller-Plesset (MP2) methods were used to perform harmonic and anharmonic calculations for the biomolecule cytosine and its deuterated derivative. The anharmonic vibrational spectra were computed using the vibrational self-consistent field (VSCF) and correlation-corrected vibrational self-consistent field (CC-VSCF) methods. Calculated anharmonic frequencies have been compared with the argon matrix spectra reported in literature. The results were analyzed with focus on the properties of anharmonic couplings between pair of modes. A simple and easy to use formula for calculation of mode-mode coupling magnitudes has been derived. The key element in present approach is the approximation that only interactions between pairs of normal modes have been taken into account, while interactions of triples or more are neglected. FTIR and Raman spectra of solid state cytosine have been recorded in the regions 400-4000 cm(-1) and 60-4000 cm(-1), respectively. Vibrational analysis and assignments are based on calculated potential energy distribution (PED) values. Copyright 2010 Elsevier B.V. All rights reserved.

Blue and red shifted temperature dependence of implicit phonon shifts in graphene

NASA Astrophysics Data System (ADS)

Mann, Sarita; Jindal, V. K.

2017-07-01

We have calculated the implicit shift for various modes of frequency in a pure graphene sheet. Thermal expansion and Grüneisen parameter which are required for implicit shift calculation have already been studied and reported. For this calculation, phonon frequencies are obtained using force constants derived from dynamical matrix calculated using VASP code where the density functional perturbation theory (DFPT) is used in interface with phonopy software. The implicit phonon shift shows an unusual behavior as compared to the bulk materials. The frequency shift is large negative (red shift) for ZA and ZO modes and the value of negative shift increases with increase in temperature. On the other hand, blue shift arises for all other longitudinal and transverse modes with a similar trend of increase with increase in temperature. The q dependence of phonon shifts has also been studied. Such simultaneous red and blue shifts in transverse or out plane modes and surface modes, respectively leads to speculation of surface softening in out of plane direction in preference to surface melting.

Design and analysis of InN - In0.25Ga0.75N single quantum well laser for short distance communication wavelength

NASA Astrophysics Data System (ADS)

Polash, Md. Mobarak Hossain; Alam, M. Shah; Biswas, Saumya

2018-03-01

A single quantum well semiconductor laser based on wurtzite-nitride is designed and analyzed for short distance communication wavelength (at around 1300 nm). The laser structure has 12 Å well layer of InN, 15 Å barrier layer of In0.25Ga0.75N, and 54 Å separate confinement heterostructure layer of GaN. To calculate the electronic characteristics of the structure, a self-consistent method is used where Hamiltonian with effective mass approximation is solved for conduction band while six-bands Hamiltonian matrix with k · p formalism including the polarization effect, valence-band mixing effect, and strain effect is solved for valence band. The interband optical transition elements, optical gain, differential gain, radiative current density, spontaneous emission rate, and threshold characteristics have been calculated. The wave function overlap integral is found to be 45.93% for TE-polarized structure. Also, the spontaneous emission rate is found to be 6.57 × 1027 s - 1 cm - 3 eV - 1 at 1288.21 nm with the carrier density of 5 × 1019 cm - 3. Furthermore, the radiative current density and the radiative recombination rate are found to be 121.92 A cm - 2 and 6.35 × 1027 s - 1 cm - 3, respectively, while the TE-polarized optical gain of the structure is 3872.1 cm - 1 at 1301.7 nm.

Metrics of cellular and vascular infiltration of human acellular dermal matrix in ventral hernia repairs.

PubMed

Campbell, Kristin Turza; Burns, Nadja K; Ensor, Joe; Butler, Charles E

2012-04-01

Human acellular dermal matrix is used for ventral hernia repair, as it resists infection and remodels by means of surrounding tissue. However, the tissue source and impact of basement membrane on cell and vessel infiltration have not been determined. The authors hypothesized that musculofascia would be the primary tissue source of cells and vessels infiltrating into human acellular dermal matrix and that the basement membrane would inhibit infiltration. Fifty-six guinea pigs underwent inlay human acellular dermal matrix ventral hernia repair with the basement membrane oriented toward or away from the peritoneum. At postoperative weeks 1, 2, or 4, repair sites were completely excised. Histologic and immunohistochemical analyses were performed to quantify cell and vessel density within repair-site zones, including interface (lateral, beneath musculofascia) and center (beneath subcutaneous fat) zones. Cell and vessel quantities were compared as functions of zone, basement membrane orientation, and time. Cellular and vascular infiltration increased over time universally. The interface demonstrated greater mean cell density than the center (weeks 1 and 2, p = 0.01 and p < 0.0001, respectively). Cell density was greater with the basement membrane oriented toward the peritoneum at week 4 (p = 0.02). The interface zone had greater mean vessel density than the center zone at week 4 (p < 0.0001). Orienting the basement membrane toward the peritoneum increased vessel density at week 4 (p = 0.0004). Cellular and vascular infiltration into human acellular dermal matrix for ventral hernia repairs was greater from musculofascia than from subcutaneous fat, and the basement membrane inhibited cellular and vascular infiltration. Human acellular dermal matrix should be placed adjacent to the best vascularizing tissue to improve fibrovascular incorporation.

Matrix density effects on the mechanical properties of SiC fiber-reinforced silicon nitride matrix properties

NASA Technical Reports Server (NTRS)

Bhatt, Ramakrishna T.; Kiser, Lames D.

1990-01-01

The room temperature mechanical properties were measured for SiC fiber reinforced reaction-bonded silicon nitride composites (SiC/RBSN) of different densities. The composites consisted of approx. 30 vol percent uniaxially aligned 142 micron diameter SiC fibers (Textron SCS-6) in a reaction-bonded Si3N4 matrix. The composite density was varied by changing the consolidation pressure during RBSN processing and by hot isostatically pressing the SiC/RBSN composites. Results indicate that as the consolidation pressure was increased from 27 to 138 MPa, the average pore size of the nitrided composites decreased from 0.04 to 0.02 microns and the composite density increased from 2.07 to 2.45 gm/cc. Nonetheless, these improvements resulted in only small increases in the first matrix cracking stress, primary elastic modulus, and ultimate tensile strength values of the composites. In contrast, HIP consolidation of SiC/RBSN resulted in a fully dense material whose first matrix cracking stress and elastic modulus were approx. 15 and 50 percent higher, respectively, and ultimate tensile strength values were approx. 40 percent lower than those for unHIPed SiC/RBSN composites. The modulus behavior for all specimens can be explained by simple rule-of-mixture theory. Also, the loss in ultimate strength for the HIPed composites appears to be related to a degradation in fiber strength at the HIP temperature. However, the density effect on matrix fracture strength was much less than would be expected based on typical monolithic Si3N4 behavior, suggesting that composite theory is indeed operating. Possible practical implications of these observations are discussed.

Isotropic matrix elements of the collision integral for the Boltzmann equation

NASA Astrophysics Data System (ADS)

Ender, I. A.; Bakaleinikov, L. A.; Flegontova, E. Yu.; Gerasimenko, A. B.

2017-09-01

We have proposed an algorithm for constructing matrix elements of the collision integral for the nonlinear Boltzmann equation isotropic in velocities. These matrix elements have been used to start the recurrent procedure for calculating matrix elements of the velocity-nonisotropic collision integral described in our previous publication. In addition, isotropic matrix elements are of independent interest for calculating isotropic relaxation in a number of physical kinetics problems. It has been shown that the coefficients of expansion of isotropic matrix elements in Ω integrals are connected by the recurrent relations that make it possible to construct the procedure of their sequential determination.

Increased extracellular matrix density decreases MCF10A breast cell acinus formation in 3D culture conditions.

PubMed

Lance, Amanda; Yang, Chih-Chao; Swamydas, Muthulekha; Dean, Delphine; Deitch, Sandy; Burg, Karen J L; Dréau, Didier

2016-01-01

The extracellular matrix (ECM) contributes to the generation and dynamic of normal breast tissue, in particular to the generation of polarized acinar and ductal structures. In vitro 3D culture conditions, including variations in the composition of the ECM, have been shown to directly influence the formation and organization of acinus-like and duct-like structures. Furthermore, the density of the ECM appears to also play a role in the normal mammary tissue and tumour formation. Here we show that the density of the ECM directly influences the number, organization and function of breast acini. Briefly, non-malignant human breast MCF10A cells were incubated in increasing densities of a Matrigel®-collagen I matrix. Elastic moduli near and distant to the acinus structures were measured by atomic force microscopy, and the number of acinus structures was determined. Immunochemistry was used to investigate the expression levels of E-cadherin, laminin, matrix metalloproteinase-14 and ß-casein in MCF10A cells. The modulus of the ECM was significantly increased near the acinus structures and the number of acinus structures decreased with the increase in Matrigel-collagen I density. As evaluated by the expression of laminin, the organization of the acinus structures present was altered as the density of the ECM increased. Increases in both E-cadherin and MMP14 expression by MCF10A cells as ECM density increased were also observed. In contrast, MCF10A cells expressed lower ß-casein levels as the ECM density increased. Taken together, these observations highlight the key role of ECM density in modulating the number, organization and function of breast acini. Copyright © 2013 John Wiley & Sons, Ltd.

Design of exceptionally strong and conductive Cu alloys beyond the conventional speculation via the interfacial energy-controlled dispersion of γ-Al2O3 nanoparticles

PubMed Central

Zeon Han, Seung; Kim, Kwang Ho; Kang, Joonhee; Joh, Hongrae; Kim, Sang Min; Ahn, Jee Hyuk; Lee, Jehyun; Lim, Sung Hwan; Han, Byungchan

2015-01-01

The development of Cu-based alloys with high-mechanical properties (strength, ductility) and electrical conductivity plays a key role over a wide range of industrial applications. Successful design of the materials, however, has been rare due to the improvement of mutually exclusive properties as conventionally speculated. In this paper, we demonstrate that these contradictory material properties can be improved simultaneously if the interfacial energies of heterogeneous interfaces are carefully controlled. We uniformly disperse γ-Al2O3 nanoparticles over Cu matrix, and then we controlled atomic level morphology of the interface γ-Al2O3//Cu by adding Ti solutes. It is shown that the Ti dramatically drives the interfacial phase transformation from very irregular to homogeneous spherical morphologies resulting in substantial enhancement of the mechanical property of Cu matrix. Furthermore, the Ti removes impurities (O and Al) in the Cu matrix by forming oxides leading to recovery of the electrical conductivity of pure Cu. We validate experimental results using TEM and EDX combined with first-principles density functional theory (DFT) calculations, which all consistently poise that our materials are suitable for industrial applications. PMID:26616045

Design of exceptionally strong and conductive Cu alloys beyond the conventional speculation via the interfacial energy-controlled dispersion of γ-Al2O3 nanoparticles.

PubMed

Han, Seung Zeon; Kim, Kwang Ho; Kang, Joonhee; Joh, Hongrae; Kim, Sang Min; Ahn, Jee Hyuk; Lee, Jehyun; Lim, Sung Hwan; Han, Byungchan

2015-11-30

The development of Cu-based alloys with high-mechanical properties (strength, ductility) and electrical conductivity plays a key role over a wide range of industrial applications. Successful design of the materials, however, has been rare due to the improvement of mutually exclusive properties as conventionally speculated. In this paper, we demonstrate that these contradictory material properties can be improved simultaneously if the interfacial energies of heterogeneous interfaces are carefully controlled. We uniformly disperse γ-Al2O3 nanoparticles over Cu matrix, and then we controlled atomic level morphology of the interface γ-Al2O3//Cu by adding Ti solutes. It is shown that the Ti dramatically drives the interfacial phase transformation from very irregular to homogeneous spherical morphologies resulting in substantial enhancement of the mechanical property of Cu matrix. Furthermore, the Ti removes impurities (O and Al) in the Cu matrix by forming oxides leading to recovery of the electrical conductivity of pure Cu. We validate experimental results using TEM and EDX combined with first-principles density functional theory (DFT) calculations, which all consistently poise that our materials are suitable for industrial applications.

Highly ordered molecular rotor matrix on a nanopatterned template: titanyl phthalocyanine molecules on FeO/Pt(111).

PubMed

Lu, Shuangzan; Huang, Min; Qin, Zhihui; Yu, Yinghui; Guo, Qinmin; Cao, Gengyu

2018-08-03

Molecular rotors, motors and gears play important roles in artificial molecular machines, in which rotor and motor matrices are highly desirable for large-scale bottom-up fabrication of molecular machines. Here we demonstrate the fabrication of a highly ordered molecular rotor matrix by depositing nonplanar dipolar titanyl phthalocyanine (TiOPc, C 32 H 16 N 8 OTi) molecules on a Moiré patterned dipolar FeO/Pt(111) substrate. TiOPc molecules with O atoms pointing outwards from the substrate (upward) or towards the substrate (downward) are alternatively adsorbed on the fcc sites by strong lateral confinement. The adsorbed molecules, i.e. two kinds of molecular rotors, show different scanning tunneling microscopy images, thermal stabilities and rotational characteristics. Density functional theory calculations clarify that TiOPc molecules anchoring upwards with high adsorption energies correspond to low-rotational-rate rotors, while those anchoring downwards with low adsorption energies correspond to high-rotational-rate rotors. A robust rotor matrix fully occupied by low-rate rotors is fabricated by depositing molecules on the substrate at elevated temperature. Such a paradigm opens up a promising route to fabricate functional molecular rotor matrices, driven motor matrices and even gear groups on solid substrates.

Infrared spectroscopic probing of dimethylamine clusters in an Ar matrix.

PubMed

Li, Siyang; Kjaergaard, Henrik G; Du, Lin

2016-02-01

Amines have many atmospheric sources and their clusters play an important role in aerosol nucleation processes. Clusters of a typical amine, dimethylamine (DMA), of different sizes were measured with matrix isolation IR (infrared) and NIR (near infrared) spectroscopy. The NIR vibrations are more separated and therefore it is easier to distinguish different sizes of clusters in this region. The DMA clusters, up to DMA tetramer, have been optimized using density functional methods, and the geometries, binding energies and thermodynamic properties of DMA clusters were obtained. The computed frequencies and intensities of NH-stretching vibrations in the DMA clusters were used to interpret the experimental spectra. We have identified the fundamental transitions of the bonded NH-stretching vibration and the first overtone transitions of the bonded and free NH-stretching vibration in the DMA clusters. Based on the changes in vibrational intensities during the annealing processes, the growth of clusters was clearly observed. The results of annealing processes indicate that DMA molecules tend to form larger clusters with lower energies under matrix temperatures, which is also supported by the calculated reaction energies of cluster formation. Copyright © 2015. Published by Elsevier B.V.

Effect of particle morphology of Ni on the mechanical behavior of AZ91E-Ni coated nano Al2O3 composites

NASA Astrophysics Data System (ADS)

Sameer Kumar, D.; Suman, K. N. S.; Poddar, Palash

2017-06-01

The properties of any composite always depend on the bonding between the matrix and reinforcement phases. One way of improving the wettability of reinforcement in a matrix is to apply a layer of coating on reinforcing particles. The present study aims at developing Ni coating on nano Al2O3 ceramic particles and dispersing them in AZ91E magnesium matrix material. The electroless plating method has been employed to coat the particles and semi solid stir casting technique was adopted to prepare the composites. Several weight fractions of dispersed phase are considered to analyze the behavior of the fabricated composites. Field emission scanning electron microscopy (FESEM) and x-ray diffraction analysis has been carried out to investigate the distribution of particles and phase characteristics of the proposed material. The physical and mechanical behavior of the material was examined through density measurements, hardness, elastic modulus, ductility and tensile strength calculations. The metal coating on reinforcement aids to promote metal-metal bonding interface reactions which result in improved properties of the composite. Tensile fractography was carried out under FESEM and presented.

Irradiated microstructure of U-10Mo monolithic fuel plate at very high fission density

NASA Astrophysics Data System (ADS)

Gan, J.; Miller, B. D.; Keiser, D. D.; Jue, J. F.; Madden, J. W.; Robinson, A. B.; Ozaltun, H.; Moore, G.; Meyer, M. K.

2017-08-01

Monolithic U-10Mo alloy fuel plates with Al-6061 cladding are being developed for use in research and test reactors as low enrichment fuel (<20% U-235 enrichment) as a result of its high uranium loading capacity compared to that of U-7Mo dispersion fuel. These fuel plates contain a Zr diffusion barrier between the U-10Mo fuel and Al-6061 cladding that suppresses the interaction between the U-Mo fuel foil and Al alloy cladding that is known to be problematic under irradiation. Different methods have been employed to fabricate monolithic fuel plates, including hot-rolling with no cold-rolling. L1P09T is a hot-rolled fuel plate irradiated to high fission density in the RERTR-9B experiment. This paper discusses the TEM characterization results for this U-10Mo/Zr/Al6061 monolithic fuel plate (∼59% U-235 enrichment) irradiated in Advanced Test Reactor at Idaho National Laboratory with an unprecedented high local fission density of 9.8E+21 fissions/cm3. The calculated fuel foil centerline temperature at the beginning of life and the end of life is 141 and 194 °C, respectively. TEM lamellas were prepared using focus ion beam lift-out technique. The estimated U-Mo fuel swelling, based on the fuel foil thickness change from SEM, is approximately 76%. Large bubbles (>1 μm) are distributed evenly in U-Mo and interlink of these bubbles is evident. The average size of subdivided grains at this fission density appears similar to that at 5.2E+21 fissions/cm3. The measured average Mo and Zr content in the fuel matrix is ∼30 at% and ∼7 at%, respectively, in general agreement with the calculated Mo and Zr from fission density.

Theoretical study of depth profiling with gamma- and X-ray spectrometry based on measurements of intensity ratios

NASA Astrophysics Data System (ADS)

Bártová, H.; Trojek, T.; Johnová, K.

2017-11-01

This article describes the method for the estimation of depth distribution of radionuclides in a material with gamma-ray spectrometry, and the identification of a layered structure of a material with X-ray fluorescence analysis. This method is based on the measurement of a ratio of two gamma or X-ray lines of a radionuclide or a chemical element, respectively. Its principle consists in different attenuation coefficient for these two lines in a measured material. The main aim of this investigation was to show how the detected ratio of these two lines depends on depth distribution of an analyte and mainly how this ratio depends on density and chemical composition of measured materials. Several different calculation arrangements were made and a lot of Monte Carlo simulation with the code MCNP - Monte Carlo N-Particle (Briesmeister, 2000) was performed to answer these questions. For X-ray spectrometry, the calculated Kα/Kβ diagrams were found to be almost independent upon matrix density and composition. Thanks to this phenomenon it would be possible to draw only one Kα/Kβ diagram for an element whose depth distribution is examined.

Calculating Path-Dependent Travel Time Prediction Variance and Covariance fro a Global Tomographic P-Velocity Model

NASA Astrophysics Data System (ADS)

Ballard, S.; Hipp, J. R.; Encarnacao, A.; Young, C. J.; Begnaud, M. L.; Phillips, W. S.

2012-12-01

Seismic event locations can be made more accurate and precise by computing predictions of seismic travel time through high fidelity 3D models of the wave speed in the Earth's interior. Given the variable data quality and uneven data sampling associated with this type of model, it is essential that there be a means to calculate high-quality estimates of the path-dependent variance and covariance associated with the predicted travel times of ray paths through the model. In this paper, we describe a methodology for accomplishing this by exploiting the full model covariance matrix and show examples of path-dependent travel time prediction uncertainty computed from SALSA3D, our global, seamless 3D tomographic P-velocity model. Typical global 3D models have on the order of 1/2 million nodes, so the challenge in calculating the covariance matrix is formidable: 0.9 TB storage for 1/2 of a symmetric matrix, necessitating an Out-Of-Core (OOC) blocked matrix solution technique. With our approach the tomography matrix (G which includes Tikhonov regularization terms) is multiplied by its transpose (GTG) and written in a blocked sub-matrix fashion. We employ a distributed parallel solution paradigm that solves for (GTG)-1 by assigning blocks to individual processing nodes for matrix decomposition update and scaling operations. We first find the Cholesky decomposition of GTG which is subsequently inverted. Next, we employ OOC matrix multiplication methods to calculate the model covariance matrix from (GTG)-1 and an assumed data covariance matrix. Given the model covariance matrix, we solve for the travel-time covariance associated with arbitrary ray-paths by summing the model covariance along both ray paths. Setting the paths equal and taking the square root yields the travel prediction uncertainty for the single path.

Lithium-coated polymeric matrix as a minimum volume-change and dendrite-free lithium metal anode

PubMed Central

Liu, Yayuan; Lin, Dingchang; Liang, Zheng; Zhao, Jie; Yan, Kai; Cui, Yi

2016-01-01

Lithium metal is the ideal anode for the next generation of high-energy-density batteries. Nevertheless, dendrite growth, side reactions and infinite relative volume change have prevented it from practical applications. Here, we demonstrate a promising metallic lithium anode design by infusing molten lithium into a polymeric matrix. The electrospun polyimide employed is stable against highly reactive molten lithium and, via a conformal layer of zinc oxide coating to render the surface lithiophilic, molten lithium can be drawn into the matrix, affording a nano-porous lithium electrode. Importantly, the polymeric backbone enables uniform lithium stripping/plating, which successfully confines lithium within the matrix, realizing minimum volume change and effective dendrite suppression. The porous electrode reduces the effective current density; thus, flat voltage profiles and stable cycling of more than 100 cycles is achieved even at a high current density of 5 mA cm−2 in both carbonate and ether electrolyte. The advantages of the porous, polymeric matrix provide important insights into the design principles of lithium metal anodes. PMID:26987481

Lithium-coated polymeric matrix as a minimum volume-change and dendrite-free lithium metal anode

DOE PAGES

Liu, Yayuan; Lin, Dingchang; Liang, Zheng; ...

2016-03-18

Lithium metal is the ideal anode for the next generation of high-energy-density batteries. Nevertheless, dendrite growth, side reactions and infinite relative volume change have prevented it from practical applications. Here, we demonstrate a promising metallic lithium anode design by infusing molten lithium into a polymeric matrix. The electrospun polyimide employed is stable against highly reactive molten lithium and, via a conformal layer of zinc oxide coating to render the surface lithiophilic, molten lithium can be drawn into the matrix, affording a nano-porous lithium electrode. Importantly, the polymeric backbone enables uniform lithium stripping/plating, which successfully confines lithium within the matrix, realizingmore » minimum volume change and effective dendrite suppression. The porous electrode reduces the effective current density; thus, flat voltage profiles and stable cycling of more than 100 cycles is achieved even at a high current density of 5 mA cm -2 in both carbonate and ether electrolyte. Furthermore, the advantages of the porous, polymeric matrix provide important insights into the design principles of lithium metal anodes.« less

Lithium-coated polymeric matrix as a minimum volume-change and dendrite-free lithium metal anode

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Yayuan; Lin, Dingchang; Liang, Zheng

Lithium metal is the ideal anode for the next generation of high-energy-density batteries. Nevertheless, dendrite growth, side reactions and infinite relative volume change have prevented it from practical applications. Here, we demonstrate a promising metallic lithium anode design by infusing molten lithium into a polymeric matrix. The electrospun polyimide employed is stable against highly reactive molten lithium and, via a conformal layer of zinc oxide coating to render the surface lithiophilic, molten lithium can be drawn into the matrix, affording a nano-porous lithium electrode. Importantly, the polymeric backbone enables uniform lithium stripping/plating, which successfully confines lithium within the matrix, realizingmore » minimum volume change and effective dendrite suppression. The porous electrode reduces the effective current density; thus, flat voltage profiles and stable cycling of more than 100 cycles is achieved even at a high current density of 5 mA cm -2 in both carbonate and ether electrolyte. Furthermore, the advantages of the porous, polymeric matrix provide important insights into the design principles of lithium metal anodes.« less

Molecular mechanics of mineralized collagen fibrils in bone

PubMed Central

Nair, Arun K.; Gautieri, Alfonso; Chang, Shu-Wei; Buehler, Markus J.

2013-01-01

Bone is a natural composite of collagen protein and the mineral hydroxyapatite. The structure of bone is known to be important to its load-bearing characteristics, but relatively little is known about this structure or the mechanism that govern deformation at the molecular scale. Here we perform full-atomistic calculations of the three-dimensional molecular structure of a mineralized collagen protein matrix to try to better understand its mechanical characteristics under tensile loading at various mineral densities. We find that as the mineral density increases, the tensile modulus of the network increases monotonically and well beyond that of pure collagen fibrils. Our results suggest that the mineral crystals within this network bears up to four times the stress of the collagen fibrils, whereas the collagen is predominantly responsible for the material’s deformation response. These findings reveal the mechanism by which bone is able to achieve superior energy dissipation and fracture resistance characteristics beyond its individual constituents. PMID:23591891

Surface-peaked medium effects in the interaction of nucleons with finite nuclei

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aguayo, F. J.; Arellano, H. F.

We investigate the asymptotic separation of the optical model potential for nucleon-nucleus scattering in momentum space, where the potential is split into a medium-independent term and another depending exclusively on the gradient of the density-dependent g matrix. This decomposition confines the medium sensitivity of the nucleon-nucleus coupling to the surface of the nucleus. We examine this feature in the context of proton-nucleus scattering at beam energies between 30 and 100 MeV and find that the pn coupling accounts for most of this sensitivity. Additionally, based on this general structure of the optical potential we are able to treat both, themore » medium dependence of the effective interaction and the full mixed density as described by single-particle shell models. The calculated scattering observables agree within 10% with those obtained by Arellano, Brieva, and Love in their momentum-space g-folding approach.« less

Local Descriptors of Dynamic and Nondynamic Correlation.

PubMed

Ramos-Cordoba, Eloy; Matito, Eduard

2017-06-13

Quantitatively accurate electronic structure calculations rely on the proper description of electron correlation. A judicious choice of the approximate quantum chemistry method depends upon the importance of dynamic and nondynamic correlation, which is usually assesed by scalar measures. Existing measures of electron correlation do not consider separately the regions of the Cartesian space where dynamic or nondynamic correlation are most important. We introduce real-space descriptors of dynamic and nondynamic electron correlation that admit orbital decomposition. Integration of the local descriptors yields global numbers that can be used to quantify dynamic and nondynamic correlation. Illustrative examples over different chemical systems with varying electron correlation regimes are used to demonstrate the capabilities of the local descriptors. Since the expressions only require orbitals and occupation numbers, they can be readily applied in the context of local correlation methods, hybrid methods, density matrix functional theory, and fractional-occupancy density functional theory.

Asteroid orbital error analysis: Theory and application

NASA Technical Reports Server (NTRS)

Muinonen, K.; Bowell, Edward

1992-01-01

We present a rigorous Bayesian theory for asteroid orbital error estimation in which the probability density of the orbital elements is derived from the noise statistics of the observations. For Gaussian noise in a linearized approximation the probability density is also Gaussian, and the errors of the orbital elements at a given epoch are fully described by the covariance matrix. The law of error propagation can then be applied to calculate past and future positional uncertainty ellipsoids (Cappellari et al. 1976, Yeomans et al. 1987, Whipple et al. 1991). To our knowledge, this is the first time a Bayesian approach has been formulated for orbital element estimation. In contrast to the classical Fisherian school of statistics, the Bayesian school allows a priori information to be formally present in the final estimation. However, Bayesian estimation does give the same results as Fisherian estimation when no priori information is assumed (Lehtinen 1988, and reference therein).

The analysis of tensegrity structures for the design of a morphing wing

NASA Astrophysics Data System (ADS)

Moored, Keith W., III; Bart-Smith, Hilary

2005-05-01

Tensegrity structures have become of engineering interest in recent years, but very few have found practical use. This lack of integration is attributed to the lack of a well formulated design procedure. In this paper, a preliminary procedure is presented for developing morphing tensegrity structures that include actuating elements. To do this, the virtual work method has been modified to allow for individual actuation of struts and cables. A generalized connectivity matrix for a cantilever beam constructed from either a single 4-strut cell or multiple 4-strut cells has been developed. Global deflections resulting from actuation of specific elements have been calculated. Furthermore, the force density method is expanded to include a necessary upper bound condition such that a physically feasible structure can be designed. Finally, the importance of relative force density values on the overall shape of a structure comprising of multiple unit cells is discussed.

Simulation of superconducting tapes and coils with convex quadratic programming method

NASA Astrophysics Data System (ADS)

Zhang, Yan; Song, Yuntao; Wang, Lei; Liu, Xufeng

2015-08-01

Second-generation (2G) high-temperature superconducting coated conductors are playing an increasingly important role in power applications due to their large current density under high magnetic fields. In this paper, we conclude and explore the ability and possible potential of J formulation from the mathematical modeling point of view. An equivalent matrix form of J formulation has been presented and a relation between electromagnetic quantities and Karush-Kuhn-Tucker (KKT) conditions in optimization theory has been discovered. The use of the latest formulae to calculate inductance in a coil system and the primal-dual interior-point method algorithm is a trial to make the process of modeling stylized and build a bridge to commercial optimization solvers. Two different dependences of the critical current density on the magnetic field have been used in order to make a comparison with those published papers.

Eigenvalue Attraction

NASA Astrophysics Data System (ADS)

Movassagh, Ramis

2016-02-01

We prove that the complex conjugate (c.c.) eigenvalues of a smoothly varying real matrix attract (Eq. 15). We offer a dynamical perspective on the motion and interaction of the eigenvalues in the complex plane, derive their governing equations and discuss applications. C.c. pairs closest to the real axis, or those that are ill-conditioned, attract most strongly and can collide to become exactly real. As an application we consider random perturbations of a fixed matrix M. If M is Normal, the total expected force on any eigenvalue is shown to be only the attraction of its c.c. (Eq. 24) and when M is circulant the strength of interaction can be related to the power spectrum of white noise. We extend this by calculating the expected force (Eq. 41) for real stochastic processes with zero-mean and independent intervals. To quantify the dominance of the c.c. attraction, we calculate the variance of other forces. We apply the results to the Hatano-Nelson model and provide other numerical illustrations. It is our hope that the simple dynamical perspective herein might help better understanding of the aggregation and low density of the eigenvalues of real random matrices on and near the real line respectively. In the appendix we provide a Matlab code for plotting the trajectories of the eigenvalues.

Communication: A difference density picture for the self-consistent field ansatz.

PubMed

Parrish, Robert M; Liu, Fang; Martínez, Todd J

2016-04-07

We formulate self-consistent field (SCF) theory in terms of an interaction picture where the working variable is the difference density matrix between the true system and a corresponding superposition of atomic densities. As the difference density matrix directly represents the electronic deformations inherent in chemical bonding, this "difference self-consistent field (dSCF)" picture provides a number of significant conceptual and computational advantages. We show that this allows for a stable and efficient dSCF iterative procedure with wholly single-precision Coulomb and exchange matrix builds. We also show that the dSCF iterative procedure can be performed with aggressive screening of the pair space. These approximations are tested and found to be accurate for systems with up to 1860 atoms and >10 000 basis functions, providing for immediate overall speedups of up to 70% in the heavily optimized TeraChem SCF implementation.

Communication: A difference density picture for the self-consistent field ansatz

NASA Astrophysics Data System (ADS)

Parrish, Robert M.; Liu, Fang; Martínez, Todd J.

2016-04-01

We formulate self-consistent field (SCF) theory in terms of an interaction picture where the working variable is the difference density matrix between the true system and a corresponding superposition of atomic densities. As the difference density matrix directly represents the electronic deformations inherent in chemical bonding, this "difference self-consistent field (dSCF)" picture provides a number of significant conceptual and computational advantages. We show that this allows for a stable and efficient dSCF iterative procedure with wholly single-precision Coulomb and exchange matrix builds. We also show that the dSCF iterative procedure can be performed with aggressive screening of the pair space. These approximations are tested and found to be accurate for systems with up to 1860 atoms and >10 000 basis functions, providing for immediate overall speedups of up to 70% in the heavily optimized TeraChem SCF implementation.

Simulation-aided constitutive law development - Assessment of low triaxiality void nucleation models via extended finite element method

NASA Astrophysics Data System (ADS)

Zhao, Jifeng; Kontsevoi, Oleg Y.; Xiong, Wei; Smith, Jacob

2017-05-01

In this work, a multi-scale computational framework has been established in order to investigate, refine and validate constitutive behaviors in the context of the Gurson-Tvergaard-Needleman (GTN) void mechanics model. The eXtended Finite Element Method (XFEM) has been implemented in order to (1) develop statistical volume elements (SVE) of a matrix material with subscale inclusions and (2) to simulate the multi-void nucleation process due to interface debonding between the matrix and particle phases. Our analyses strongly suggest that under low stress triaxiality the nucleation rate of the voids f˙ can be well described by a normal distribution function with respect to the matrix equivalent stress (σe), as opposed to that proposed (σbar + 1 / 3σkk) in the original form of the single void GTN model. The modified form of the multi-void nucleation model has been validated based on a series of numerical experiments with different loading conditions, material properties, particle shape/size and spatial distributions. The utilization of XFEM allows for an invariant finite element mesh to represent varying microstructures, which implies suitability for drastically reducing complexity in generating the finite element discretizations for large stochastic arrays of microstructure configurations. The modified form of the multi-void nucleation model is further applied to study high strength steels by incorporating first principles calculations. The necessity of using a phenomenological interface separation law has been fully eliminated and replaced by the physics-based cohesive relationship obtained from Density Functional Theory (DFT) calculations in order to provide an accurate macroscopic material response.

Orbital optimisation in the perfect pairing hierarchy: applications to full-valence calculations on linear polyacenes

NASA Astrophysics Data System (ADS)

Lehtola, Susi; Parkhill, John; Head-Gordon, Martin

2018-03-01

We describe the implementation of orbital optimisation for the models in the perfect pairing hierarchy. Orbital optimisation, which is generally necessary to obtain reliable results, is pursued at perfect pairing (PP) and perfect quadruples (PQ) levels of theory for applications on linear polyacenes, which are believed to exhibit strong correlation in the π space. While local minima and σ-π symmetry breaking solutions were found for PP orbitals, no such problems were encountered for PQ orbitals. The PQ orbitals are used for single-point calculations at PP, PQ and perfect hextuples (PH) levels of theory, both only in the π subspace, as well as in the full σπ valence space. It is numerically demonstrated that the inclusion of single excitations is necessary also when optimised orbitals are used. PH is found to yield good agreement with previously published density matrix renormalisation group data in the π space, capturing over 95% of the correlation energy. Full-valence calculations made possible by our novel, efficient code reveal that strong correlations are weaker when larger basis sets or active spaces are employed than in previous calculations. The largest full-valence PH calculations presented correspond to a (192e,192o) problem.

Petrophysical analysis of geophysical logs of the National Drilling Company-U.S. Geological Survey ground-water research project for Abu Dhabi Emirate, United Arab Emirates

USGS Publications Warehouse

Jorgensen, Donald G.; Petricola, Mario

1994-01-01

A program of borehole-geophysical logging was implemented to supply geologic and geohydrologic information for a regional ground-water investigation of Abu Dhabi Emirate. Analysis of geophysical logs was essential to provide information on geohydrologic properties because drill cuttings were not always adequate to define lithologic boundaries. The standard suite of logs obtained at most project test holes consisted of caliper, spontaneous potential, gamma ray, dual induction, microresistivity, compensated neutron, compensated density, and compensated sonic. Ophiolitic detritus from the nearby Oman Mountains has unusual petrophysical properties that complicated the interpretation of geophysical logs. The density of coarse ophiolitic detritus is typically greater than 3.0 grams per cubic centimeter, porosity values are large, often exceeding 45 percent, and the clay fraction included unusual clays, such as lizardite. Neither the spontaneous-potential log nor the natural gamma-ray log were useable clay indicators. Because intrinsic permeability is a function of clay content, additional research in determining clay content was critical. A research program of geophysical logging was conducted to determine the petrophysical properties of the shallow subsurface formations. The logging included spectral-gamma and thermal-decay-time logs. These logs, along with the standard geophysical logs, were correlated to mineralogy and whole-rock chemistry as determined from sidewall cores. Thus, interpretation of lithology and fluids was accomplished. Permeability and specific yield were calculated from geophysical-log data and correlated to results from an aquifer test. On the basis of results from the research logging, a method of lithologic and water-resistivity interpretation was developed for the test holes at which the standard suite of logs were obtained. In addition, a computer program was developed to assist in the analysis of log data. Geohydrologic properties were estimated, including volume of clay matrix, volume of matrix other than clay, density of matrix other than clay, density of matrix, intrinsic permeability, specific yield, and specific storage. Geophysical logs were used to (1) determine lithology, (2) correlate lithologic and permeable zones, (3) calibrate seismic reprocessing, (4) calibrate transient-electromagnetic surveys, and (5) calibrate uphole-survey interpretations. Logs were used at the drill site to (1) determine permeability zones, (2) determine dissolved-solids content, which is a function of water resistivity, and (3) design wells accordingly. Data and properties derived from logs were used to determine transmissivity and specific yield of aquifer materials.

Single-Sided Noinvasive Inspection of Multielement Sample Using Fan-Beam Multiplexed Compton Scatter Tomography

DTIC Science & Technology

2000-05-01

a vector , ρ "# represents the set of voxel densities sorted into a vector , and ( )A ρ $# "# represents a 8 mapping of the voxel densities to...density vector in equation (4) suggests that solving for ρ "# by direct inversion is not possible, calling for an iterative technique beginning with...the vector of measured spectra, and D is the diagonal matrix of the inverse of the variances. The diagonal matrix provides weighting terms, which

Matrix elements of explicitly correlated Gaussian basis functions with arbitrary angular momentum

DOE Office of Scientific and Technical Information (OSTI.GOV)

Joyce, Tennesse; Varga, Kálmán

2016-05-14

A new algorithm for calculating the Hamiltonian matrix elements with all-electron explicitly correlated Gaussian functions for quantum-mechanical calculations of atoms with arbitrary angular momentum is presented. The calculations are checked on several excited states of three and four electron systems. The presented formalism can be used as unified framework for high accuracy calculations of properties of small atoms and molecules.

Entanglement entropy in a one-dimensional disordered interacting system: the role of localization.

PubMed

Berkovits, Richard

2012-04-27

The properties of the entanglement entropy (EE) in one-dimensional disordered interacting systems are studied. Anderson localization leaves a clear signature on the average EE, as it saturates on the length scale exceeding the localization length. This is verified by numerically calculating the EE for an ensemble of disordered realizations using the density matrix renormalization group method. A heuristic expression describing the dependence of the EE on the localization length, which takes into account finite-size effects, is proposed. This is used to extract the localization length as a function of the interaction strength. The localization length dependence on the interaction fits nicely with the expectations.

Light-matter interaction in doped microcavities

NASA Astrophysics Data System (ADS)

Averkiev, N. S.; Glazov, M. M.

2007-07-01

We discuss theoretically the light-matter coupling in a microcavity containing a quantum well with a two-dimensional electron gas. The high density limit where the bound exciton states are absent is considered. The matrix element of an interband optical absorption demonstrates the Mahan singularity [Phys. Rev. B153, 882 (1967); 163, 612 (1967)] due to strong Coulomb effect between the electrons and a photocreated hole. We extend the nonlocal dielectric response theory to calculate the quantum well reflection and transmission coefficients as well as the microcavity transmission spectra. The new eigenmodes of the system are discussed. Their implications for the steady state and time-resolved spectroscopy experiments are analyzed.

Subbarrier absorption in a stationary superlattice

NASA Technical Reports Server (NTRS)

Arutyunyan, G. M.; Nerkararyan, K. V.

1984-01-01

The calculation of the interband absorption coefficient was carried out in the classical case, when the frequency of light was assumed to bind two miniband subbarrier states of different bands. The influence of two dimensional Mott excitons on this absorption was studied and a comparison was made with the experiment. All of these considerations were done taking into account the photon wave vector (the phase spatial heterogeneity). The basic traits of the energy spectra of superlattice semiconductors, their kinetic and optical properties, and possible means of electromagnetic wave intensification were examined. By the density matrix method, a theory of electrical and electromagnetic properties of superlattices was suggested.

Single-particle spectral functions in the normal phase of a strongly attractive Bose-Fermi mixture

NASA Astrophysics Data System (ADS)

Fratini, E.; Pieri, P.

2013-07-01

We calculate the single-particle spectral functions and quasiparticle dispersions for a Bose-Fermi mixture when the boson-fermion attraction is sufficiently strong to suppress completely the condensation of bosons at zero temperature. Within a T-matrix diagrammatic approach, we vary the boson-fermion attraction from the critical value where the boson condensate first disappears to the strongly attractive (molecular) regime and study the effect of both mass and density imbalance on the spectral weights and dispersions. An interesting spectrum of particle-hole excitations mixing two different Fermi surfaces is found. These unconventional excitations could be produced and explored experimentally with radio-frequency spectroscopy.

Microscopic nonlinear relativistic quantum theory of absorption of powerful x-ray radiation in plasma.

PubMed

Avetissian, H K; Ghazaryan, A G; Matevosyan, H H; Mkrtchian, G F

2015-10-01

The microscopic quantum theory of plasma nonlinear interaction with the coherent shortwave electromagnetic radiation of arbitrary intensity is developed. The Liouville-von Neumann equation for the density matrix is solved analytically considering a wave field exactly and a scattering potential of plasma ions as a perturbation. With the help of this solution we calculate the nonlinear inverse-bremsstrahlung absorption rate for a grand canonical ensemble of electrons. The latter is studied in Maxwellian, as well as in degenerate quantum plasma for x-ray lasers at superhigh intensities and it is shown that one can achieve the efficient absorption coefficient in these cases.

Phase Fluctuations and a Negative U Hubbard Model: Single-Particle and Thermodyanic Properties in a Conserving Approximation

NASA Astrophysics Data System (ADS)

Serene, J. W.; Deisz, J. J.; Hess, D. W.

1997-03-01

Calculations performed in the fluctuation exchange approximation for the single-band 2D Hubbard model on a cylinder and threaded by a flux, show the appearance of a finite superfluid density below T ~ 0.13t, for U=-4t and at three-eighths filling.(J.J. Deisz, D.W. Hess, Bull. Am. Phys. Soc. 41, 239 (1996); J.J. Deisz, D.W. Hess, and J.W. Serene, in preparation.) We show the evolution, with decreasing temperature, of the single-particle spectral function, the self-energy, the particle-particle T-matrix, and thermodynamic properties as the superfluid state is approached and entered.

Ultrathin multi-slit metamaterial as excellent sound absorber: Influence of micro-structure

NASA Astrophysics Data System (ADS)

Ren, S. W.; Meng, H.; Xin, F. X.; Lu, T. J.

2016-01-01

An ultrathin (subwavelength) hierarchy multi-slit metamaterial with simultaneous negative effective density and negative compressibility is proposed to absorb sound over a wide frequency range. Different from conventional acoustic metamaterials having only negative real parts of acoustic parameters, the imaginary parts of effective density and compressibility are both negative for the proposed metamaterial, which result in superior viscous and thermal dissipation of sound energy. By combining the slit theory of sound absorption with the double porosity theory for porous media, a theoretical model is developed to investigate the sound absorption performance of the metamaterial. To verify the model, a finite element model is established to calculate the effective density, compressibility, and sound absorption of the metamaterial. It is theoretically and numerically confirmed that, upon introducing micro-slits into the meso-slits matrix, the multi-slit metamaterial possesses indeed negative imaginary parts of effective density and compressibility. The influence of micro-slits on the acoustical performance of the metamaterial is analyzed in the context of its specific surface area and static flow resistivity. This work shows great potential of multi-slit metamaterials in noise control applications that require both small volume and small weight of sound-absorbing materials.

Exploring Hill Ciphers with Graphing Calculators.

ERIC Educational Resources Information Center

St. John, Dennis

1998-01-01

Explains how to code and decode messages using Hill ciphers which combine matrix multiplication and modular arithmetic. Discusses how a graphing calculator can facilitate the matrix and modular arithmetic used in the coding and decoding procedures. (ASK)

Fundamental study of hydrogen-attachment-induced peptide fragmentation occurring in the gas phase and during the matrix-assisted laser desorption/ionization process.

PubMed

Asakawa, Daiki; Takahashi, Hidenori; Iwamoto, Shinichi; Tanaka, Koichi

2018-05-09

Mass spectrometry with hydrogen-radical-mediated fragmentation techniques has been used for the sequencing of proteins/peptides. The two methods, matrix-assisted laser desorption/ionization in-source decay (MALDI-ISD) and hydrogen attachment/abstraction dissociation (HAD) are known as hydrogen-radical-mediated fragmentation techniques. MALDI-ISD occurs during laser induced desorption processes, whereas HAD utilizes the association of hydrogen with peptide ions in the gas phase. In this study, the general mechanisms of MALDI-ISD and HAD of peptides were investigated. We demonstrated the fragmentation of four model peptides and investigated the fragment formation pathways using density functional theory (DFT) calculations. The current experimental and computational joint study indicated that MALDI-ISD and HAD produce aminoketyl radical intermediates, which immediately undergo radical-induced cleavage at the N-Cα bond located on the C-terminal side of the radical site, leading to the c'/z˙ fragment pair. In the case of MALDI-ISD, the z˙ fragments undergo a subsequent reaction with the matrix to give z' and matrix adducts of the z fragments. In contrast, the c' and z˙ fragments react with hydrogen atoms during the HAD processes, and various fragment species, such as c˙, c', z˙ and z', were observed in the HAD-MS/MS mass spectra.

NON-GAUSSIANITIES IN THE LOCAL CURVATURE OF THE FIVE-YEAR WMAP DATA

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rudjord, Oeystein; Groeneboom, Nicolaas E.; Hansen, Frode K.

Using the five-year WMAP data, we re-investigate claims of non-Gaussianities and asymmetries detected in local curvature statistics of the one-year WMAP data. In Hansen et al., it was found that the northern ecliptic hemisphere was non-Gaussian at the {approx}1% level testing the densities of hill, lake, and saddle points based on the second derivatives of the cosmic microwave background temperature map. The five-year WMAP data have a much lower noise level and better control of systematics. Using these, we find that the anomalies are still present at a consistent level. Also the direction of maximum non-Gaussianity remains. Due to limitedmore » availability of computer resources, Hansen et al. were unable to calculate the full covariance matrix for the {chi}{sup 2}-test used. Here, we apply the full covariance matrix instead of the diagonal approximation and find that the non-Gaussianities disappear and there is no preferred non-Gaussian direction. We compare with simulations of weak lensing to see if this may cause the observed non-Gaussianity when using a diagonal covariance matrix. We conclude that weak lensing does not produce non-Gaussianity in the local curvature statistics at the scales investigated in this paper. The cause of the non-Gaussian detection in the case of a diagonal matrix remains unclear.« less

Matrix density alters zyxin phosphorylation, which limits peripheral process formation and extension in endothelial cells invading 3D collagen matrices.

PubMed

Abbey, Colette A; Bayless, Kayla J

2014-09-01

This study was designed to determine the optimal conditions required for known pro-angiogenic stimuli to elicit successful endothelial sprouting responses. We used an established, quantifiable model of endothelial cell (EC) sprout initiation where ECs were tested for invasion in low (1 mg/mL) and high density (5 mg/mL) 3D collagen matrices. Sphingosine 1-phosphate (S1P) alone, or S1P combined with stromal derived factor-1α (SDF) and phorbol ester (TPA), elicited robust sprouting responses. The ability of these factors to stimulate sprouting was more effective in higher density collagen matrices. S1P stimulation resulted in a significant increase in invasion distance, and with the exception of treatment groups containing phorbol ester, invasion distance was longer in 1mg/mL compared to 5mg/mL collagen matrices. Closer examination of cell morphology revealed that increasing matrix density and supplementing with SDF and TPA enhanced the formation of multicellular structures more closely resembling capillaries. TPA enhanced the frequency and size of lumen formation and correlated with a robust increase in phosphorylation of p42/p44 Erk kinase, while S1P and SDF did not. Also, a higher number of significantly longer extended processes formed in 5mg/mL compared to 1mg/mL collagen matrices. Because collagen matrices at higher density have been reported to be stiffer, we tested for changes in the mechanosensitive protein, zyxin. Interestingly, zyxin phosphorylation levels inversely correlated with matrix density, while levels of total zyxin did not change significantly. Immunofluorescence and localization studies revealed that total zyxin was distributed evenly throughout invading structures, while phosphorylated zyxin was slightly more intense in extended peripheral processes. Silencing zyxin expression increased extended process length and number of processes, while increasing zyxin levels decreased extended process length. Altogether these data indicate that ECs integrate signals from multiple exogenous factors, including changes in matrix density, to accomplish successful sprouting responses. We show here for the first time that zyxin limited the formation and extension of fine peripheral processes used by ECs for matrix interrogation, providing a molecular explanation for altered EC responses to high and low density collagen matrices. Copyright © 2014 International Society of Matrix Biology. Published by Elsevier B.V. All rights reserved.

Axial-Current Matrix Elements in Light Nuclei from Lattice QCD

DOE Office of Scientific and Technical Information (OSTI.GOV)

Savage, Martin; Shanahan, Phiala E.; Tiburzi, Brian C.

2016-12-01

I present results from the first lattice QCD calculations of axial-current matrix elements in light nuclei, performed by the NPLQCD collaboration. Precision calculations of these matrix elements, and the subsequent extraction of multi-nucleon axial-current operators, are essential in refining theoretical predictions of the proton-proton fusion cross section, neutrino-nucleus cross sections andmore » $$\\beta\\beta$$-decay rates of nuclei. In addition, they are expected to shed light on the phenomenological quenching of $$g_A$$ that is required in nuclear many-body calculations.« less

Optical Control of Intersubband Absorption in a Multiple Quantum Well-Embedded Semiconductor Microcravity

NASA Technical Reports Server (NTRS)

Liu, Ansheng; Ning, Cun-Zheng

2000-01-01

Optical intersubband response of a multiple quantum well (MQW)-embedded microcavity driven by a coherent pump field is studied theoretically. The n-type doped MQW structure with three subbands in the conduction band is sandwiched between a semi-infinite medium and a distributed Bragg reflector (DBR). A strong pump field couples the two upper subbands and a weak field probes the two lower subbands. To describe the optical response of the MQW-embedded microcavity, we adopt a semi-classical nonlocal response theory. Taking into account the pump-probe interaction, we derive the probe-induced current density associated with intersubband transitions from the single-particle density-matrix formalism. By incorporating the current density into the Maxwell equation, we solve the probe local field exactly by means of Green's function technique and the transfer-matrix method. We obtain an exact expression for the probe absorption coefficient of the microcavity. For a GaAs/Al(sub x)Ga(sub 1-x)As MQW structure sandwiched between a GaAs/AlAs DBR and vacuum, we performed numerical calculations of the probe absorption spectra for different parameters such as pump intensity, pump detuning, and cavity length. We find that the probe spectrum is strongly dependent on these parameters. In particular, we find that the combination of the cavity effect and the Autler-Townes effect results in a triplet in the optical spectrum of the MQW system. The optical absorption peak value and its location can be feasibly controlled by varying the pump intensity and detuning.

Spin-adapted matrix product states and operators

DOE Office of Scientific and Technical Information (OSTI.GOV)

Keller, Sebastian, E-mail: sebastian.keller@phys.chem.ethz.ch; Reiher, Markus, E-mail: markus.reiher@phys.chem.ethz.ch

Matrix product states (MPSs) and matrix product operators (MPOs) allow an alternative formulation of the density matrix renormalization group algorithm introduced by White. Here, we describe how non-abelian spin symmetry can be exploited in MPSs and MPOs by virtue of the Wigner–Eckart theorem at the example of the spin-adapted quantum chemical Hamiltonian operator.

Stress and Damage in Polymer Matrix Composite Materials Due to Material Degradation at High Temperatures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mcmanus, H.L.; Chamis, C.C.

1996-01-01

This report describes analytical methods for calculating stresses and damage caused by degradation of the matrix constituent in polymer matrix composite materials. Laminate geometry, material properties, and matrix degradation states are specified as functions of position and time. Matrix shrinkage and property changes are modeled as functions of the degradation states. The model is incorporated into an existing composite mechanics computer code. Stresses, strains, and deformations at the laminate, ply, and micro levels are calculated, and from these calculations it is determined if there is failure of any kind. The rationale for the model (based on published experimental work) ismore » presented, its integration into the laminate analysis code is outlined, and example results are given, with comparisons to existing material and structural data. The mechanisms behind the changes in properties and in surface cracking during long-term aging of polyimide matrix composites are clarified. High-temperature-material test methods are also evaluated.« less

Ab initio quantum chemical calculation of electron transfer matrix elements for large molecules

NASA Astrophysics Data System (ADS)

Zhang, Linda Yu; Friesner, Richard A.; Murphy, Robert B.

1997-07-01

Using a diabatic state formalism and pseudospectral numerical methods, we have developed an efficient ab initio quantum chemical approach to the calculation of electron transfer matrix elements for large molecules. The theory is developed at the Hartree-Fock level and validated by comparison with results in the literature for small systems. As an example of the power of the method, we calculate the electronic coupling between two bacteriochlorophyll molecules in various intermolecular geometries. Only a single self-consistent field (SCF) calculation on each of the monomers is needed to generate coupling matrix elements for all of the molecular pairs. The largest calculations performed, utilizing 1778 basis functions, required ˜14 h on an IBM 390 workstation. This is considerably less cpu time than would be necessitated with a supermolecule adiabatic state calculation and a conventional electronic structure code.

Experimental verification of a progressive damage model for composite laminates based on continuum damage mechanics. M.S. Thesis Final Report

NASA Technical Reports Server (NTRS)

Coats, Timothy William

1994-01-01

Progressive failure is a crucial concern when using laminated composites in structural design. Therefore the ability to model damage and predict the life of laminated composites is vital. The purpose of this research was to experimentally verify the application of the continuum damage model, a progressive failure theory utilizing continuum damage mechanics, to a toughened material system. Damage due to tension-tension fatigue was documented for the IM7/5260 composite laminates. Crack density and delamination surface area were used to calculate matrix cracking and delamination internal state variables, respectively, to predict stiffness loss. A damage dependent finite element code qualitatively predicted trends in transverse matrix cracking, axial splits and local stress-strain distributions for notched quasi-isotropic laminates. The predictions were similar to the experimental data and it was concluded that the continuum damage model provided a good prediction of stiffness loss while qualitatively predicting damage growth in notched laminates.

Phase-field study of ripening and rearrangement of precipitates under chemomechanical coupling

NASA Astrophysics Data System (ADS)

Schwarze, C.; Gupta, A.; Hickel, T.; Darvishi Kamachali, R.

2017-05-01

We investigate the evolution of large number of δ' coherent precipitates from a supersaturated Al-8 at.% Li alloy using large-scale phase-field simulations. A chemomechanical cross-coupling between mechanical relaxation and diffusion is taken into account by considering the dependence of elastic constants of the matrix phase onto the local concentration of solute atoms. The elastic constants as a function of solute concentration have been obtained using density functional theory calculations. As a result of the coupling, inverse ripening has been observed where the smaller precipitates grow at the expense of the larger ones. This is due to size-dependent concentration gradients existing around the precipitates. At the same time, precipitates rearrange themselves as a consequence of minimization of the total elastic energy of the system. It is found that the anisotropy of the chemomechanical coupling leads to the formation of new patterns of elasticity in the matrix thereby resulting in new alignments of the precipitates.

Experimental Verification of a Progressive Damage Model for IM7/5260 Laminates Subjected to Tension-Tension Fatigue

NASA Technical Reports Server (NTRS)

Coats, Timothy W.; Harris, Charles E.

1995-01-01

The durability and damage tolerance of laminated composites are critical design considerations for airframe composite structures. Therefore, the ability to model damage initiation and growth and predict the life of laminated composites is necessary to achieve structurally efficient and economical designs. The purpose of this research is to experimentally verify the application of a continuum damage model to predict progressive damage development in a toughened material system. Damage due to monotonic and tension-tension fatigue was documented for IM7/5260 graphite/bismaleimide laminates. Crack density and delamination surface area were used to calculate matrix cracking and delamination internal state variables to predict stiffness loss in unnotched laminates. A damage dependent finite element code predicted the stiffness loss for notched laminates with good agreement to experimental data. It was concluded that the continuum damage model can adequately predict matrix damage progression in notched and unnotched laminates as a function of loading history and laminate stacking sequence.

Fully nonlocal inelastic scattering computations for spectroscopical transmission electron microscopy methods

NASA Astrophysics Data System (ADS)

Rusz, Ján; Lubk, Axel; Spiegelberg, Jakob; Tyutyunnikov, Dmitry

2017-12-01

The complex interplay of elastic and inelastic scattering amenable to different levels of approximation constitutes the major challenge for the computation and hence interpretation of TEM-based spectroscopical methods. The two major approaches to calculate inelastic scattering cross sections of fast electrons on crystals—Yoshioka-equations-based forward propagation and the reciprocal wave method—are founded in two conceptually differing schemes—a numerical forward integration of each inelastically scattered wave function, yielding the exit density matrix, and a computation of inelastic scattering matrix elements using elastically scattered initial and final states (double channeling). Here, we compare both approaches and show that the latter is computationally competitive to the former by exploiting analytical integration schemes over multiple excited states. Moreover, we show how to include full nonlocality of the inelastic scattering event, neglected in the forward propagation approaches, at no additional computing costs in the reciprocal wave method. Detailed simulations show in some cases significant errors due to the z -locality approximation and hence pitfalls in the interpretation of spectroscopical TEM results.

Floating matrix tablets based on low density foam powder: effects of formulation and processing parameters on drug release.

PubMed

Streubel, A; Siepmann, J; Bodmeier, R

2003-01-01

The aim of this study was to develop and physicochemically characterize single unit, floating controlled drug delivery systems consisting of (i). polypropylene foam powder, (ii). matrix-forming polymer(s), (iii). drug, and (iv). filler (optional). The highly porous foam powder provided low density and, thus, excellent in vitro floating behavior of the tablets. All foam powder-containing tablets remained floating for at least 8 h in 0.1 N HCl at 37 degrees C. Different types of matrix-forming polymers were studied: hydroxypropyl methylcellulose (HPMC), polyacrylates, sodium alginate, corn starch, carrageenan, gum guar and gum arabic. The tablets eroded upon contact with the release medium, and the relative importance of drug diffusion, polymer swelling and tablet erosion for the resulting release patterns varied significantly with the type of matrix former. The release rate could effectively be modified by varying the "matrix-forming polymer/foam powder" ratio, the initial drug loading, the tablet geometry (radius and height), the type of matrix-forming polymer, the use of polymer blends and the addition of water-soluble or water-insoluble fillers (such as lactose or microcrystalline cellulose). The floating behavior of the low density drug delivery systems could successfully be combined with accurate control of the drug release patterns.

Nonlinear optical microscopy reveals invading endothelial cells anisotropically alter three-dimensional collagen matrices

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lee, P.-F.; Yeh, Alvin T.; Bayless, Kayla J.

The interactions between endothelial cells (ECs) and the extracellular matrix (ECM) are fundamental in mediating various steps of angiogenesis, including cell adhesion, migration and sprout formation. Here, we used a noninvasive and non-destructive nonlinear optical microscopy (NLOM) technique to optically image endothelial sprouting morphogenesis in three-dimensional (3D) collagen matrices. We simultaneously captured signals from collagen fibers and endothelial cells using second harmonic generation (SHG) and two-photon excited fluorescence (TPF), respectively. Dynamic 3D imaging revealed EC interactions with collagen fibers along with quantifiable alterations in collagen matrix density elicited by EC movement through and morphogenesis within the matrix. Specifically, we observedmore » increased collagen density in the area between bifurcation points of sprouting structures and anisotropic increases in collagen density around the perimeter of lumenal structures, but not advancing sprout tips. Proteinase inhibition studies revealed membrane-associated matrix metalloproteinase were utilized for sprout advancement and lumen expansion. Rho-associated kinase (p160ROCK) inhibition demonstrated that the generation of cell tension increased collagen matrix alterations. This study followed sprouting ECs within a 3D matrix and revealed that the advancing structures recognize and significantly alter their extracellular environment at the periphery of lumens as they progress.« less

Improved Dielectric Properties and Energy Storage Density of Poly(vinylidene fluoride-co-hexafluoropropylene) Nanocomposite with Hydantoin Epoxy Resin Coated BaTiO3.

PubMed

Luo, Hang; Zhang, Dou; Jiang, Chao; Yuan, Xi; Chen, Chao; Zhou, Kechao

2015-04-22

Energy storage materials are urgently demanded in modern electric power supply and renewable energy systems. The introduction of inorganic fillers to polymer matrix represents a promising avenue for the development of high energy density storage materials, which combines the high dielectric constant of inorganic fillers with supernal dielectric strength of polymer matrix. However, agglomeration and phase separation of inorganic fillers in the polymer matrix remain the key barriers to promoting the practical applications of the composites for energy storage. Here, we developed a low-cost and environmentally friendly route to modifying BaTiO3 (BT) nanoparticles by a kind of water-soluble hydantoin epoxy resin. The modified BT nanoparticles exhibited homogeneous dispersion in the ferroelectric polymer poly(vinylidene fluoride-co-hexafluoropropylene) (P(VDF-HFP)) matrix and strong interfacial adhesion with the polymer matrix. The dielectric constants of the nanocomposites increased significantly with the increase of the coated BT loading, while the dielectric loss of the nanocomposites was still as low as that of the pure P(VDF-HFP). The energy storage density of the nanocomposites was largely enhanced with the coated BT loading at the same electric field. The nanocomposite with 20 vol % BT exhibited an estimated maximum energy density of 8.13 J cm(-3), which was much higher than that of pure P(VDF-HFP) and other dielectric polymers. The findings of this research could provide a feasible approach to produce high energy density materials for practical application in energy storage.

Three-dimensional imaging for precise structural control of Si quantum dot networks for all-Si solar cells

NASA Astrophysics Data System (ADS)

Kourkoutis, Lena F.; Hao, Xiaojing; Huang, Shujuan; Puthen-Veettil, Binesh; Conibeer, Gavin; Green, Martin A.; Perez-Wurfl, Ivan

2013-07-01

All-Si tandem solar cells based on Si quantum dots (QDs) are a promising approach to future high-performance, thin film solar cells using abundant, stable and non-toxic materials. An important prerequisite to achieve a high conversion efficiency in such cells is the ability to control the geometry of the Si QD network. This includes the ability to control both, the size and arrangement of Si QDs embedded in a higher bandgap matrix. Using plasmon tomography we show the size, shape and density of Si QDs, that form in Si rich oxide (SRO)/SiO2 multilayers upon annealing, can be controlled by varying the SRO stoichiometry. Smaller, more spherical QDs of higher densities are obtained at lower Si concentrations. In richer SRO layers ellipsoidal QDs tend to form. Using electronic structure calculations within the effective mass approximation we show that ellipsoidal QDs give rise to reduced inter-QD coupling in the layer. Efficient carrier transport via mini-bands is in this case more likely across the multilayers provided the SiO2 spacer layer is thin enough to allow coupling in the vertical direction.All-Si tandem solar cells based on Si quantum dots (QDs) are a promising approach to future high-performance, thin film solar cells using abundant, stable and non-toxic materials. An important prerequisite to achieve a high conversion efficiency in such cells is the ability to control the geometry of the Si QD network. This includes the ability to control both, the size and arrangement of Si QDs embedded in a higher bandgap matrix. Using plasmon tomography we show the size, shape and density of Si QDs, that form in Si rich oxide (SRO)/SiO2 multilayers upon annealing, can be controlled by varying the SRO stoichiometry. Smaller, more spherical QDs of higher densities are obtained at lower Si concentrations. In richer SRO layers ellipsoidal QDs tend to form. Using electronic structure calculations within the effective mass approximation we show that ellipsoidal QDs give rise to reduced inter-QD coupling in the layer. Efficient carrier transport via mini-bands is in this case more likely across the multilayers provided the SiO2 spacer layer is thin enough to allow coupling in the vertical direction. Electronic supplementary information (ESI) available: Electron tomography reconstruction movies. See DOI: 10.1039/c3nr01998e

Theoretical Infrared Spectra for Polycyclic Aromatic Hydrocarbon Neutrals, Cations and Anions

NASA Technical Reports Server (NTRS)

Langhoff, Stephen R.

1995-01-01

Calculations are carried out using density functional theory (DFT) to determine the harmonic frequencies and intensities of the neutrals and cations of thirteen polycyclic aromatic hydrocarbons (PAHs) up to the size of ovalene. Calculations are also carried out for a few PAH anions. The DFT harmonic frequencies, when uniformly scaled by the factor of 0.958 to account primarily for anharmonicity, agree with the matrix isolation fundamentals to within an average error of about 10 per centimeter. Electron correlation is found to significantly reduce the intensities of many of the cation harmonics, bringing them into much better agreement with the available experimental data. While the theoretical infrared spectra agree well with the experimental data for the neutral systems and for many of the cations, there are notable discrepancies with the experimental matrix isolation data for some PAH cations that are difficult to explain in terms of limitations in the calculations. In agreement with previous theoretical work, the present calculations show that the relative intensities for the astronomical unidentified infrared (UIR) bands agree reasonably well with those for a distribution of polycyclic aromatic hydrocarbon (PAH) cations, but not with a distribution of PAH neutrals. We also observe that the infrared spectra of highly symmetrical cations such as coronene agree much better with astronomical observations than do those of, for example, the polyacenes such as tetracene and pentacene. The total integrated intensities for the neutral species are found to increase linearly with size, while the total integrated intensities are much larger for the cations and scale more nearly quadratically with size. We conclude that emission from moderate-sized highly symmetric PAH cations such as coronene and larger could account for the UIR bands.

Efficient calculation of the polarizability: a simplified effective-energy technique

NASA Astrophysics Data System (ADS)

Berger, J. A.; Reining, L.; Sottile, F.

2012-09-01

In a recent publication [J.A. Berger, L. Reining, F. Sottile, Phys. Rev. B 82, 041103(R) (2010)] we introduced the effective-energy technique to calculate in an accurate and numerically efficient manner the GW self-energy as well as the polarizability, which is required to evaluate the screened Coulomb interaction W. In this work we show that the effective-energy technique can be used to further simplify the expression for the polarizability without a significant loss of accuracy. In contrast to standard sum-over-state methods where huge summations over empty states are required, our approach only requires summations over occupied states. The three simplest approximations we obtain for the polarizability are explicit functionals of an independent- or quasi-particle one-body reduced density matrix. We provide evidence of the numerical accuracy of this simplified effective-energy technique as well as an analysis of our method.

The dynamics of the optically driven Lambda transition of the 15N-V- center in diamond.

PubMed

González, Gabriel; Leuenberger, Michael N

2010-07-09

Recent experimental results demonstrate the possibility of writing quantum information in the ground state triplet of the (15)N-V(-) center in diamond by means of an optically driven spin non-conserving two-photon Lambda transition in the presence of a strong applied electric field. Our calculations show that the hyperfine interaction in the (15)N-V(-) center is capable of mediating such a transition. We use a density matrix approach to describe the exact dynamics for the allowed optical spin non-conserving transitions between two sublevels of the ground state triplet. This approach allows us to calculate the Rabi oscillations, by means of which we obtain a Rabi frequency with an upper bound determined by the hyperfine interaction. This result is crucial for the success of implementing optically driven quantum information processing with the N-V center in diamond.

Realistic Covariance Prediction for the Earth Science Constellation

NASA Technical Reports Server (NTRS)

Duncan, Matthew; Long, Anne

2006-01-01

Routine satellite operations for the Earth Science Constellation (ESC) include collision risk assessment between members of the constellation and other orbiting space objects. One component of the risk assessment process is computing the collision probability between two space objects. The collision probability is computed using Monte Carlo techniques as well as by numerically integrating relative state probability density functions. Each algorithm takes as inputs state vector and state vector uncertainty information for both objects. The state vector uncertainty information is expressed in terms of a covariance matrix. The collision probability computation is only as good as the inputs. Therefore, to obtain a collision calculation that is a useful decision-making metric, realistic covariance matrices must be used as inputs to the calculation. This paper describes the process used by the NASA/Goddard Space Flight Center's Earth Science Mission Operations Project to generate realistic covariance predictions for three of the Earth Science Constellation satellites: Aqua, Aura and Terra.

Computational nano-material design of exotic luminescent materials based upon europium doped gallium nitrides

NASA Astrophysics Data System (ADS)

Masago, Akira; Fukushima, Tetsuya; Sato, Kazunori; Katayama-Yoshida, Hiroshi

2015-03-01

Eu-doped GaN has attracted much attention, because the red light luminescence ability provides us with expectations to realize monolithic full-color LEDs, which work on seamless conditions such as substrates, electrodes, and operating bias voltages. Toward implementation of multifunctional activity into the luminescent materials using the spinodal nano-structures, we investigate atomic configurations and magnetic structures of the GaN crystal codoped with Eu, Mg, Si, O, and/or the vacancies using the density functional method (DFT) calculations. Our calculations show that the impurity clusterized distributions are energetically favorable more than the homogeneous distribution. Moreover, analyses of the formation energy and binding energy suggest that the clusterized distributions are spontaneously formed by the nano-spinodal decomposition. Though the host matrix has no magnetic moments, the cluster has finite magnetic moments, where Zener's p-f exchange interaction works between the Eu f-state and the nearby N p-states.

Kapitza resistance at segregated boundaries in β-SiC

NASA Astrophysics Data System (ADS)

Goel, Nipun; Webb, Edmund, III; Oztekin, Alparslan; Rickman, Jeffrey; Neti, Sudhakar

Silicon Carbide is a candidate material for high-temperature thermoelectric applications for harvesting waste heat associated with exhaust from automotive and furnaces as well hot surfaces in solar towers and power electronics. However, for SiC to be a viable thermoelectric material, its thermoelectric figure of merit must be improved significantly. In this talk we examine the role of grain-boundary segregation on phononic thermal transport, an important factor in determining the figure of merit, via non-equilibrium molecular dynamics simulations. In particular, we consider the role of dopant concentration and dopant/matrix interactions on the enhancement of the Kapitza resistance of symmetric tilt grain boundaries. We find that the calculated resistance depends on the segregation profile, with increases of more than a factor of 50 (relative to an unsegregated boundary) at the highest dopant concentrations. Finally, we relate the calculated phonon density of states to changes in the Kapitza resistance.

The least-squares finite element method for low-mach-number compressible viscous flows

NASA Technical Reports Server (NTRS)

Yu, Sheng-Tao

1994-01-01

The present paper reports the development of the Least-Squares Finite Element Method (LSFEM) for simulating compressible viscous flows at low Mach numbers in which the incompressible flows pose as an extreme. Conventional approach requires special treatments for low-speed flows calculations: finite difference and finite volume methods are based on the use of the staggered grid or the preconditioning technique; and, finite element methods rely on the mixed method and the operator-splitting method. In this paper, however, we show that such difficulty does not exist for the LSFEM and no special treatment is needed. The LSFEM always leads to a symmetric, positive-definite matrix through which the compressible flow equations can be effectively solved. Two numerical examples are included to demonstrate the method: first, driven cavity flows at various Reynolds numbers; and, buoyancy-driven flows with significant density variation. Both examples are calculated by using full compressible flow equations.

Theoretical and experimental studies of the structure and vibrational spectra of NTO

NASA Astrophysics Data System (ADS)

Sorescu, Dan C.; Sutton, Teressa R. L.; Thompson, Donald L.; Beardall, David; Wight, Charles A.

1996-10-01

The structure and vibrational spectra of the high explosive 5-nitro-2,4-dihydro-3H-1,2,4-triazol-3-one (NTO) have been determined by ab initio molecular orbital calculations at the Hartree-Fock and second-order Møller-Plesset levels and by density functional theory (B3LYP). Experimental frequencies for the molecule have been determined from infrared spectra of pure NTO films and NTO molecules isolated in an argon matrix at 21 K. A force field for gas phase NTO has been obtained based on calculated results at the MP2/6-311G∗∗ level. In addition, a force field for solid state NTO has been constructed using the experimental vibrational frequencies for NTO films and scaled ab initio vibrational frequencies. Differences between the solid state and gas phase results indicate that the environment and preparation procedure exert a marked influence on the spectral characteristics of the NTO molecule.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bezák, Viktor, E-mail: bezak@fmph.uniba.sk

Quantum theory of the non-harmonic oscillator defined by the energy operator proposed by Yurke and Buks (2006) is presented. Although these authors considered a specific problem related to a model of transmission lines in a Kerr medium, our ambition is not to discuss the physical substantiation of their model. Instead, we consider the problem from an abstract, logically deductive, viewpoint. Using the Yurke–Buks energy operator, we focus attention on the imaginary-time propagator. We derive it as a functional of the Mehler kernel and, alternatively, as an exact series involving Hermite polynomials. For a statistical ensemble of identical oscillators defined bymore » the Yurke–Buks energy operator, we calculate the partition function, average energy, free energy and entropy. Using the diagonal element of the canonical density matrix of this ensemble in the coordinate representation, we define a probability density, which appears to be a deformed Gaussian distribution. A peculiarity of this probability density is that it may reveal, when plotted as a function of the position variable, a shape with two peaks located symmetrically with respect to the central point.« less

Tuning three-dimensional collagen matrix stiffness independently of collagen concentration modulates endothelial cell behavior.

PubMed

Mason, Brooke N; Starchenko, Alina; Williams, Rebecca M; Bonassar, Lawrence J; Reinhart-King, Cynthia A

2013-01-01

Numerous studies have described the effects of matrix stiffening on cell behavior using two-dimensional synthetic surfaces; however, less is known about the effects of matrix stiffening on cells embedded in three-dimensional in vivo-like matrices. A primary limitation in investigating the effects of matrix stiffness in three dimensions is the lack of materials that can be tuned to control stiffness independently of matrix density. Here, we use collagen-based scaffolds where the mechanical properties are tuned using non-enzymatic glycation of the collagen in solution, prior to polymerization. Collagen solutions glycated prior to polymerization result in collagen gels with a threefold increase in compressive modulus without significant changes to the collagen architecture. Using these scaffolds, we show that endothelial cell spreading increases with matrix stiffness, as does the number and length of angiogenic sprouts and the overall spheroid outgrowth. Differences in sprout length are maintained even when the receptor for advanced glycation end products is inhibited. Our results demonstrate the ability to de-couple matrix stiffness from matrix density and structure in collagen gels, and that increased matrix stiffness results in increased sprouting and outgrowth. Copyright © 2012 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Core Level Shifts of Hydrogenated Pyridinic and Pyrrolic Nitrogen in the Nitrogen-Containing Graphene-Based Electrocatalysts: In-Plane vs Edge Defects

DOE Office of Scientific and Technical Information (OSTI.GOV)

Matanovic, Ivana; Artyushkova, Kateryna; Strand, Matthew B.

A combination of N 1s X-ray photoelectron spectroscopy (XPS) and first principles calculations of nitrogen-containing model electrocatalysts was used to elucidate the nature of the nitrogen defects that contribute to the binding energy (BE) range of the N 1s XPS spectra of these materials above ~400 eV. Experimental core level shifts were obtained for a set of model materials, namely N-doped carbon nanospheres, Fe–N–carbon nanospheres, polypyrrole, polypyridine, and pyridinium chloride, and were compared to the shifts calculated using density functional theory. The results confirm that the broad peak positioned at ~400.7 eV in the N 1s XPS spectra of N-containingmore » catalysts, which is typically assigned to pyrrolic nitrogen, contains contributions from other hydrogenated nitrogen species such as hydrogenated pyridinic functionalities. Namely, N 1s BEs of hydrogenated pyridinic-N and pyrrolic-N were calculated as 400.6 and 400.7 eV, respectively, using the Perdew–Burke–Ernzerhof exchange-correlation functional. A special emphasis was placed on the study of the differences in the XPS imprint of N-containing defects that are situated in the plane and on the edges of the graphene sheet. Density functional theory calculations for BEs of the N 1s of in-plane and edge defects show that hydrogenated N defects are more sensitive to the change in the chemical environment in the carbon matrix than the non-hydrogenated N defects. In conclusion, calculations also show that edge-hydrogenated pyridinic-N and pyrrolic-N defects only contribute to the N 1s XPS peak located at ~400.7 eV if the graphene edges are oxygenated or terminated with bare carbon atoms.« less

Core Level Shifts of Hydrogenated Pyridinic and Pyrrolic Nitrogen in the Nitrogen-Containing Graphene-Based Electrocatalysts: In-Plane vs Edge Defects

DOE PAGES

Matanovic, Ivana; Artyushkova, Kateryna; Strand, Matthew B.; ...

2016-12-07

A combination of N 1s X-ray photoelectron spectroscopy (XPS) and first principles calculations of nitrogen-containing model electrocatalysts was used to elucidate the nature of the nitrogen defects that contribute to the binding energy (BE) range of the N 1s XPS spectra of these materials above ~400 eV. Experimental core level shifts were obtained for a set of model materials, namely N-doped carbon nanospheres, Fe–N–carbon nanospheres, polypyrrole, polypyridine, and pyridinium chloride, and were compared to the shifts calculated using density functional theory. The results confirm that the broad peak positioned at ~400.7 eV in the N 1s XPS spectra of N-containingmore » catalysts, which is typically assigned to pyrrolic nitrogen, contains contributions from other hydrogenated nitrogen species such as hydrogenated pyridinic functionalities. Namely, N 1s BEs of hydrogenated pyridinic-N and pyrrolic-N were calculated as 400.6 and 400.7 eV, respectively, using the Perdew–Burke–Ernzerhof exchange-correlation functional. A special emphasis was placed on the study of the differences in the XPS imprint of N-containing defects that are situated in the plane and on the edges of the graphene sheet. Density functional theory calculations for BEs of the N 1s of in-plane and edge defects show that hydrogenated N defects are more sensitive to the change in the chemical environment in the carbon matrix than the non-hydrogenated N defects. In conclusion, calculations also show that edge-hydrogenated pyridinic-N and pyrrolic-N defects only contribute to the N 1s XPS peak located at ~400.7 eV if the graphene edges are oxygenated or terminated with bare carbon atoms.« less

Size Reduction of Hamiltonian Matrix for Large-Scale Energy Band Calculations Using Plane Wave Bases

NASA Astrophysics Data System (ADS)

Morifuji, Masato

2018-01-01

We present a method of reducing the size of a Hamiltonian matrix used in calculations of electronic states. In the electronic states calculations using plane wave basis functions, a large number of plane waves are often required to obtain precise results. Even using state-of-the-art techniques, the Hamiltonian matrix often becomes very large. The large computational time and memory necessary for diagonalization limit the widespread use of band calculations. We show a procedure of deriving a reduced Hamiltonian constructed using a small number of low-energy bases by renormalizing high-energy bases. We demonstrate numerically that the significant speedup of eigenstates evaluation is achieved without losing accuracy.

Role of the Euclidean signature in lattice calculations of quasidistributions and other nonlocal matrix elements

NASA Astrophysics Data System (ADS)

Briceño, Raúl A.; Hansen, Maxwell T.; Monahan, Christopher J.

2017-07-01

Lattice quantum chromodynamics (QCD) provides the only known systematic, nonperturbative method for first-principles calculations of nucleon structure. However, for quantities such as light-front parton distribution functions (PDFs) and generalized parton distributions (GPDs), the restriction to Euclidean time prevents direct calculation of the desired observable. Recently, progress has been made in relating these quantities to matrix elements of spatially nonlocal, zero-time operators, referred to as quasidistributions. Still, even for these time-independent matrix elements, potential subtleties have been identified in the role of the Euclidean signature. In this work, we investigate the analytic behavior of spatially nonlocal correlation functions and demonstrate that the matrix elements obtained from Euclidean lattice QCD are identical to those obtained using the Lehmann-Symanzik-Zimmermann reduction formula in Minkowski space. After arguing the equivalence on general grounds, we also show that it holds in a perturbative calculation, where special care is needed to identify the lattice prediction. Finally we present a proof of the uniqueness of the matrix elements obtained from Minkowski and Euclidean correlation functions to all order in perturbation theory.

Role of the Euclidean signature in lattice calculations of quasidistributions and other nonlocal matrix elements

DOE PAGES

Briceno, Raul A.; Hansen, Maxwell T.; Monahan, Christopher J.

2017-07-11

Lattice quantum chromodynamics (QCD) provides the only known systematic, nonperturbative method for first-principles calculations of nucleon structure. However, for quantities such as light-front parton distribution functions (PDFs) and generalized parton distributions (GPDs), the restriction to Euclidean time prevents direct calculation of the desired observable. Recently, progress has been made in relating these quantities to matrix elements of spatially nonlocal, zero-time operators, referred to as quasidistributions. Still, even for these time-independent matrix elements, potential subtleties have been identified in the role of the Euclidean signature. In this work, we investigate the analytic behavior of spatially nonlocal correlation functions and demonstrate thatmore » the matrix elements obtained from Euclidean lattice QCD are identical to those obtained using the Lehmann-Symanzik-Zimmermann reduction formula in Minkowski space. After arguing the equivalence on general grounds, we also show that it holds in a perturbative calculation, where special care is needed to identify the lattice prediction. Lastly, we present a proof of the uniqueness of the matrix elements obtained from Minkowski and Euclidean correlation functions to all order in perturbation theory.« less

Hydrogen bonds, interfacial stiffness moduli, and the interlaminar shear strength of carbon fiber-epoxy matrix composites

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cantrell, John H., E-mail: john.h.cantrell@nasa.gov

2015-03-15

The chemical treatment of carbon fibers used in carbon fiber-epoxy matrix composites greatly affects the fraction of hydrogen bonds (H-bonds) formed at the fiber-matrix interface. The H-bonds are major contributors to the fiber-matrix interfacial shear strength and play a direct role in the interlaminar shear strength (ILSS) of the composite. The H-bond contributions τ to the ILSS and magnitudes K{sub N} of the fiber-matrix interfacial stiffness moduli of seven carbon fiber-epoxy matrix composites, subjected to different fiber surface treatments, are calculated from the Morse potential for the interactions of hydroxyl and carboxyl acid groups formed on the carbon fiber surfacesmore » with epoxy receptors. The τ calculations range from 7.7 MPa to 18.4 MPa in magnitude, depending on fiber treatment. The K{sub N} calculations fall in the range (2.01 – 4.67) ×10{sup 17} N m{sup −3}. The average ratio K{sub N}/|τ| is calculated to be (2.59 ± 0.043) × 10{sup 10} m{sup −1} for the seven composites, suggesting a nearly linear connection between ILSS and H-bonding at the fiber-matrix interfaces. The linear connection indicates that τ may be assessable nondestructively from measurements of K{sub N} via a technique such as angle beam ultrasonic spectroscopy.« less

A parallel algorithm for Hamiltonian matrix construction in electron-molecule collision calculations: MPI-SCATCI

NASA Astrophysics Data System (ADS)

Al-Refaie, Ahmed F.; Tennyson, Jonathan

2017-12-01

Construction and diagonalization of the Hamiltonian matrix is the rate-limiting step in most low-energy electron - molecule collision calculations. Tennyson (1996) implemented a novel algorithm for Hamiltonian construction which took advantage of the structure of the wavefunction in such calculations. This algorithm is re-engineered to make use of modern computer architectures and the use of appropriate diagonalizers is considered. Test calculations demonstrate that significant speed-ups can be gained using multiple CPUs. This opens the way to calculations which consider higher collision energies, larger molecules and / or more target states. The methodology, which is implemented as part of the UK molecular R-matrix codes (UKRMol and UKRMol+) can also be used for studies of bound molecular Rydberg states, photoionization and positron-molecule collisions.

Variational second order density matrix study of F3-: importance of subspace constraints for size-consistency.

PubMed

van Aggelen, Helen; Verstichel, Brecht; Bultinck, Patrick; Van Neck, Dimitri; Ayers, Paul W; Cooper, David L

2011-02-07

Variational second order density matrix theory under "two-positivity" constraints tends to dissociate molecules into unphysical fractionally charged products with too low energies. We aim to construct a qualitatively correct potential energy surface for F(3)(-) by applying subspace energy constraints on mono- and diatomic subspaces of the molecular basis space. Monoatomic subspace constraints do not guarantee correct dissociation: the constraints are thus geometry dependent. Furthermore, the number of subspace constraints needed for correct dissociation does not grow linearly with the number of atoms. The subspace constraints do impose correct chemical properties in the dissociation limit and size-consistency, but the structure of the resulting second order density matrix method does not exactly correspond to a system of noninteracting units.

Confinement of anomalous liquids in nanoporous matrices.

PubMed

Strekalova, Elena G; Luo, Jiayuan; Stanley, H Eugene; Franzese, Giancarlo; Buldyrev, Sergey V

2012-09-07

Using molecular dynamics simulations, we investigate the effects of different nanoconfinements on complex liquids-e.g., colloids or protein solutions-with density anomalies and a liquid-liquid phase transition (LLPT). In all the confinements, we find a strong depletion effect with a large increase in liquid density near the confining surface. If the nanoconfinement is modeled by an ordered matrix of nanoparticles, we find that the anomalies are preserved. On the contrary, if the confinement is modeled by a disordered matrix of nanoparticles, we find a drastically different phase diagram: the LLPT shifts to lower pressures and temperatures, and the anomalies become weaker, as the disorder increases. We find that the density heterogeneities induced by the disordered matrix are responsible for the weakening of the LLPT and the disappearance of the anomalies.

Hybrid reconstruction of quantum density matrix: when low-rank meets sparsity

NASA Astrophysics Data System (ADS)

Li, Kezhi; Zheng, Kai; Yang, Jingbei; Cong, Shuang; Liu, Xiaomei; Li, Zhaokai

2017-12-01

Both the mathematical theory and experiments have verified that the quantum state tomography based on compressive sensing is an efficient framework for the reconstruction of quantum density states. In recent physical experiments, we found that many unknown density matrices in which people are interested in are low-rank as well as sparse. Bearing this information in mind, in this paper we propose a reconstruction algorithm that combines the low-rank and the sparsity property of density matrices and further theoretically prove that the solution of the optimization function can be, and only be, the true density matrix satisfying the model with overwhelming probability, as long as a necessary number of measurements are allowed. The solver leverages the fixed-point equation technique in which a step-by-step strategy is developed by utilizing an extended soft threshold operator that copes with complex values. Numerical experiments of the density matrix estimation for real nuclear magnetic resonance devices reveal that the proposed method achieves a better accuracy compared to some existing methods. We believe that the proposed method could be leveraged as a generalized approach and widely implemented in the quantum state estimation.

Quantum non-Abelian hydrodynamics: Anyonic or spin-orbital entangled liquids, nonunitarity of scattering matrix and charge fractionalization

NASA Astrophysics Data System (ADS)

Pareek, Tribhuvan Prasad

2015-09-01

In this article, we develop an exact (nonadiabatic, nonperturbative) density matrix scattering theory for a two component quantum liquid which interacts or scatters off from a generic spin-dependent quantum potential. The generic spin dependent quantum potential [Eq. (1)] is a matrix potential, hence, adiabaticity criterion is ill-defined. Therefore the full matrix potential should be treated nonadiabatically. We succeed in doing so using the notion of vectorial matrices which allows us to obtain an exact analytical expression for the scattered density matrix (SDM), ϱsc [Eq. (30)]. We find that the number or charge density in scattered fluid, Tr(ϱsc), expressions in Eqs. (32) depends on nontrivial quantum interference coefficients, Qα β 0ijk, which arises due to quantum interference between spin-independent and spin-dependent scattering amplitudes and among spin-dependent scattering amplitudes. Further it is shown that Tr(ϱsc) can be expressed in a compact form [Eq. (39)] where the effect of quantum interference coefficients can be included using a vector Qαβ, which allows us to define a vector order parameterQ. Since the number density is obtained using an exact scattered density matrix, therefore, we do not need to prove that Q is non-zero. However, for sake of completeness, we make detailed mathematical analysis for the conditions under which the vector order parameterQ would be zero or nonzero. We find that in presence of spin-dependent interaction the vector order parameterQ is necessarily nonzero and is related to the commutator and anti-commutator of scattering matrix S with its dagger S† [Eq. (78)]. It is further shown that Q≠0, implies four physically equivalent conditions,i.e., spin-orbital entanglement is nonzero, non-Abelian scattering phase, i.e., matrices, scattering matrix is nonunitary and the broken time reversal symmetry for SDM. This also implies that quasi particle excitation are anyonic in nature, hence, charge fractionalization is a natural consequence. This aspect has also been discussed from the perspective of number or charge density conservation, which implies i.e., Tr(ϱ} sc) = Tr(ϱin). On the other hand Q = 0 turns out to be a mathematically forced unphysical solution in presence of spin-dependent potential or scattering which is equivalent to Abelian hydrodynamics, unitary scattering matrix, absence of spin-space entanglement and preserved time reversal symmetry. We have formulated the theory using mesoscopic language, specifically, we have considered two terminal systems connected to spin-dependent scattering region, which is equivalent to having two potential wells separated by a generic spin-dependent potential barrier. The formulation using mesoscopic language is practically useful because it leads directly to the measured quantities such as conductance and spin-polarization density in the leads, however, the presented formulation is not limited to the mesoscopic system only, its generality has been stressed at various places in this article.

Topics in QCD at Nonzero Temperature and Density

NASA Astrophysics Data System (ADS)

Pangeni, Kamal

Understanding the behavior of matter at ultra-high density such as neutron stars require the knowledge of ground state properties of Quantum chromodynamics (QCD) at finite chemical potential. However, this task has turned out to be very difficult because of two main reasons: 1) QCD may still be strongly coupled at those regimes making perturbative calculations unreliable and 2) QCD at finite density suffers from the sign problem that makes the use of lattice simulation problematic and it even affects phenomenological models. In the first part of this thesis, we show that the sign problem in analytical calculations of finite density models can be solved by considering the CK-symmetric, where C is charge conjugation and K is complex conjugation, complex saddle points of the effective action. We then explore the properties and consequences of such complex saddle points at non-zero temperature and density. Due to CK symmetry, the mass matrix eigenvalues in these models are not always real but can be complex, which results in damped oscillation of the density-density correlation function, a new feature of finite density models. To address the generality of such behavior, we next consider a lattice model of QCD with static quarks at strong-coupling. Computation of the mass spectrum confirms the existence of complex eigenvalues in much of temperature-chemical potential plane. This provides an independent confirmation of our results obtained using phenomenological models of QCD. The existence of regions in parameter space where density-density correlation function exhibit damped oscillation is one of the hallmarks of typical liquid-gas system. The formalism developed to tackle the sign problem in QCD models actually gives a simple understanding for the existence of such behavior in liquid-gas system. To this end, we develop a generic field theoretic model for the treatment of liquid-gas phase transition. An effective field theory at finite density derived from a fundamental four dimensional field theory turns out to be complex but CK symmetric. The existence of CK symmetry results in complex mass eigenvalues, which in turn leads to damped oscillatory behavior of the density-density correlation function. In the last part of this thesis, we study the effect of large amplitude density oscillations on the transport properties of superfluid nuclear matter. In nuclear matter at neutron-star densities and temperature, Cooper pairing leads to the formations of a gap in the nucleon excitation spectra resulting in exponentially strong Boltzmann suppression of many transport coefficients. Previous calculations have shown evidence that density oscillations of sufficiently large amplitude can overcome this suppression for flavor-changing beta processes via the mechanism of "gap-bridging". We address the simplifications made in that initial work, and show that gap bridging can counteract Boltzmann suppression of neutrino emissivity for the realistic case of modified Urca processes in matter with 3 P2 neutron pairing.

Reservoir characterization of the Upper Jurassic geothermal target formations (Molasse Basin, Germany): role of thermofacies as exploration tool

NASA Astrophysics Data System (ADS)

Homuth, S.; Götz, A. E.; Sass, I.

2015-06-01

The Upper Jurassic carbonates of the southern German Molasse Basin are the target of numerous geothermal combined heat and power production projects since the year 2000. A production-orientated reservoir characterization is therefore of high economic interest. Outcrop analogue studies enable reservoir property prediction by determination and correlation of lithofacies-related thermo- and petrophysical parameters. A thermofacies classification of the carbonate formations serves to identify heterogeneities and production zones. The hydraulic conductivity is mainly controlled by tectonic structures and karstification, whilst the type and grade of karstification is facies related. The rock permeability has only a minor effect on the reservoir's sustainability. Physical parameters determined on oven-dried samples have to be corrected, applying reservoir transfer models to water-saturated reservoir conditions. To validate these calculated parameters, a Thermo-Triaxial-Cell simulating the temperature and pressure conditions of the reservoir is used and calorimetric and thermal conductivity measurements under elevated temperature conditions are performed. Additionally, core and cutting material from a 1600 m deep research drilling and a 4850 m (total vertical depth, measured depth: 6020 m) deep well is used to validate the reservoir property predictions. Under reservoir conditions a decrease in permeability of 2-3 magnitudes is observed due to the thermal expansion of the rock matrix. For tight carbonates the matrix permeability is temperature-controlled; the thermophysical matrix parameters are density-controlled. Density increases typically with depth and especially with higher dolomite content. Therefore, thermal conductivity increases; however the dominant factor temperature also decreases the thermal conductivity. Specific heat capacity typically increases with increasing depth and temperature. The lithofacies-related characterization and prediction of reservoir properties based on outcrop and drilling data demonstrates that this approach is a powerful tool for exploration and operation of geothermal reservoirs.

Numerical simulations of electromagnetic scattering by Solar system objects

NASA Astrophysics Data System (ADS)

Dlugach, Janna M.

2016-11-01

Having been profoundly stimulated by the seminal work of Viktor V. Sobolev, I have been involved in multi-decadal research in the fields of radiative transfer, electromagnetic scattering by morphologically complex particles and particulate media, and planetary remote sensing. Much of this research has been done in close collaboration with other "descendants" of Academician Sobolev. This tutorial paper gives a representative overview of the results of extensive numerical simulations (in the vast majority carried out in collaboration with Michael Mishchenko) used to analyze remote-sensing observations of Solar system objects and based on highly accurate methods of the radiative transfer theory and direct computer solvers of the Maxwell equations. Using the atmosphere of Jupiter as a proving ground and performing T-matrix and radiative-transfer calculations helps demonstrate the strong effect of aerosol-particle shapes on the accuracy of remote-sensing retrievals. I then discuss the application of the T-matrix method, a numerically exact solution of the vector radiative transfer equation, and the theory of coherent backscattering to an analysis of polarimetric radar observations of Saturn's rings. Numerical modeling performed by using the superposition T-matrix method in application to cometary dust in the form of aggregates serves to reproduce the results of polarimetric observations of the distant comet C/2010 S1. On the basis of direct computer solutions of the Maxwell equations, it is demonstrated that all backscattering effects predicted by the low-density theories of radiative transfer and coherent backscattering can also be identified for media with volume packing densities typically encountered in natural and artificial environments. This result implies that spectacular opposition effects observed for some high-albedo atmoshereless Solar system bodies can be attributed to coherent backscattering of sunlight by regolith layers composed of microscopic particles.

Generation of Stationary Non-Gaussian Time Histories with a Specified Cross-spectral Density

DOE PAGES

Smallwood, David O.

1997-01-01

The paper reviews several methods for the generation of stationary realizations of sampled time histories with non-Gaussian distributions and introduces a new method which can be used to control the cross-spectral density matrix and the probability density functions (pdfs) of the multiple input problem. Discussed first are two methods for the specialized case of matching the auto (power) spectrum, the skewness, and kurtosis using generalized shot noise and using polynomial functions. It is then shown that the skewness and kurtosis can also be controlled by the phase of a complex frequency domain description of the random process. The general casemore » of matching a target probability density function using a zero memory nonlinear (ZMNL) function is then covered. Next methods for generating vectors of random variables with a specified covariance matrix for a class of spherically invariant random vectors (SIRV) are discussed. Finally the general case of matching the cross-spectral density matrix of a vector of inputs with non-Gaussian marginal distributions is presented.« less

Enhanced osteoprogenitor elongated collagen fiber matrix formation by bioactive glass ionic silicon dependent on Sp7 (osterix) transcription.

PubMed

Varanasi, Venu G; Odatsu, Tetsurou; Bishop, Timothy; Chang, Joyce; Owyoung, Jeremy; Loomer, Peter M

2016-10-01

Bioactive glasses release ions, those enhance osteoblast collagen matrix synthesis and osteogenic marker expression during bone healing. Collagen matrix density and osteogenic marker expression depend on osteogenic transcription factors, (e.g., Osterix (OSX)). We hypothesize that enhanced expression and formation of collagen by Si(4+) depends on enhanced expression of OSX transcription. Experimental bioactive glass (6P53-b) and commercial Bioglass(TM) (45S5) were dissolved in basal medium to make glass conditioned medium (GCM). ICP-MS analysis was used to measure bioactive glass ion release rates. MC3T3-E1 cells were cultured for 20 days, and gene expression and extracellular matrix collagen formation was analyzed. In a separate study, siRNA was used to determine the effect of OSX knockdown on impacting the effect of Si(4+) on osteogenic markers and matrix collagen formation. Each bioactive glass exhibited similar ion release rates for all ions, except Mg(2+) released by 6P53-b. Gene expression results showed that GCM markedly enhanced many osteogenic markers, and 45S5 GCM showed higher levels of expression and collagen matrix fiber bundle density than 6P53-b GCM. Upon knockdown of OSX transcription, collagen type 5, alkaline phosphatase, and matrix density were not enhanced as compared to wild type cells. This study illustrates that the enhancement of elongated collagen fiber matrix formation by Si(±) depends on OSX transcription. © 2016 Wiley Periodicals, Inc. J Biomed Mater Res Part A: 104A: 2604-2615, 2016. © 2016 Wiley Periodicals, Inc.

Simple derivation of the Lindblad equation

NASA Astrophysics Data System (ADS)

Pearle, Philip

2012-07-01

The Lindblad equation is an evolution equation for the density matrix in quantum theory. It is the general linear, Markovian, form which ensures that the density matrix is Hermitian, trace 1, positive and completely positive. Some elementary examples of the Lindblad equation are given. The derivation of the Lindblad equation presented here is ‘simple’ in that all it uses is the expression of a Hermitian matrix in terms of its orthonormal eigenvectors and real eigenvalues. Thus, it is appropriate for students who have learned the algebra of quantum theory. Where helpful, arguments are first given in a two-dimensional Hilbert space.

Cross-linked κ-carrageenan polymer/zinc nanoporous composite matrix for expanded bed application: Fabrication and hydrodynamic characterization.

PubMed

Mohsenkhani, Sadaf; Jahanshahi, Mohsen; Rahimpour, Ahmad

2015-08-21

Expanded bed adsorption (EBA) is a reliable separation technique for the purification of bioproducts from complex feedstocks. The specifically designed adsorbent is necessary to form a stable expanded bed. In the present work, a novel custom-designed composite matrix has been prepared through the method of water-in-oil emulsification. In order to develop an adsorbent with desirable qualities and reduce the costs, κ-carrageenan and zinc powder were used as the polymeric skeleton and the densifier, respectively. The prepared composite matrix was named as KC-Zn. Optical microscope (OM) and scanning electron microscope (SEM) were applied to characterize the morphology and structure of prepared composite matrix. These analyses approved good spherical shape and porous structure with nano-scale pores in the range of about 60-180nm. The results from the particle size analyzer (PSA) revealed that all the KC-Zn beads followed logarithmic normal size distribution with the range of 50-350μm and average diameter of 160-230μm, respectively. Main physical properties of KC-Zn matrices were measured as a function of zinc powder ratio to κ-carrageenan slurry, which showed an appropriate wet density in the range of 1.39-2.27g/ml, water content of 72.67-36.41% and porosity of 98.07-80.24%, respectively. The effects of matrix density and liquid phase viscosity on hydrodynamic behavior of prepared matrix have been investigated by residence time distribution (RTD) experiments in an expanded bed. The results indicated that in a constant liquid velocity as the matrix density was increased, the expansion factor of bed decreased and the axial mixing coefficient increased. Moreover, an enhancement in the fluid viscosity led to an increase in the bed expansion and a decrease in the stability of expanded bed. Therefore using a matrix with higher density seems necessary to face viscous feedstocks. All the results demonstrated that proper physical properties and hydrodynamic characteristics of KC-Zn matrix confirm good potential for possible use in high flow rate expanded bed operations. Copyright © 2015 Elsevier B.V. All rights reserved.

Optical factors determined by the T-matrix method in turbidity measurement of absolute coagulation rate constants.

PubMed

Xu, Shenghua; Liu, Jie; Sun, Zhiwei

2006-12-01

Turbidity measurement for the absolute coagulation rate constants of suspensions has been extensively adopted because of its simplicity and easy implementation. A key factor in deriving the rate constant from experimental data is how to theoretically evaluate the so-called optical factor involved in calculating the extinction cross section of doublets formed during aggregation. In a previous paper, we have shown that compared with other theoretical approaches, the T-matrix method provides a robust solution to this problem and is effective in extending the applicability range of the turbidity methodology, as well as increasing measurement accuracy. This paper will provide a more comprehensive discussion of the physical insight for using the T-matrix method in turbidity measurement and associated technical details. In particular, the importance of ensuring the correct value for the refractive indices for colloidal particles and the surrounding medium used in the calculation is addressed, because the indices generally vary with the wavelength of the incident light. The comparison of calculated results with experiments shows that the T-matrix method can correctly calculate optical factors even for large particles, whereas other existing theories cannot. In addition, the data of the optical factor calculated by the T-matrix method for a range of particle radii and incident light wavelengths are listed.

Propensity, Probability, and Quantum Theory

NASA Astrophysics Data System (ADS)

Ballentine, Leslie E.

2016-08-01

Quantum mechanics and probability theory share one peculiarity. Both have well established mathematical formalisms, yet both are subject to controversy about the meaning and interpretation of their basic concepts. Since probability plays a fundamental role in QM, the conceptual problems of one theory can affect the other. We first classify the interpretations of probability into three major classes: (a) inferential probability, (b) ensemble probability, and (c) propensity. Class (a) is the basis of inductive logic; (b) deals with the frequencies of events in repeatable experiments; (c) describes a form of causality that is weaker than determinism. An important, but neglected, paper by P. Humphreys demonstrated that propensity must differ mathematically, as well as conceptually, from probability, but he did not develop a theory of propensity. Such a theory is developed in this paper. Propensity theory shares many, but not all, of the axioms of probability theory. As a consequence, propensity supports the Law of Large Numbers from probability theory, but does not support Bayes theorem. Although there are particular problems within QM to which any of the classes of probability may be applied, it is argued that the intrinsic quantum probabilities (calculated from a state vector or density matrix) are most naturally interpreted as quantum propensities. This does not alter the familiar statistical interpretation of QM. But the interpretation of quantum states as representing knowledge is untenable. Examples show that a density matrix fails to represent knowledge.

The Density Matrix for Single-mode Light after k-Photon Absorption

NASA Astrophysics Data System (ADS)

Voigt, H.; Bandilla, A.

In order to continue and generalize the studies of the density matrix of a light field undergoing k-photon absorption, in this paper we put the emphasis on the off-diagonal elements. The solution obtained earlier for the diagonal elements describing the photon statistics can be found as a special case but will not be discussed again. The general solution calculated by recursion shows an asymptotic behaviour if the initial photon number is sufficiently high. Only the initial phase information survives. Illustrating the solution we start with coherent light and a generalized coherent state.Translated AbstractDie Dichtematrix eines Lichtstrahls nach k-Photonen-Absorption aus einer ModeWir führen die Betrachtungen über das Verhalten der Dichtematrix eines Lichtfeldes nach k-Photonen-Absorption aus einer Mode verallgemeinernd weiter und konzentrieren uns auf die Nichtdiagonalelemente. Die im folgenden angegebene allgemeine Lösung, die durch Rekursion gefunden wurde, enthält die schon früher erhaltene, jedoch hier nicht weiter diskutierte Lösung für die Diagonalelemente als Spezialfall. Sie zeigt ferner, daß es einen asymptotischen Zustand gibt, der eine von der Ausgangsintensität unabhängige Information über die Ausgangsphase enthält. Zur Diskussion der Lösung werden verschiedene Anfangsbedingungen betrachtet, so z. B. kohärentes Licht und kohärentes Licht, das ein Medium mit nichtlinearem Brechungsindex durchlaufen hat (Kerr-Effekt).

Exploiting the spatial locality of electron correlation within the parametric two-electron reduced-density-matrix method

NASA Astrophysics Data System (ADS)

DePrince, A. Eugene; Mazziotti, David A.

2010-01-01

The parametric variational two-electron reduced-density-matrix (2-RDM) method is applied to computing electronic correlation energies of medium-to-large molecular systems by exploiting the spatial locality of electron correlation within the framework of the cluster-in-molecule (CIM) approximation [S. Li et al., J. Comput. Chem. 23, 238 (2002); J. Chem. Phys. 125, 074109 (2006)]. The 2-RDMs of individual molecular fragments within a molecule are determined, and selected portions of these 2-RDMs are recombined to yield an accurate approximation to the correlation energy of the entire molecule. In addition to extending CIM to the parametric 2-RDM method, we (i) suggest a more systematic selection of atomic-orbital domains than that presented in previous CIM studies and (ii) generalize the CIM method for open-shell quantum systems. The resulting method is tested with a series of polyacetylene molecules, water clusters, and diazobenzene derivatives in minimal and nonminimal basis sets. Calculations show that the computational cost of the method scales linearly with system size. We also compute hydrogen-abstraction energies for a series of hydroxyurea derivatives. Abstraction of hydrogen from hydroxyurea is thought to be a key step in its treatment of sickle cell anemia; the design of hydroxyurea derivatives that oxidize more rapidly is one approach to devising more effective treatments.

Silicon quantum dots embedded in a SiO2 matrix: From structural study to carrier transport properties

NASA Astrophysics Data System (ADS)

Garcia-Castello, Nuria; Illera, Sergio; Guerra, Roberto; Prades, Joan Daniel; Ossicini, Stefano; Cirera, Albert

2013-08-01

We study the details of electronic transport related to the atomistic structure of silicon quantum dots embedded in a silicon dioxide matrix using ab initio calculations of the density of states. Several structural and composition features of quantum dots (QDs), such as diameter and amorphization level, are studied and correlated with transport under transfer Hamiltonian formalism. The current is strongly dependent on the QD density of states and on the conduction gap, both dependent on the dot diameter. In particular, as size increases, the available states inside the QD increase, while the QD band gap decreases due to relaxation of quantum confinement. Both effects contribute to increasing the current with the dot size. Besides, valence band offset between the band edges of the QD and the silica, and conduction band offset in a minor grade, increases with the QD diameter up to the theoretical value corresponding to planar heterostructures, thus decreasing the tunneling transmission probability and hence the total current. We discuss the influence of these parameters on electron and hole transport, evidencing a correlation between the electron (hole) barrier value and the electron (hole) current, and obtaining a general enhancement of the electron (hole) transport for larger (smaller) QD. Finally, we show that crystalline and amorphous structures exhibit enhanced probability of hole and electron current, respectively.