On the resolvents methods in quantum perturbation calculations

International Nuclear Information System (INIS)

Burzynski, A.

1979-01-01

This paper gives a systematic review of resolvent methods in quantum perturbation calculations. The case of discrete spectrum of hamiltonian is considered specially (in the literature this is the fewest considered case). The topics of calculations of quantum transitions by using of the resolvent formalism, quantum transitions between states from particular subspaces, the shifts of energy levels, are shown. The main ideas of stationary perturbation theory developed by Lippmann and Schwinger are considered too. (author)

Accurate quantum dynamics calculations using symmetrized Gaussians on a doubly dense Von Neumann lattice

International Nuclear Information System (INIS)

Halverson, Thomas; Poirier, Bill

2012-01-01

In a series of earlier articles [B. Poirier, J. Theor. Comput. Chem. 2, 65 (2003); B. Poirier and A. Salam, J. Chem. Phys. 121, 1690 (2004); and ibid. 121, 1704 (2004)], a new method was introduced for performing exact quantum dynamics calculations. The method uses a “weylet” basis set (orthogonalized Weyl-Heisenberg wavelets) combined with phase space truncation, to defeat the exponential scaling of CPU effort with system dimensionality—the first method ever able to achieve this long-standing goal. Here, we develop another such method, which uses a much more convenient basis of momentum-symmetrized Gaussians. Despite being non-orthogonal, symmetrized Gaussians are collectively local, allowing for effective phase space truncation. A dimension-independent code for computing energy eigenstates of both coupled and uncoupled systems has been created, exploiting massively parallel algorithms. Results are presented for model isotropic uncoupled harmonic oscillators and coupled anharmonic oscillators up to 27 dimensions. These are compared with the previous weylet calculations (uncoupled harmonic oscillators up to 15 dimensions), and found to be essentially just as efficient. Coupled system results are also compared to corresponding exact results obtained using a harmonic oscillator basis, and also to approximate results obtained using first-order perturbation theory up to the maximum dimensionality for which the latter may be feasibly obtained (four dimensions).

Accurate quantum dynamics calculations using symmetrized Gaussians on a doubly dense Von Neumann lattice

Energy Technology Data Exchange (ETDEWEB)

Halverson, Thomas; Poirier, Bill [Department of Chemistry and Biochemistry and Department of Physics, Texas Tech University, P.O. Box 41061, Lubbock, Texas 79409-1061 (United States)

2012-12-14

In a series of earlier articles [B. Poirier, J. Theor. Comput. Chem. 2, 65 (2003); B. Poirier and A. Salam, J. Chem. Phys. 121, 1690 (2004); and ibid. 121, 1704 (2004)], a new method was introduced for performing exact quantum dynamics calculations. The method uses a 'weylet' basis set (orthogonalized Weyl-Heisenberg wavelets) combined with phase space truncation, to defeat the exponential scaling of CPU effort with system dimensionality-the first method ever able to achieve this long-standing goal. Here, we develop another such method, which uses a much more convenient basis of momentum-symmetrized Gaussians. Despite being non-orthogonal, symmetrized Gaussians are collectively local, allowing for effective phase space truncation. A dimension-independent code for computing energy eigenstates of both coupled and uncoupled systems has been created, exploiting massively parallel algorithms. Results are presented for model isotropic uncoupled harmonic oscillators and coupled anharmonic oscillators up to 27 dimensions. These are compared with the previous weylet calculations (uncoupled harmonic oscillators up to 15 dimensions), and found to be essentially just as efficient. Coupled system results are also compared to corresponding exact results obtained using a harmonic oscillator basis, and also to approximate results obtained using first-order perturbation theory up to the maximum dimensionality for which the latter may be feasibly obtained (four dimensions).

Methods for accurate calculations in high-energy quantum electrodynamics

Energy Technology Data Exchange (ETDEWEB)

Ericsson, K. E. [Institute of Theoretical Physics, Uppsala (Sweden)

1963-01-15

In this paper ''quantum electrodynamics'' (QED) will be used in the sense of a closed theory of point-like photons and electrons. Muons could then easily be included. We make the usual assumption that the perturbation expansion of renormalized QED gives at least an asymptotic expression of the exact theory, i.e. that the sum over a few terms in the beginning of the perturbation series is a good approximation of the exact theory. We expect QED in this sense to break down at small distances, i. e. at large momentum transfers, because of structure effects resulting from other kinds of interaction, primarily the interactions of the electromagnetic field with the current of strongly interacting particles. This will first show up as vacuum polarization through mesons. On the other hand we have no reason to believe that the fundamental theory of electrodynamics, i.e. the theory of a massless vector field interacting with a.conserved current, will break down.

Quantum Monte Carlo Calculations Applied to Magnetic Molecules

Energy Technology Data Exchange (ETDEWEB)

Engelhardt, Larry [Iowa State Univ., Ames, IA (United States)

2006-01-01

We have calculated the equilibrium thermodynamic properties of Heisenberg spin systems using a quantum Monte Carlo (QMC) method. We have used some of these systems as models to describe recently synthesized magnetic molecules, and-upon comparing the results of these calculations with experimental data-have obtained accurate estimates for the basic parameters of these models. We have also performed calculations for other systems that are of more general interest, being relevant both for existing experimental data and for future experiments. Utilizing the concept of importance sampling, these calculations can be carried out in an arbitrarily large quantum Hilbert space, while still avoiding any approximations that would introduce systematic errors. The only errors are statistical in nature, and as such, their magnitudes are accurately estimated during the course of a simulation. Frustrated spin systems present a major challenge to the QMC method, nevertheless, in many instances progress can be made. In this chapter, the field of magnetic molecules is introduced, paying particular attention to the characteristics that distinguish magnetic molecules from other systems that are studied in condensed matter physics. We briefly outline the typical path by which we learn about magnetic molecules, which requires a close relationship between experiments and theoretical calculations. The typical experiments are introduced here, while the theoretical methods are discussed in the next chapter. Each of these theoretical methods has a considerable limitation, also described in Chapter 2, which together serve to motivate the present work. As is shown throughout the later chapters, the present QMC method is often able to provide useful information where other methods fail. In Chapter 3, the use of Monte Carlo methods in statistical physics is reviewed, building up the fundamental ideas that are necessary in order to understand the method that has been used in this work. With these

Quantum Monte Carlo Calculations Applied to Magnetic Molecules

International Nuclear Information System (INIS)

Larry Engelhardt

2006-01-01

We have calculated the equilibrium thermodynamic properties of Heisenberg spin systems using a quantum Monte Carlo (QMC) method. We have used some of these systems as models to describe recently synthesized magnetic molecules, and-upon comparing the results of these calculations with experimental data-have obtained accurate estimates for the basic parameters of these models. We have also performed calculations for other systems that are of more general interest, being relevant both for existing experimental data and for future experiments. Utilizing the concept of importance sampling, these calculations can be carried out in an arbitrarily large quantum Hilbert space, while still avoiding any approximations that would introduce systematic errors. The only errors are statistical in nature, and as such, their magnitudes are accurately estimated during the course of a simulation. Frustrated spin systems present a major challenge to the QMC method, nevertheless, in many instances progress can be made. In this chapter, the field of magnetic molecules is introduced, paying particular attention to the characteristics that distinguish magnetic molecules from other systems that are studied in condensed matter physics. We briefly outline the typical path by which we learn about magnetic molecules, which requires a close relationship between experiments and theoretical calculations. The typical experiments are introduced here, while the theoretical methods are discussed in the next chapter. Each of these theoretical methods has a considerable limitation, also described in Chapter 2, which together serve to motivate the present work. As is shown throughout the later chapters, the present QMC method is often able to provide useful information where other methods fail. In Chapter 3, the use of Monte Carlo methods in statistical physics is reviewed, building up the fundamental ideas that are necessary in order to understand the method that has been used in this work. With these

ROLAIDS-CPM: A code for accurate resonance absorption calculations

International Nuclear Information System (INIS)

Kruijf, W.J.M. de.

1993-08-01

ROLAIDS is used to calculate group-averaged cross sections for specific zones in a one-dimensional geometry. This report describes ROLAIDS-CPM which is an extended version of ROLAIDS. The main extension in ROLAIDS-CPM is the possibility to use the collision probability method for a slab- or cylinder-geometry instead of the less accurate interface-currents method. In this way accurate resonance absorption calculations can be performed with ROLAIDS-CPM. ROLAIDS-CPM has been developed at ECN. (orig.)

Numerical renormalization group calculation of impurity internal energy and specific heat of quantum impurity models

Science.gov (United States)

Merker, L.; Costi, T. A.

2012-08-01

We introduce a method to obtain the specific heat of quantum impurity models via a direct calculation of the impurity internal energy requiring only the evaluation of local quantities within a single numerical renormalization group (NRG) calculation for the total system. For the Anderson impurity model we show that the impurity internal energy can be expressed as a sum of purely local static correlation functions and a term that involves also the impurity Green function. The temperature dependence of the latter can be neglected in many cases, thereby allowing the impurity specific heat Cimp to be calculated accurately from local static correlation functions; specifically via Cimp=(∂Eionic)/(∂T)+(1)/(2)(∂Ehyb)/(∂T), where Eionic and Ehyb are the energies of the (embedded) impurity and the hybridization energy, respectively. The term involving the Green function can also be evaluated in cases where its temperature dependence is non-negligible, adding an extra term to Cimp. For the nondegenerate Anderson impurity model, we show by comparison with exact Bethe ansatz calculations that the results recover accurately both the Kondo induced peak in the specific heat at low temperatures as well as the high-temperature peak due to the resonant level. The approach applies to multiorbital and multichannel Anderson impurity models with arbitrary local Coulomb interactions. An application to the Ohmic two-state system and the anisotropic Kondo model is also given, with comparisons to Bethe ansatz calculations. The approach could also be of interest within other impurity solvers, for example, within quantum Monte Carlo techniques.

Continuum variational and diffusion quantum Monte Carlo calculations

International Nuclear Information System (INIS)

Needs, R J; Towler, M D; Drummond, N D; Lopez RIos, P

2010-01-01

This topical review describes the methodology of continuum variational and diffusion quantum Monte Carlo calculations. These stochastic methods are based on many-body wavefunctions and are capable of achieving very high accuracy. The algorithms are intrinsically parallel and well suited to implementation on petascale computers, and the computational cost scales as a polynomial in the number of particles. A guide to the systems and topics which have been investigated using these methods is given. The bulk of the article is devoted to an overview of the basic quantum Monte Carlo methods, the forms and optimization of wavefunctions, performing calculations under periodic boundary conditions, using pseudopotentials, excited-state calculations, sources of calculational inaccuracy, and calculating energy differences and forces. (topical review)

Matrix product state calculations for one-dimensional quantum chains and quantum impurity models

Energy Technology Data Exchange (ETDEWEB)

Muender, Wolfgang

2011-09-28

involving a Kondo exciton and population switching in quantum dots. It turns out that both phenomena rely on the various manifestations of Anderson orthogonality (AO), which describes the fact that the response of the Fermi sea to a quantum quench (i.e. an abrupt change of some property of the impurity or quantum dot) is a change of the scattering phase shifts of all the single-particle wave functions, therefore drastically changing the system. In this context, we demonstrate that NRG, a highly accurate method for quantum impurity models, allows for the calculation of all static and dynamic quantities related to AO and present an extensive NRG study for population switching in quantum dots. (orig.)

Matrix product state calculations for one-dimensional quantum chains and quantum impurity models

International Nuclear Information System (INIS)

Muender, Wolfgang

2011-01-01

involving a Kondo exciton and population switching in quantum dots. It turns out that both phenomena rely on the various manifestations of Anderson orthogonality (AO), which describes the fact that the response of the Fermi sea to a quantum quench (i.e. an abrupt change of some property of the impurity or quantum dot) is a change of the scattering phase shifts of all the single-particle wave functions, therefore drastically changing the system. In this context, we demonstrate that NRG, a highly accurate method for quantum impurity models, allows for the calculation of all static and dynamic quantities related to AO and present an extensive NRG study for population switching in quantum dots. (orig.)

On the validity of microscopic calculations of double-quantum-dot spin qubits based on Fock-Darwin states

Science.gov (United States)

Chan, GuoXuan; Wang, Xin

2018-04-01

We consider two typical approximations that are used in the microscopic calculations of double-quantum dot spin qubits, namely, the Heitler-London (HL) and the Hund-Mulliken (HM) approximations, which use linear combinations of Fock-Darwin states to approximate the two-electron states under the double-well confinement potential. We compared these results to a case in which the solution to a one-dimensional Schr¨odinger equation was exactly known and found that typical microscopic calculations based on Fock-Darwin states substantially underestimate the value of the exchange interaction, which is the key parameter that controls the quantum dot spin qubits. This underestimation originates from the lack of tunneling of Fock-Darwin states, which is accurate only in the case with a single potential well. Our results suggest that the accuracies of the current two-dimensional molecular- orbit-theoretical calculations based on Fock-Darwin states should be revisited since underestimation could only deteriorate in dimensions that are higher than one.

How Accurately can we Calculate Thermal Systems?

International Nuclear Information System (INIS)

Cullen, D; Blomquist, R N; Dean, C; Heinrichs, D; Kalugin, M A; Lee, M; Lee, Y; MacFarlan, R; Nagaya, Y; Trkov, A

2004-01-01

I would like to determine how accurately a variety of neutron transport code packages (code and cross section libraries) can calculate simple integral parameters, such as K eff , for systems that are sensitive to thermal neutron scattering. Since we will only consider theoretical systems, we cannot really determine absolute accuracy compared to any real system. Therefore rather than accuracy, it would be more precise to say that I would like to determine the spread in answers that we obtain from a variety of code packages. This spread should serve as an excellent indicator of how accurately we can really model and calculate such systems today. Hopefully, eventually this will lead to improvements in both our codes and the thermal scattering models that they use in the future. In order to accomplish this I propose a number of extremely simple systems that involve thermal neutron scattering that can be easily modeled and calculated by a variety of neutron transport codes. These are theoretical systems designed to emphasize the effects of thermal scattering, since that is what we are interested in studying. I have attempted to keep these systems very simple, and yet at the same time they include most, if not all, of the important thermal scattering effects encountered in a large, water-moderated, uranium fueled thermal system, i.e., our typical thermal reactors

Accounting for Interference, Scattering, and Electrode Absorption to Make Accurate Internal Quantum Efficiency Measurements in Organic and Other Thin Solar Cells

KAUST Repository

Burkhard, George F.; Hoke, Eric T.; McGehee, Michael D.

2010-01-01

Accurately measuring internal quantum efficiency requires knowledge of absorption in the active layer of a solar cell. The experimentally accessible total absorption includes significant contributions from the electrodes and other nonactive layers. We suggest a straightforward method for calculating the active layer contribution that minimizes error by subtracting optically-modeled electrode absorption from experimentally measured total absorption. (Figure Presented) © 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Accounting for Interference, Scattering, and Electrode Absorption to Make Accurate Internal Quantum Efficiency Measurements in Organic and Other Thin Solar Cells

KAUST Repository

Burkhard, George F.

2010-05-31

Accurately measuring internal quantum efficiency requires knowledge of absorption in the active layer of a solar cell. The experimentally accessible total absorption includes significant contributions from the electrodes and other nonactive layers. We suggest a straightforward method for calculating the active layer contribution that minimizes error by subtracting optically-modeled electrode absorption from experimentally measured total absorption. (Figure Presented) © 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Methods for Efficiently and Accurately Computing Quantum Mechanical Free Energies for Enzyme Catalysis.

Science.gov (United States)

Kearns, F L; Hudson, P S; Boresch, S; Woodcock, H L

2016-01-01

Enzyme activity is inherently linked to free energies of transition states, ligand binding, protonation/deprotonation, etc.; these free energies, and thus enzyme function, can be affected by residue mutations, allosterically induced conformational changes, and much more. Therefore, being able to predict free energies associated with enzymatic processes is critical to understanding and predicting their function. Free energy simulation (FES) has historically been a computational challenge as it requires both the accurate description of inter- and intramolecular interactions and adequate sampling of all relevant conformational degrees of freedom. The hybrid quantum mechanical molecular mechanical (QM/MM) framework is the current tool of choice when accurate computations of macromolecular systems are essential. Unfortunately, robust and efficient approaches that employ the high levels of computational theory needed to accurately describe many reactive processes (ie, ab initio, DFT), while also including explicit solvation effects and accounting for extensive conformational sampling are essentially nonexistent. In this chapter, we will give a brief overview of two recently developed methods that mitigate several major challenges associated with QM/MM FES: the QM non-Boltzmann Bennett's acceptance ratio method and the QM nonequilibrium work method. We will also describe usage of these methods to calculate free energies associated with (1) relative properties and (2) along reaction paths, using simple test cases with relevance to enzymes examples. © 2016 Elsevier Inc. All rights reserved.

Approximate calculation of electronic energy levels of axially symmetric quantum dot and quantum ring by using energy dependent effective mass

International Nuclear Information System (INIS)

Yu-Min, Liu; Zhong-Yuan, Yu; Xiao-Min, Ren

2009-01-01

Calculations of electronic structures about the semiconductor quantum dot and the semiconductor quantum ring are presented in this paper. To reduce the calculation costs, for the quantum dot and the quantum ring, their simplified axially symmetric shapes are utilized in our analysis. The energy dependent effective mass is taken into account in solving the Schrödinger equations in the single band effective mass approximation. The calculated results show that the energy dependent effective mass should be considered only for relatively small volume quantum dots or small quantum rings. For large size quantum materials, both the energy dependent effective mass and the parabolic effective mass can give the same results. The energy states and the effective masses of the quantum dot and the quantum ring as a function of geometric parameters are also discussed in detail. (general)

Fast and accurate inductance and coupling calculation for a multi-layer Nb process

International Nuclear Information System (INIS)

Fourie, Coenrad J; Takahashi, Akitomo; Yoshikawa, Nobuyuki

2015-01-01

Currently, fabrication processes for superconductive integrated circuits are moving to multiple wiring and shielding layers, some of which are placed below the main ground plane (GP) and device layers. The Advanced Industrial Science and Technology advanced process (ADP2) was the first such multi-layer Nb process with planarized passive transmission line and GP layers below the junction layer, and is at the time of writing still the most developed. This process allows complex circuit designs, and accurate inductance extraction helps to push the boundaries of the layouts possible. We show that the position of ground connections between ground layers influences the inductance of structures for which these GPs act as return path, and that this needs to be accounted for in modelling. However, due to the number of wiring layers and GPs, full layout modelling of large cells causes long calculation times. In this paper we discuss methods with which to reduce model size, and calibrate InductEx calculations using these methods against measured results. We show that model reduction followed by calibration results in fast calculation times while good accuracy is maintained. We also show that InductEx correctly handles coupling between conductors in a multi-layer layout, and how to model layouts to gauge unwanted coupling between power lines and single flux quantum electronics. (paper)

Bridging quantum chemistry and nuclear structure theory: Coupled-cluster calculations for closed- and open-shell nuclei

International Nuclear Information System (INIS)

Piecuch, Piotr; Wloch, Marta; Gour, Jeffrey R.; Dean, David J.; Papenbrock, Thomas; Hjorth-Jensen, Morten

2005-01-01

We review basic elements of the single-reference coupled-cluster theory and discuss large scale ab initio calculations of ground and excited states of 15O, 16O, and 17O using coupled-cluster methods and algorithms developed in quantum chemistry. By using realistic two-body interactions and the renormalized form of the Hamiltonian obtained with a no-core G-matrix approach, we obtain the converged results for 16O and promising preliminary results for 15O and 17O at the level of two-body interactions. The calculated properties other than energies include matter density, charge radius, and charge form factor. The relatively low costs of coupled-cluster calculations, which are characterized by the low-order polynomial scaling with the system size, enable us to probe large model spaces with up to 7 or 8 major oscillator shells, for which non-truncated shell-model calculations for nuclei with A = 15 17 active particles are presently not possible. We argue that the use of coupled-cluster methods and computer algorithms developed by quantum chemists to calculate properties of nuclei is an important step toward the development of accurate and affordable many-body theories that cross the boundaries of various physical sciences

molecular dynamics simulations and quantum chemical calculations

African Journals Online (AJOL)

ABSTRACT. The molecular dynamic (MD) simulation and quantum chemical calculations for the adsorption of [2-(2-Henicos-10- .... electronic properties of molecule clusters, surfaces and ... The local reactivity was analyzed by determining the.

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

Energy Technology Data Exchange (ETDEWEB)

Pavanello, Michele [Department of Chemistry, Rutgers University, Newark, New Jersey 07102-1811 (United States); Van Voorhis, Troy [Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139-4307 (United States); Visscher, Lucas [Amsterdam Center for Multiscale Modeling, VU University, De Boelelaan 1083, 1081 HV Amsterdam (Netherlands); Neugebauer, Johannes [Theoretische Organische Chemie, Organisch-Chemisches Institut der Westfaelischen Wilhelms-Universitaet Muenster, Corrensstrasse 40, 48149 Muenster (Germany)

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 Angstroms. Numerical examples are provided for molecular clusters comprised of up to 56 non-covalently bound molecules.

Spectral neighbor analysis method for automated generation of quantum-accurate interatomic potentials

International Nuclear Information System (INIS)

Thompson, A.P.; Swiler, L.P.; Trott, C.R.; Foiles, S.M.; Tucker, G.J.

2015-01-01

We present a new interatomic potential for solids and liquids called Spectral Neighbor Analysis Potential (SNAP). The SNAP potential has a very general form and uses machine-learning techniques to reproduce the energies, forces, and stress tensors of a large set of small configurations of atoms, which are obtained using high-accuracy quantum electronic structure (QM) calculations. The local environment of each atom is characterized by a set of bispectrum components of the local neighbor density projected onto a basis of hyperspherical harmonics in four dimensions. The bispectrum components are the same bond-orientational order parameters employed by the GAP potential [1]. The SNAP potential, unlike GAP, assumes a linear relationship between atom energy and bispectrum components. The linear SNAP coefficients are determined using weighted least-squares linear regression against the full QM training set. This allows the SNAP potential to be fit in a robust, automated manner to large QM data sets using many bispectrum components. The calculation of the bispectrum components and the SNAP potential are implemented in the LAMMPS parallel molecular dynamics code. We demonstrate that a previously unnoticed symmetry property can be exploited to reduce the computational cost of the force calculations by more than one order of magnitude. We present results for a SNAP potential for tantalum, showing that it accurately reproduces a range of commonly calculated properties of both the crystalline solid and the liquid phases. In addition, unlike simpler existing potentials, SNAP correctly predicts the energy barrier for screw dislocation migration in BCC tantalum

Spectral neighbor analysis method for automated generation of quantum-accurate interatomic potentials

Energy Technology Data Exchange (ETDEWEB)

Thompson, Aidan P. [Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States). Multiscale Science Dept.; Swiler, Laura P. [Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States). Optimization and Uncertainty Quantification Dept.; Trott, Christian R. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Scalable Algorithms Dept.; Foiles, Stephen M. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Computational Materials and Data Science Dept.; Tucker, Garritt J. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Computational Materials and Data Science Dept.; Drexel Univ., Philadelphia, PA (United States). Dept. of Materials Science and Engineering

2015-03-15

Here, we present a new interatomic potential for solids and liquids called Spectral Neighbor Analysis Potential (SNAP). The SNAP potential has a very general form and uses machine-learning techniques to reproduce the energies, forces, and stress tensors of a large set of small configurations of atoms, which are obtained using high-accuracy quantum electronic structure (QM) calculations. The local environment of each atom is characterized by a set of bispectrum components of the local neighbor density projected onto a basis of hyperspherical harmonics in four dimensions. The bispectrum components are the same bond-orientational order parameters employed by the GAP potential [1]. The SNAP potential, unlike GAP, assumes a linear relationship between atom energy and bispectrum components. The linear SNAP coefficients are determined using weighted least-squares linear regression against the full QM training set. This allows the SNAP potential to be fit in a robust, automated manner to large QM data sets using many bispectrum components. The calculation of the bispectrum components and the SNAP potential are implemented in the LAMMPS parallel molecular dynamics code. We demonstrate that a previously unnoticed symmetry property can be exploited to reduce the computational cost of the force calculations by more than one order of magnitude. We present results for a SNAP potential for tantalum, showing that it accurately reproduces a range of commonly calculated properties of both the crystalline solid and the liquid phases. In addition, unlike simpler existing potentials, SNAP correctly predicts the energy barrier for screw dislocation migration in BCC tantalum.

Spectral neighbor analysis method for automated generation of quantum-accurate interatomic potentials

Energy Technology Data Exchange (ETDEWEB)

Thompson, A.P., E-mail: athomps@sandia.gov [Multiscale Science Department, Sandia National Laboratories, PO Box 5800, MS 1322, Albuquerque, NM 87185 (United States); Swiler, L.P., E-mail: lpswile@sandia.gov [Optimization and Uncertainty Quantification Department, Sandia National Laboratories, PO Box 5800, MS 1318, Albuquerque, NM 87185 (United States); Trott, C.R., E-mail: crtrott@sandia.gov [Scalable Algorithms Department, Sandia National Laboratories, PO Box 5800, MS 1322, Albuquerque, NM 87185 (United States); Foiles, S.M., E-mail: foiles@sandia.gov [Computational Materials and Data Science Department, Sandia National Laboratories, PO Box 5800, MS 1411, Albuquerque, NM 87185 (United States); Tucker, G.J., E-mail: gtucker@coe.drexel.edu [Computational Materials and Data Science Department, Sandia National Laboratories, PO Box 5800, MS 1411, Albuquerque, NM 87185 (United States); Department of Materials Science and Engineering, Drexel University, Philadelphia, PA 19104 (United States)

2015-03-15

We present a new interatomic potential for solids and liquids called Spectral Neighbor Analysis Potential (SNAP). The SNAP potential has a very general form and uses machine-learning techniques to reproduce the energies, forces, and stress tensors of a large set of small configurations of atoms, which are obtained using high-accuracy quantum electronic structure (QM) calculations. The local environment of each atom is characterized by a set of bispectrum components of the local neighbor density projected onto a basis of hyperspherical harmonics in four dimensions. The bispectrum components are the same bond-orientational order parameters employed by the GAP potential [1]. The SNAP potential, unlike GAP, assumes a linear relationship between atom energy and bispectrum components. The linear SNAP coefficients are determined using weighted least-squares linear regression against the full QM training set. This allows the SNAP potential to be fit in a robust, automated manner to large QM data sets using many bispectrum components. The calculation of the bispectrum components and the SNAP potential are implemented in the LAMMPS parallel molecular dynamics code. We demonstrate that a previously unnoticed symmetry property can be exploited to reduce the computational cost of the force calculations by more than one order of magnitude. We present results for a SNAP potential for tantalum, showing that it accurately reproduces a range of commonly calculated properties of both the crystalline solid and the liquid phases. In addition, unlike simpler existing potentials, SNAP correctly predicts the energy barrier for screw dislocation migration in BCC tantalum.

Energetics and stability of azulene: From experimental thermochemistry to high-level quantum chemical calculations

International Nuclear Information System (INIS)

Sousa, Clara C.S.; Matos, M. Agostinha R.; Morais, Victor M.F.

2014-01-01

Highlights: • Experimental standard molar enthalpy of formation, sublimation azulene. • Mini-bomb combustion calorimetry, sublimation Calvet microcalorimetry. • High level composite ab initio calculations. • Computational estimate of the enthalpy of formation of azulene. • Discussion of stability and aromaticity of azulene. - Abstract: The standard (p 0 = 0.1 MPa) molar enthalpy of formation for crystalline azulene was derived from the standard molar enthalpy of combustion, in oxygen, at T = 298.15 K, measured in a mini-bomb combustion calorimeter (aneroid isoperibol calorimeter) and the standard molar enthalpy of sublimation, at T = 298.15 K, measured by Calvet microcalorimetry. From these experiments, the standard molar enthalpy of formation of azulene in the gaseous phase at T = 298.15 K was calculated. In addition, very accurate quantum chemical calculations at the G3 and G4 composite levels of calculation were conducted in order to corroborate our experimental findings and further clarify and establish the definitive standard enthalpy of formation of this interesting non-benzenoid hydrocarbon

Application of dynamic pseudo fission products and actinides for accurate burnup calculations

Energy Technology Data Exchange (ETDEWEB)

Hoogenboom, J.E.; Leege, P.F.A. de [Technische Univ. Delft (Netherlands). Interfacultair Reactor Inst.; Kloosterman, J.L.

1996-09-01

The introduction of pseudo fission products for accurate fine-group spectrum calculations during burnup is discussed. The calculation of the density of the pseudo nuclides is done before each spectrum calculation from the actual densities and their cross sections of all nuclides to be lumped into a pseudo fission product. As there are also many actinides formed in the fuel during its life cycle, a pseudo actinide with fission cross section is also introduced. From a realistic burnup calculation it is demonstrated that only a few fission products and actinides need to be included explicitly in a spectrum calculation. All other fission products and actinides can be accurately represented in the pseudo nuclides. (author)

Low-Mode Conformational Search Method with Semiempirical Quantum Mechanical Calculations: Application to Enantioselective Organocatalysis.

Science.gov (United States)

Kamachi, Takashi; Yoshizawa, Kazunari

2016-02-22

A conformational search program for finding low-energy conformations of large noncovalent complexes has been developed. A quantitatively reliable semiempirical quantum mechanical PM6-DH+ method, which is able to accurately describe noncovalent interactions at a low computational cost, was employed in contrast to conventional conformational search programs in which molecular mechanical methods are usually adopted. Our approach is based on the low-mode method whereby an initial structure is perturbed along one of its low-mode eigenvectors to generate new conformations. This method was applied to determine the most stable conformation of transition state for enantioselective alkylation by the Maruoka and cinchona alkaloid catalysts and Hantzsch ester hydrogenation of imines by chiral phosphoric acid. Besides successfully reproducing the previously reported most stable DFT conformations, the conformational search with the semiempirical quantum mechanical calculations newly discovered a more stable conformation at a low computational cost.

Introduction to quantum calculation methods in high resolution NMR

International Nuclear Information System (INIS)

Goldman, M.

1996-01-01

New techniques as for instance the polarization transfer, the coherence with several quanta and the double Fourier transformation have appeared fifteen years ago. These techniques constitute a considerable advance in NMR. Indeed, they allow to study more complex molecules than it was before possible. But with these advances, the classical description of the NMR is not enough to understand precisely the physical phenomena induced by these methods. It is then necessary to resort to quantum calculation methods. The aim of this work is to present these calculation methods. After some recalls of quantum mechanics, the author describes the NMR with the density matrix, reviews the main methods of double Fourier transformation and then gives the principle of the relaxation times calculation. (O.M.)

Quantum Chemistry on Quantum Computers: A Polynomial-Time Quantum Algorithm for Constructing the Wave Functions of Open-Shell Molecules.

Science.gov (United States)

Sugisaki, Kenji; Yamamoto, Satoru; Nakazawa, Shigeaki; Toyota, Kazuo; Sato, Kazunobu; Shiomi, Daisuke; Takui, Takeji

2016-08-18

Quantum computers are capable to efficiently perform full configuration interaction (FCI) calculations of atoms and molecules by using the quantum phase estimation (QPE) algorithm. Because the success probability of the QPE depends on the overlap between approximate and exact wave functions, efficient methods to prepare accurate initial guess wave functions enough to have sufficiently large overlap with the exact ones are highly desired. Here, we propose a quantum algorithm to construct the wave function consisting of one configuration state function, which is suitable for the initial guess wave function in QPE-based FCI calculations of open-shell molecules, based on the addition theorem of angular momentum. The proposed quantum algorithm enables us to prepare the wave function consisting of an exponential number of Slater determinants only by a polynomial number of quantum operations.

Full-Dimensional Quantum Calculations of Vibrational Levels of NH4(+) and Isotopomers on An Accurate Ab Initio Potential Energy Surface.

Science.gov (United States)

Yu, Hua-Gen; Han, Huixian; Guo, Hua

2016-04-14

Vibrational energy levels of the ammonium cation (NH4(+)) and its deuterated isotopomers are calculated using a numerically exact kinetic energy operator on a recently developed nine-dimensional permutation invariant semiglobal potential energy surface fitted to a large number of high-level ab initio points. Like CH4, the vibrational levels of NH4(+) and ND4(+) exhibit a polyad structure, characterized by a collective quantum number P = 2(v1 + v3) + v2 + v4. The low-lying vibrational levels of all isotopomers are assigned and the agreement with available experimental data is better than 1 cm(-1).

Quantum complex rotation and uniform semiclassical calculations of complex energy eigenvalues

International Nuclear Information System (INIS)

Connor, J.N.L.; Smith, A.D.

1983-01-01

Quantum and semiclassical calculations of complex energy eigenvalues have been carried out for an exponential potential of the form V 0 r 2 exp(-r) and Lennard-Jones (12,6) potential. A straightforward method, based on the complex coordinate rotation technique, is described for the quantum calculation of complex eigenenergies. For singular potentials, the method involves an inward and outward integration of the radial Schroedinger equation, followed by matching of the logarithmic derivatives of the wave functions at an intermediate point. For regular potentials, the method is simpler, as only an inward integration is required. Attention is drawn to the World War II researches of Hartree and co-workers who anticipated later quantum mechanical work on the complex rotation method. Complex eigenenergies are also calculated from a uniform semiclassical three turning point quantization formula, which allows for the proximity of the outer pair of complex turning points. Limiting cases of this formula, which are valid for very narrow or very broad widths, are also used in the calculations. We obtain good agreement between the semiclassical and quantum results. For the Lennard-Jones (12,6) potential, we compare resonance energies and widths from the complex energy definition of a resonance with those obtained from the time delay definition

Communication: Calculation of interatomic forces and optimization of molecular geometry with auxiliary-field quantum Monte Carlo

Science.gov (United States)

Motta, Mario; Zhang, Shiwei

2018-05-01

We propose an algorithm for accurate, systematic, and scalable computation of interatomic forces within the auxiliary-field quantum Monte Carlo (AFQMC) method. The algorithm relies on the Hellmann-Feynman theorem and incorporates Pulay corrections in the presence of atomic orbital basis sets. We benchmark the method for small molecules by comparing the computed forces with the derivatives of the AFQMC potential energy surface and by direct comparison with other quantum chemistry methods. We then perform geometry optimizations using the steepest descent algorithm in larger molecules. With realistic basis sets, we obtain equilibrium geometries in agreement, within statistical error bars, with experimental values. The increase in computational cost for computing forces in this approach is only a small prefactor over that of calculating the total energy. This paves the way for a general and efficient approach for geometry optimization and molecular dynamics within AFQMC.

An Accurate Technique for Calculation of Radiation From Printed Reflectarrays

DEFF Research Database (Denmark)

Zhou, Min; Sorensen, Stig B.; Jorgensen, Erik

2011-01-01

The accuracy of various techniques for calculating the radiation from printed reflectarrays is examined, and an improved technique based on the equivalent currents approach is proposed. The equivalent currents are found from a continuous plane wave spectrum calculated by use of the spectral dyadic...... Green's function. This ensures a correct relation between the equivalent electric and magnetic currents and thus allows an accurate calculation of the radiation over the entire far-field sphere. A comparison to DTU-ESA Facility measurements of a reference offset reflectarray designed and manufactured...

Accurate calculation of the differential cross section of compton scattering with electron mixed chain propagator in SM

International Nuclear Information System (INIS)

Chen Xuewen; Fang Zhenyun; Shi Chengye

2012-01-01

By using the electroweak standard model (SM), we analyzed the framework of electron mixed chain propagator which composed of serious of different physical loops participating in electroweak interaction and completed the relevant analytical calculation. Then, we obtained the analytical result of electron mixed chain propagator. By applying our result to Compton scattering, the differential cross section of Compton scattering dσ SM (chain) /dcosθ is counted accurately. This result is compared with the lowest order differential cross section dσ (tree) /dcosθ and the electronic chain propagator Compton scattering differential cross section dσ QED (chain) /dcosθ in quantum electrodynamics (QED). It can be seen that dσ SM (chain ) /dcosθ can show the radiation correction more subtly than dσ QED (chain) /dcosθ. (authors)

Quantum mechanical calculation of diffusion of hydrogen isotopes in vanadium

International Nuclear Information System (INIS)

Yoshinari, Osamu

2013-01-01

Highlights: • Diffusion of H isotopes in V was investigated with a quantum mechanical calculation. • Calculated diffusion coefficients quantitatively agreed with the experimental data. • H in V jumps via quantum mechanical tunneling between the two tetrahedral sites. • H tunneling between ground states is dominant at low temperatures. • H tunneling between exited states becomes important at higher temperatures. -- Abstract: Diffusion of hydrogen isotopes in vanadium was investigated by a quantum mechanical calculation. Wave functions and the corresponding eigen energies (E) for hydrogen isotopes were obtained as a function of hydrogen position along the diffusion path (ξ) by solving the three dimensional Schrödinger equation. Hydrogen potential was calculated by using a first principles method with a nudged elastic band technique. By analyzing the E–ξ curves, the tunneling matrix elements were obtained for the coincidence states between two neighboring tetrahedral sites. It was clarified that the tunneling between ground states was dominant at low temperatures, whereas the contribution of that between the first exited states becomes larger at higher temperatures. The transition temperature of the dominant tunneling decreases with the isotope mass. The calculated temperature dependence of the diffusion for the V–H system quantitatively agreed with the experimental data in the literature, although those for the V–D and –T systems were somewhat underestimated

Using quantum chemistry muscle to flex massive systems: How to respond to something perturbing

Energy Technology Data Exchange (ETDEWEB)

Bertoni, Colleen [Iowa State Univ., Ames, IA (United States)

2016-12-17

Computational chemistry uses the theoretical advances of quantum mechanics and the algorithmic and hardware advances of computer science to give insight into chemical problems. It is currently possible to do highly accurate quantum chemistry calculations, but the most accurate methods are very computationally expensive. Thus it is only feasible to do highly accurate calculations on small molecules, since typically more computationally efficient methods are also less accurate. The overall goal of my dissertation work has been to try to decrease the computational expense of calculations without decreasing the accuracy. In particular, my dissertation work focuses on fragmentation methods, intermolecular interactions methods, analytic gradients, and taking advantage of new hardware.

Increasing the efficiency and accuracy of time-resolved electronic spectra calculations with on-the-fly ab initio quantum dynamics methods

Science.gov (United States)

Vanicek, Jiri

2014-03-01

Rigorous quantum-mechanical calculations of coherent ultrafast electronic spectra remain difficult. I will present several approaches developed in our group that increase the efficiency and accuracy of such calculations: First, we justified the feasibility of evaluating time-resolved spectra of large systems by proving that the number of trajectories needed for convergence of the semiclassical dephasing representation/phase averaging is independent of dimensionality. Recently, we further accelerated this approximation with a cellular scheme employing inverse Weierstrass transform and optimal scaling of the cell size. The accuracy of potential energy surfaces was increased by combining the dephasing representation with accurate on-the-fly ab initio electronic structure calculations, including nonadiabatic and spin-orbit couplings. Finally, the inherent semiclassical approximation was removed in the exact quantum Gaussian dephasing representation, in which semiclassical trajectories are replaced by communicating frozen Gaussian basis functions evolving classically with an average Hamiltonian. Among other examples I will present an on-the-fly ab initio semiclassical dynamics calculation of the dispersed time-resolved stimulated emission spectrum of the 54-dimensional azulene. This research was supported by EPFL and by the Swiss National Science Foundation NCCR MUST (Molecular Ultrafast Science and Technology) and Grant No. 200021124936/1.

Benchmarking density-functional-theory calculations of rotational g tensors and magnetizabilities using accurate coupled-cluster calculations.

Science.gov (United States)

Lutnaes, Ola B; Teale, Andrew M; Helgaker, Trygve; Tozer, David J; Ruud, Kenneth; Gauss, Jürgen

2009-10-14

An accurate set of benchmark rotational g tensors and magnetizabilities are calculated using coupled-cluster singles-doubles (CCSD) theory and coupled-cluster single-doubles-perturbative-triples [CCSD(T)] theory, in a variety of basis sets consisting of (rotational) London atomic orbitals. The accuracy of the results obtained is established for the rotational g tensors by careful comparison with experimental data, taking into account zero-point vibrational corrections. After an analysis of the basis sets employed, extrapolation techniques are used to provide estimates of the basis-set-limit quantities, thereby establishing an accurate benchmark data set. The utility of the data set is demonstrated by examining a wide variety of density functionals for the calculation of these properties. None of the density-functional methods are competitive with the CCSD or CCSD(T) methods. The need for a careful consideration of vibrational effects is clearly illustrated. Finally, the pure coupled-cluster results are compared with the results of density-functional calculations constrained to give the same electronic density. The importance of current dependence in exchange-correlation functionals is discussed in light of this comparison.

Benchmarking quantum mechanical calculations with experimental NMR chemical shifts of 2-HADNT

Science.gov (United States)

Liu, Yuemin; Junk, Thomas; Liu, Yucheng; Tzeng, Nianfeng; Perkins, Richard

2015-04-01

In this study, both GIAO-DFT and GIAO-MP2 calculations of nuclear magnetic resonance (NMR) spectra were benchmarked with experimental chemical shifts. The experimental chemical shifts were determined experimentally for carbon-13 (C-13) of seven carbon atoms for the TNT degradation product 2-hydroxylamino-4,6-dinitrotoluene (2-HADNT). Quantum mechanics GIAO calculations were implemented using Becke-3-Lee-Yang-Parr (B3LYP) and other six hybrid DFT methods (Becke-1-Lee-Yang-Parr (B1LYP), Becke-half-and-half-Lee-Yang-Parr (BH and HLYP), Cohen-Handy-3-Lee-Yang-Parr (O3LYP), Coulomb-attenuating-B3LYP (CAM-B3LYP), modified-Perdew-Wang-91-Lee-Yang-Parr (mPW1LYP), and Xu-3-Lee-Yang-Parr (X3LYP)) which use the same correlation functional LYP. Calculation results showed that the GIAO-MP2 method gives the most accurate chemical shift values, and O3LYP method provides the best prediction of chemical shifts among the B3LYP and other five DFT methods. Three types of atomic partial charges, Mulliken (MK), electrostatic potential (ESP), and natural bond orbital (NBO), were also calculated using MP2/aug-cc-pVDZ method. A reasonable correlation was discovered between NBO partial charges and experimental chemical shifts of carbon-13 (C-13).

Nonperturbative calculation of symmetry breaking in quantum field theory

OpenAIRE

Bender, Carl M.; Milton, Kimball A.

1996-01-01

A new version of the delta expansion is presented, which, unlike the conventional delta expansion, can be used to do nonperturbative calculations in a self-interacting scalar quantum field theory having broken symmetry. We calculate the expectation value of the scalar field to first order in delta, where delta is a measure of the degree of nonlinearity in the interaction term.

Quantum mechanical calculations related to ionization and charge transfer in DNA

International Nuclear Information System (INIS)

Cauët, E; Liévin, J; Valiev, M; Weare, J H

2012-01-01

Ionization and charge migration in DNA play crucial roles in mechanisms of DNA damage caused by ionizing radiation, oxidizing agents and photo-irradiation. Therefore, an evaluation of the ionization properties of the DNA bases is central to the full interpretation and understanding of the elementary reactive processes that occur at the molecular level during the initial exposure and afterwards. Ab initio quantum mechanical (QM) methods have been successful in providing highly accurate evaluations of key parameters, such as ionization energies (IE) of DNA bases. Hence, in this study, we performed high-level QM calculations to characterize the molecular energy levels and potential energy surfaces, which shed light on ionization and charge migration between DNA bases. In particular, we examined the IEs of guanine, the most easily oxidized base, isolated and embedded in base clusters, and investigated the mechanism of charge migration over two and three stacked guanines. The IE of guanine in the human telomere sequence has also been evaluated. We report a simple molecular orbital analysis to explain how modifications in the base sequence are expected to change the efficiency of the sequence as a hole trap. Finally, the application of a hybrid approach combining quantum mechanics with molecular mechanics brings an interesting discussion as to how the native aqueous DNA environment affects the IE threshold of nucleobases.

Calculating Casimir energies in renormalizable quantum field theory

International Nuclear Information System (INIS)

Milton, Kimball A.

2003-01-01

Quantum vacuum energy has been known to have observable consequences since 1948 when Casimir calculated the force of attraction between parallel uncharged plates, a phenomenon confirmed experimentally with ever increasing precision. Casimir himself suggested that a similar attractive self-stress existed for a conducting spherical shell, but Boyer obtained a repulsive stress. Other geometries and higher dimensions have been considered over the years. Local effects, and divergences associated with surfaces and edges were studied by several authors. Quite recently, Graham et al. have reexamined such calculations, using conventional techniques of perturbative quantum field theory to remove divergences, and have suggested that previous self-stress results may be suspect. Here we show that the examples considered in their work are misleading; in particular, it is well known that in two space dimensions a circular boundary has a divergence in the Casimir energy for massless fields, while for general spatial dimension D not equal to an even integer the corresponding Casimir energy arising from massless fields interior and exterior to a hyperspherical shell is finite. It has also long been recognized that the Casimir energy for massive fields is divergent for curved boundaries. These conclusions are reinforced by a calculation of the relevant leading Feynman diagram in D and in three dimensions. There is therefore no doubt of the validity of the conventional finite Casimir calculations

Quantum-mechanical calculation of carrier distribution in MOS accumulation and strong inversion layers

Directory of Open Access Journals (Sweden)

Chien-Wei Lee

2013-10-01

Full Text Available We derive a statistical physics model of two-dimensional electron gas (2DEG and propose an accurate approximation method for calculating the quantum-mechanical effects of metal-oxide-semiconductor (MOS structure in accumulation and strong inversion regions. We use an exponential surface potential approximation in solving the quantization energy levels and derive the function of density of states in 2D to 3D transition region by applying uncertainty principle and Schrödinger equation in k-space. The simulation results show that our approximation method and theory of density of states solve the two major problems of previous researches: the non-negligible error caused by the linear potential approximation and the inconsistency of density of states and carrier distribution in 2D to 3D transition region.

Multiple environment single system quantum mechanical/molecular mechanical (MESS-QM/MM) calculations. 1. Estimation of polarization energies.

Science.gov (United States)

Sodt, Alexander J; Mei, Ye; König, Gerhard; Tao, Peng; Steele, Ryan P; Brooks, Bernard R; Shao, Yihan

2015-03-05

In combined quantum mechanical/molecular mechanical (QM/MM) free energy calculations, it is often advantageous to have a frozen geometry for the quantum mechanical (QM) region. For such multiple-environment single-system (MESS) cases, two schemes are proposed here for estimating the polarization energy: the first scheme, termed MESS-E, involves a Roothaan step extrapolation of the self-consistent field (SCF) energy; whereas the other scheme, termed MESS-H, employs a Newton-Raphson correction using an approximate inverse electronic Hessian of the QM region (which is constructed only once). Both schemes are extremely efficient, because the expensive Fock updates and SCF iterations in standard QM/MM calculations are completely avoided at each configuration. They produce reasonably accurate QM/MM polarization energies: MESS-E can predict the polarization energy within 0.25 kcal/mol in terms of the mean signed error for two of our test cases, solvated methanol and solvated β-alanine, using the M06-2X or ωB97X-D functionals; MESS-H can reproduce the polarization energy within 0.2 kcal/mol for these two cases and for the oxyluciferin-luciferase complex, if the approximate inverse electronic Hessians are constructed with sufficient accuracy.

Classical-quantum correspondence in electron-positron pair creation

International Nuclear Information System (INIS)

Chott, N. I.; Su, Q.; Grobe, R.

2007-01-01

We examine the creation of electron-positron pairs in a very strong force field. Using numerical solutions to quantum field theory we calculate the spatial and momentum probability distributions for the created particles. A comparison with classical mechanical phase space calculations suggests that despite the fully relativistic and quantum mechanical nature of the matter creation process, most aspects can be reproduced accurately in terms of classical mechanics

Performance test of multicomponent quantum mechanical calculation with polarizable continuum model for proton chemical shift.

Science.gov (United States)

Kanematsu, Yusuke; Tachikawa, Masanori

2015-05-21

Multicomponent quantum mechanical (MC_QM) calculations with polarizable continuum model (PCM) have been tested against liquid (1)H NMR chemical shifts for a test set of 80 molecules. Improvement from conventional quantum mechanical calculations was achieved for MC_QM calculations. The advantage of the multicomponent scheme could be attributed to the geometrical change from the equilibrium geometry by the incorporation of the hydrogen nuclear quantum effect, while that of PCM can be attributed to the change of the electronic structure according to the polarization by solvent effects.

Quantum Monte Carlo calculations with chiral effective field theory interactions

Energy Technology Data Exchange (ETDEWEB)

Tews, Ingo

2015-10-12

The neutron-matter equation of state connects several physical systems over a wide density range, from cold atomic gases in the unitary limit at low densities, to neutron-rich nuclei at intermediate densities, up to neutron stars which reach supranuclear densities in their core. An accurate description of the neutron-matter equation of state is therefore crucial to describe these systems. To calculate the neutron-matter equation of state reliably, precise many-body methods in combination with a systematic theory for nuclear forces are needed. Chiral effective field theory (EFT) is such a theory. It provides a systematic framework for the description of low-energy hadronic interactions and enables calculations with controlled theoretical uncertainties. Chiral EFT makes use of a momentum-space expansion of nuclear forces based on the symmetries of Quantum Chromodynamics, which is the fundamental theory of strong interactions. In chiral EFT, the description of nuclear forces can be systematically improved by going to higher orders in the chiral expansion. On the other hand, continuum Quantum Monte Carlo (QMC) methods are among the most precise many-body methods available to study strongly interacting systems at finite densities. They treat the Schroedinger equation as a diffusion equation in imaginary time and project out the ground-state wave function of the system starting from a trial wave function by propagating the system in imaginary time. To perform this propagation, continuum QMC methods require as input local interactions. However, chiral EFT, which is naturally formulated in momentum space, contains several sources of nonlocality. In this Thesis, we show how to construct local chiral two-nucleon (NN) and three-nucleon (3N) interactions and discuss results of first QMC calculations for pure neutron systems. We have performed systematic auxiliary-field diffusion Monte Carlo (AFDMC) calculations for neutron matter using local chiral NN interactions. By

Accurate alpha sticking fractions from improved calculations relevant for muon catalyzed fusion

International Nuclear Information System (INIS)

Szalewicz, K.

1990-05-01

Recent experiments have shown that under proper conditions a single muon may catalyze almost two hundred fusions in its lifetime. This process proceeds through formation of muonic molecular ions. Properties of these ions are central to the understanding of the phenomenon. Our work included the most accurate calculations of the energy levels and Coulombic sticking fractions for tdμ and other muonic molecular ions, calculations of Auger transition rates, calculations of corrections to the energy levels due to interactions with the most molecule, and calculation of the reactivation of muons from α particles. The majority of our effort has been devoted to the theory and computation of the influence of the strong nuclear forces on fusion rates and sticking fractions. We have calculated fusion rates for tdμ including the effects of nuclear forces on the molecular wave functions. We have also shown that these results can be reproduced to almost four digit accuracy by using a very simple quasifactorizable expression which does not require modifications of the molecular wave functions. Our sticking fractions are more accurate than any other theoretical values. We have used a more sophisticated theory than any other work and our numerical calculations have converged to at least three significant digits

Quantum chemical calculations of using density functional theory ...

Indian Academy of Sciences (India)

K RACKESH JAWAHER

2018-02-15

Feb 15, 2018 ... Quantum chemical calculations have been employed to study the molecular effects produced by. Cr2O3/SnO2 optimised structure. ... are exploited in solar cells [2], high-capacity lithium– storage [3], solid-state chemical ..... bond distance of metal–oxygen is positively (0.5 Е) deviated to oxygen–oxygen ...

Chemical Shifts of the Carbohydrate Binding Domain of Galectin-3 from Magic Angle Spinning NMR and Hybrid Quantum Mechanics/Molecular Mechanics Calculations.

Science.gov (United States)

Kraus, Jodi; Gupta, Rupal; Yehl, Jenna; Lu, Manman; Case, David A; Gronenborn, Angela M; Akke, Mikael; Polenova, Tatyana

2018-03-22

Magic angle spinning NMR spectroscopy is uniquely suited to probe the structure and dynamics of insoluble proteins and protein assemblies at atomic resolution, with NMR chemical shifts containing rich information about biomolecular structure. Access to this information, however, is problematic, since accurate quantum mechanical calculation of chemical shifts in proteins remains challenging, particularly for 15 N H . Here we report on isotropic chemical shift predictions for the carbohydrate recognition domain of microcrystalline galectin-3, obtained from using hybrid quantum mechanics/molecular mechanics (QM/MM) calculations, implemented using an automated fragmentation approach, and using very high resolution (0.86 Å lactose-bound and 1.25 Å apo form) X-ray crystal structures. The resolution of the X-ray crystal structure used as an input into the AF-NMR program did not affect the accuracy of the chemical shift calculations to any significant extent. Excellent agreement between experimental and computed shifts is obtained for 13 C α , while larger scatter is observed for 15 N H chemical shifts, which are influenced to a greater extent by electrostatic interactions, hydrogen bonding, and solvation.

The Strength of Chaos: Accurate Simulation of Resonant Electron Scattering by Many-Electron Ions and Atoms in the Presence of Quantum Chaos

Science.gov (United States)

2017-01-20

AFRL-AFOSR-JP-TR-2017-0012 The Strength of Chaos : accurate simulation of resonant electron scattering by many-electron ions and atoms in the presence...of quantum chaos Igor Bray CURTIN UNIVERSITY OF TECHNOLOGY Final Report 01/20/2017 DISTRIBUTION A: Distribution approved for public release. AF...SUBTITLE The Strength of Chaos : accurate simulation of resonant electron scattering by many- electron ions and atoms in the presence of quantum chaos

Quantum Monte Carlo calculations of light nuclei

International Nuclear Information System (INIS)

Pandharipande, V. R.

1999-01-01

Quantum Monte Carlo methods provide an essentially exact way to calculate various properties of nuclear bound, and low energy continuum states, from realistic models of nuclear interactions and currents. After a brief description of the methods and modern models of nuclear forces, we review the results obtained for all the bound, and some continuum states of up to eight nucleons. Various other applications of the methods are reviewed along with future prospects

Large scale exact quantum dynamics calculations: Ten thousand quantum states of acetonitrile

Science.gov (United States)

Halverson, Thomas; Poirier, Bill

2015-03-01

'Exact' quantum dynamics (EQD) calculations of the vibrational spectrum of acetonitrile (CH3CN) are performed, using two different methods: (1) phase-space-truncated momentum-symmetrized Gaussian basis and (2) correlated truncated harmonic oscillator basis. In both cases, a simple classical phase space picture is used to optimize the selection of individual basis functions-leading to drastic reductions in basis size, in comparison with existing methods. Massive parallelization is also employed. Together, these tools-implemented into a single, easy-to-use computer code-enable a calculation of tens of thousands of vibrational states of CH3CN to an accuracy of 0.001-10 cm-1.

Spin-driven structural effects in alkali doped (4)He clusters from quantum calculations.

Science.gov (United States)

Bovino, S; Coccia, E; Bodo, E; Lopez-Durán, D; Gianturco, F A

2009-06-14

In this paper, we carry out variational Monte Carlo and diffusion Monte Carlo (DMC) calculations for Li(2)((1)Sigma(g) (+))((4)He)(N) and Li(2)((3)Sigma(u) (+))((4)He)(N) with N up to 30 and discuss in detail the results of our computations. After a comparison between our DMC energies with the "exact" discrete variable representation values for the species with one (4)He, in order to test the quality of our computations at 0 K, we analyze the structural features of the whole range of doped clusters. We find that both species reside on the droplet surface, but that their orientation is spin driven, i.e., the singlet molecule is perpendicular and the triplet one is parallel to the droplet's surface. We have also computed quantum vibrational relaxation rates for both dimers in collision with a single (4)He and we find them to differ by orders of magnitude at the estimated surface temperature. Our results therefore confirm the findings from a great number of experimental data present in the current literature and provide one of the first attempts at giving an accurate, fully quantum picture for the nanoscopic properties of alkali dimers in (4)He clusters.

Efficient methods for including quantum effects in Monte Carlo calculations of large systems: extension of the displaced points path integral method and other effective potential methods to calculate properties and distributions.

Science.gov (United States)

Mielke, Steven L; Dinpajooh, Mohammadhasan; Siepmann, J Ilja; Truhlar, Donald G

2013-01-07

We present a procedure to calculate ensemble averages, thermodynamic derivatives, and coordinate distributions by effective classical potential methods. In particular, we consider the displaced-points path integral (DPPI) method, which yields exact quantal partition functions and ensemble averages for a harmonic potential and approximate quantal ones for general potentials, and we discuss the implementation of the new procedure in two Monte Carlo simulation codes, one that uses uncorrelated samples to calculate absolute free energies, and another that employs Metropolis sampling to calculate relative free energies. The results of the new DPPI method are compared to those from accurate path integral calculations as well as to results of two other effective classical potential schemes for the case of an isolated water molecule. In addition to the partition function, we consider the heat capacity and expectation values of the energy, the potential energy, the bond angle, and the OH distance. We also consider coordinate distributions. The DPPI scheme performs best among the three effective potential schemes considered and achieves very good accuracy for all of the properties considered. A key advantage of the effective potential schemes is that they display much lower statistical sampling variances than those for accurate path integral calculations. The method presented here shows great promise for including quantum effects in calculations on large systems.

Reducing dose calculation time for accurate iterative IMRT planning

International Nuclear Information System (INIS)

Siebers, Jeffrey V.; Lauterbach, Marc; Tong, Shidong; Wu Qiuwen; Mohan, Radhe

2002-01-01

A time-consuming component of IMRT optimization is the dose computation required in each iteration for the evaluation of the objective function. Accurate superposition/convolution (SC) and Monte Carlo (MC) dose calculations are currently considered too time-consuming for iterative IMRT dose calculation. Thus, fast, but less accurate algorithms such as pencil beam (PB) algorithms are typically used in most current IMRT systems. This paper describes two hybrid methods that utilize the speed of fast PB algorithms yet achieve the accuracy of optimizing based upon SC algorithms via the application of dose correction matrices. In one method, the ratio method, an infrequently computed voxel-by-voxel dose ratio matrix (R=D SC /D PB ) is applied for each beam to the dose distributions calculated with the PB method during the optimization. That is, D PB xR is used for the dose calculation during the optimization. The optimization proceeds until both the IMRT beam intensities and the dose correction ratio matrix converge. In the second method, the correction method, a periodically computed voxel-by-voxel correction matrix for each beam, defined to be the difference between the SC and PB dose computations, is used to correct PB dose distributions. To validate the methods, IMRT treatment plans developed with the hybrid methods are compared with those obtained when the SC algorithm is used for all optimization iterations and with those obtained when PB-based optimization is followed by SC-based optimization. In the 12 patient cases studied, no clinically significant differences exist in the final treatment plans developed with each of the dose computation methodologies. However, the number of time-consuming SC iterations is reduced from 6-32 for pure SC optimization to four or less for the ratio matrix method and five or less for the correction method. Because the PB algorithm is faster at computing dose, this reduces the inverse planning optimization time for our implementation

Accurate density-functional calculations on large systems: Fullerenes and magnetic clusters

International Nuclear Information System (INIS)

Dunlap, B.I.

1996-01-01

Efforts to accurately compute all-electron density-functional energies for large molecules and clusters using Gaussian basis sets will be reviewed. The foundation of this effort, variational fitting, will be described and followed by three applications of the method. The first application concerns fullerenes. When first discovered, C 60 is quite unstable relative to the higher fullerenes. In addition, to raising questions about the relative abundance of the various fullerenes, this work conflicted with the then state-of-the art density-funcitonal calculations on crystalline graphite. Now high accuracy molecular and band structure calculations are in fairly good agreement. Second, we have used these methods to design transition metal clusters having the highest magnetic moment by maximizing the symmetry-required degeneracy of the one-electron orbitals. Most recently, we have developed accurate, variational generalized-gradient approximation (GGA) forces for use in geometry optimization of clusters and in molecular-dynamics simulations of friction. The GGA optimized geometries of a number of large clusters will be given

Importance of Accurate Charges in Binding Affinity Calculations: A Case of Neuraminidase Series

Energy Technology Data Exchange (ETDEWEB)

Park, Kichul; Kyun, Nack Sung; Cho, Art E. [Korea Univ., Sejong (Korea, Republic of)

2013-02-15

It has been shown that calculating atomic charges using quantum mechanical level theory greatly improves the accuracy of docking. A protocol was developed and shown to be effective. That this protocol works is just a manifestation of the fact that electrostatic interactions are important in protein-ligand binding. In order to investigate how the same protocol helps in prediction of binding affinities, we took a series of known cocrystal structures of influenza neuraminidase inhibitors with the receptor and performed docking with Glide SP, Glide XP, and QPLD, the last being a workflow that incorporates QM/MM calculations to replace the fixed atomic charges of force fields with quantum mechanically recalculated ones at a given docking pose, and predicted the binding affinities of each cocrystal. The correlation with experimental binding affinities considerably improved with QPLD compared to Glide SP/XP yielding r{sup 2} = 0.83. The results suggest that for binding sites, such as that of neuraminidase, which are laden with hydrophilic residues, protocols such as QPLD which utilizes QM-based atomic charges can better predict the binding affinities.

Low field Monte-Carlo calculations in heterojunctions and quantum wells

NARCIS (Netherlands)

Hall, van P.J.; Rooij, de R.; Wolter, J.H.

1990-01-01

We present results of low-field Monte-Carlo calculations and compare them with experimental results. The negative absolute mobility of minority electrons in p-type quantum wells, as found in recent experiments, is described quite well.

Advances in computational methods for Quantum Field Theory calculations

NARCIS (Netherlands)

Ruijl, B.J.G.

2017-01-01

In this work we describe three methods to improve the performance of Quantum Field Theory calculations. First, we simplify large expressions to speed up numerical integrations. Second, we design Forcer, a program for the reduction of four-loop massless propagator integrals. Third, we extend the R*

Efficient Calculation of Exact Exchange Within the Quantum Espresso Software Package

Science.gov (United States)

Barnes, Taylor; Kurth, Thorsten; Carrier, Pierre; Wichmann, Nathan; Prendergast, David; Kent, Paul; Deslippe, Jack

Accurate simulation of condensed matter at the nanoscale requires careful treatment of the exchange interaction between electrons. In the context of plane-wave DFT, these interactions are typically represented through the use of approximate functionals. Greater accuracy can often be obtained through the use of functionals that incorporate some fraction of exact exchange; however, evaluation of the exact exchange potential is often prohibitively expensive. We present an improved algorithm for the parallel computation of exact exchange in Quantum Espresso, an open-source software package for plane-wave DFT simulation. Through the use of aggressive load balancing and on-the-fly transformation of internal data structures, our code exhibits speedups of approximately an order of magnitude for practical calculations. Additional optimizations are presented targeting the many-core Intel Xeon-Phi ``Knights Landing'' architecture, which largely powers NERSC's new Cori system. We demonstrate the successful application of the code to difficult problems, including simulation of water at a platinum interface and computation of the X-ray absorption spectra of transition metal oxides.

A calculational scheme for nonequilibrium quantum field system

International Nuclear Information System (INIS)

Yamanaka, Y.

1991-01-01

A new calculational scheme is presented for interacting nonequi-librium time dependent quantum field systems within the framework of thermo field dynamics (TFD), taking account of the fact that the thermal vacuum should go through many inequivalent state vector spaces. A para-meter parametrizing various state vector spaces has to be introduced and plays a role of new time-variable. Thus we have double-time TFD. The 2 requirements in this double-time TFD are imposed to establish a quasi-particle picture to get an attainable scheme of perturbative calculation : the existence of the spectral representation for the full propagator and the diagonalization of the quasi-particle Hamiltonian. The 1st condition turns out to amount to the existence of local-time tempera-ture. The 2nd condition leads to the master equation for the number density. This formalism is applied to high-energy heavy ion collision process. The very fundamental question is then how the thermodynamical properties such as heat and temperature appear in such an isolated system. This double-time TFD, suitable for isolated thermal systems of quantum fields, can handle the situation from the beginning of the process. (author). 24 refs.; 1 fig

Quantum Mechanics/Molecular Mechanics Method Combined with Hybrid All-Atom and Coarse-Grained Model: Theory and Application on Redox Potential Calculations.

Science.gov (United States)

Shen, Lin; Yang, Weitao

2016-04-12

We developed a new multiresolution method that spans three levels of resolution with quantum mechanical, atomistic molecular mechanical, and coarse-grained models. The resolution-adapted all-atom and coarse-grained water model, in which an all-atom structural description of the entire system is maintained during the simulations, is combined with the ab initio quantum mechanics and molecular mechanics method. We apply this model to calculate the redox potentials of the aqueous ruthenium and iron complexes by using the fractional number of electrons approach and thermodynamic integration simulations. The redox potentials are recovered in excellent accordance with the experimental data. The speed-up of the hybrid all-atom and coarse-grained water model renders it computationally more attractive. The accuracy depends on the hybrid all-atom and coarse-grained water model used in the combined quantum mechanical and molecular mechanical method. We have used another multiresolution model, in which an atomic-level layer of water molecules around redox center is solvated in supramolecular coarse-grained waters for the redox potential calculations. Compared with the experimental data, this alternative multilayer model leads to less accurate results when used with the coarse-grained polarizable MARTINI water or big multipole water model for the coarse-grained layer.

Free energies of binding from large-scale first-principles quantum mechanical calculations: application to ligand hydration energies.

Science.gov (United States)

Fox, Stephen J; Pittock, Chris; Tautermann, Christofer S; Fox, Thomas; Christ, Clara; Malcolm, N O J; Essex, Jonathan W; Skylaris, Chris-Kriton

2013-08-15

Schemes of increasing sophistication for obtaining free energies of binding have been developed over the years, where configurational sampling is used to include the all-important entropic contributions to the free energies. However, the quality of the results will also depend on the accuracy with which the intermolecular interactions are computed at each molecular configuration. In this context, the energy change associated with the rearrangement of electrons (electronic polarization and charge transfer) upon binding is a very important effect. Classical molecular mechanics force fields do not take this effect into account explicitly, and polarizable force fields and semiempirical quantum or hybrid quantum-classical (QM/MM) calculations are increasingly employed (at higher computational cost) to compute intermolecular interactions in free-energy schemes. In this work, we investigate the use of large-scale quantum mechanical calculations from first-principles as a way of fully taking into account electronic effects in free-energy calculations. We employ a one-step free-energy perturbation (FEP) scheme from a molecular mechanical (MM) potential to a quantum mechanical (QM) potential as a correction to thermodynamic integration calculations within the MM potential. We use this approach to calculate relative free energies of hydration of small aromatic molecules. Our quantum calculations are performed on multiple configurations from classical molecular dynamics simulations. The quantum energy of each configuration is obtained from density functional theory calculations with a near-complete psinc basis set on over 600 atoms using the ONETEP program.

Accurate calculation of the geometric measure of entanglement for multipartite quantum states

Science.gov (United States)

Teng, Peiyuan

2017-07-01

This article proposes an efficient way of calculating the geometric measure of entanglement using tensor decomposition methods. The connection between these two concepts is explored using the tensor representation of the wavefunction. Numerical examples are benchmarked and compared. Furthermore, we search for highly entangled qubit states to show the applicability of this method.

Quantum-Chemical Electron Densities of Proteins and of Selected Protein Sites from Subsystem Density Functional Theory

NARCIS (Netherlands)

Kiewisch, K.; Jacob, C.R.; Visscher, L.

2013-01-01

The ability to calculate accurate electron densities of full proteins or of selected sites in proteins is a prerequisite for a fully quantum-mechanical calculation of protein-protein and protein-ligand interaction energies. Quantum-chemical subsystem methods capable of treating proteins and other

Pseudopotentials for quantum-Monte-Carlo-calculations

International Nuclear Information System (INIS)

Burkatzki, Mark Thomas

2008-01-01

The author presents scalar-relativistic energy-consistent Hartree-Fock pseudopotentials for the main-group and 3d-transition-metal elements. The pseudopotentials do not exhibit a singularity at the nucleus and are therefore suitable for quantum Monte Carlo (QMC) calculations. The author demonstrates their transferability through extensive benchmark calculations of atomic excitation spectra as well as molecular properties. In particular, the author computes the vibrational frequencies and binding energies of 26 first- and second-row diatomic molecules using post Hartree-Fock methods, finding excellent agreement with the corresponding all-electron values. The author shows that the presented pseudopotentials give superior accuracy than other existing pseudopotentials constructed specifically for QMC. The localization error and the efficiency in QMC are discussed. The author also presents QMC calculations for selected atomic and diatomic 3d-transitionmetal systems. Finally, valence basis sets of different sizes (VnZ with n=D,T,Q,5 for 1st and 2nd row; with n=D,T for 3rd to 5th row; with n=D,T,Q for the 3d transition metals) optimized for the pseudopotentials are presented. (orig.)

Accurate Mapping of Multilevel Rydberg Atoms on Interacting Spin-1 /2 Particles for the Quantum Simulation of Ising Models

Science.gov (United States)

de Léséleuc, Sylvain; Weber, Sebastian; Lienhard, Vincent; Barredo, Daniel; Büchler, Hans Peter; Lahaye, Thierry; Browaeys, Antoine

2018-03-01

We study a system of atoms that are laser driven to n D3 /2 Rydberg states and assess how accurately they can be mapped onto spin-1 /2 particles for the quantum simulation of anisotropic Ising magnets. Using nonperturbative calculations of the pair potentials between two atoms in the presence of electric and magnetic fields, we emphasize the importance of a careful selection of experimental parameters in order to maintain the Rydberg blockade and avoid excitation of unwanted Rydberg states. We benchmark these theoretical observations against experiments using two atoms. Finally, we show that in these conditions, the experimental dynamics observed after a quench is in good agreement with numerical simulations of spin-1 /2 Ising models in systems with up to 49 spins, for which numerical simulations become intractable.

Numerical calculations in elementary quantum mechanics using Feynman path integrals

International Nuclear Information System (INIS)

Scher, G.; Smith, M.; Baranger, M.

1980-01-01

We show that it is possible to do numerical calculations in elementary quantum mechanics using Feynman path integrals. Our method involves discretizing both time and space, and summing paths through matrix multiplication. We give numerical results for various one-dimensional potentials. The calculations of energy levels and wavefunctions take approximately 100 times longer than with standard methods, but there are other problems for which such an approach should be more efficient

Large scale calculations for hadron spectroscopy

International Nuclear Information System (INIS)

Rebbi, C.

1985-01-01

The talk reviews some recent Monte Carlo calculations for Quantum Chromodynamics, performed on Euclidean lattices of rather large extent. Purpose of the calculations is to provide accurate determinations of quantities, such as interquark potentials or mass eigenvalues, which are relevant for hadronic spectroscopy. Results obtained in quenched QCD on 16 3 x 32 lattices are illustrated, and a discussion of computational resources and techniques required for the calculations is presented. 18 refs.,3 figs., 2 tabs

Accurate quasiparticle calculation of x-ray photoelectron spectra of solids.

Science.gov (United States)

Aoki, Tsubasa; Ohno, Kaoru

2018-05-31

It has been highly desired to provide an accurate and reliable method to calculate core electron binding energies (CEBEs) of crystals and to understand the final state screening effect on a core hole in high resolution x-ray photoelectron spectroscopy (XPS), because the ΔSCF method cannot be simply used for bulk systems. We propose to use the quasiparticle calculation based on many-body perturbation theory for this problem. In this study, CEBEs of band-gapped crystals, silicon, diamond, β-SiC, BN, and AlP, are investigated by means of the GW approximation (GWA) using the full ω integration and compared with the preexisting XPS data. The screening effect on a deep core hole is also investigated in detail by evaluating the relaxation energy (RE) from the core and valence contributions separately. Calculated results show that not only the valence electrons but also the core electrons have an important contribution to the RE, and the GWA have a tendency to underestimate CEBEs due to the excess RE. This underestimation can be improved by introducing the self-screening correction to the GWA. The resulting C1s, B1s, N1s, Si2p, and Al2p CEBEs are in excellent agreement with the experiments within 1 eV absolute error range. The present self-screening corrected GW approach has the capability to achieve the highly accurate prediction of CEBEs without any empirical parameter for band-gapped crystals, and provide a more reliable theoretical approach than the conventional ΔSCF-DFT method.

Accurate quasiparticle calculation of x-ray photoelectron spectra of solids

Science.gov (United States)

Aoki, Tsubasa; Ohno, Kaoru

2018-05-01

It has been highly desired to provide an accurate and reliable method to calculate core electron binding energies (CEBEs) of crystals and to understand the final state screening effect on a core hole in high resolution x-ray photoelectron spectroscopy (XPS), because the ΔSCF method cannot be simply used for bulk systems. We propose to use the quasiparticle calculation based on many-body perturbation theory for this problem. In this study, CEBEs of band-gapped crystals, silicon, diamond, β-SiC, BN, and AlP, are investigated by means of the GW approximation (GWA) using the full ω integration and compared with the preexisting XPS data. The screening effect on a deep core hole is also investigated in detail by evaluating the relaxation energy (RE) from the core and valence contributions separately. Calculated results show that not only the valence electrons but also the core electrons have an important contribution to the RE, and the GWA have a tendency to underestimate CEBEs due to the excess RE. This underestimation can be improved by introducing the self-screening correction to the GWA. The resulting C1s, B1s, N1s, Si2p, and Al2p CEBEs are in excellent agreement with the experiments within 1 eV absolute error range. The present self-screening corrected GW approach has the capability to achieve the highly accurate prediction of CEBEs without any empirical parameter for band-gapped crystals, and provide a more reliable theoretical approach than the conventional ΔSCF-DFT method.

Predicted phototoxicities of carbon nano-material by quantum mechanical calculations

Science.gov (United States)

The purpose of this research is to develop a predictive model for the phototoxicity potential of carbon nanomaterials (fullerenols and single-walled carbon nanotubes). This model is based on the quantum mechanical (ab initio) calculations on these carbon-based materials and compa...

Quantum leptogenesis I

International Nuclear Information System (INIS)

Anisimov, A.; Drewes, M.; Mendizabal, S.

2010-12-01

Thermal leptogenesis explains the observed matter-antimatter asymmetry of the universe in terms of neutrino masses, consistent with neutrino oscillation experiments. We present a full quantum mechanical calculation of the generated lepton asymmetry based on Kadanoff-Baym equations. Origin of the asymmetry is the departure from equilibrium of the statistical propagator of the heavy Majorana neutrino, together with CP violating couplings. The lepton asymmetry is calculated directly in terms of Green's functions without referring to ''number densities''. Compared to Boltzmann and quantum Boltzmann equations, the crucial difference are memory effects, rapid oscillations much faster than the heavy neutrino equilibration time. These oscillations strongly suppress the generated lepton asymmetry, unless the standard model gauge interactions, which cause thermal damping, are properly taken into account. We find that these damping effects essentially compensate the enhancement due to quantum statistical factors, so that finally the conventional Boltzmann equations again provide rather accurate predictions for the lepton asymmetry. (orig.)

Accurate nonadiabatic quantum dynamics on the cheap: Making the most of mean field theory with master equations

Energy Technology Data Exchange (ETDEWEB)

Kelly, Aaron; Markland, Thomas E., E-mail: tmarkland@stanford.edu [Department of Chemistry, Stanford University, Stanford, California 94305 (United States); Brackbill, Nora [Department of Physics, Stanford University, Stanford, California 94305 (United States)

2015-03-07

In this article, we show how Ehrenfest mean field theory can be made both a more accurate and efficient method to treat nonadiabatic quantum dynamics by combining it with the generalized quantum master equation framework. The resulting mean field generalized quantum master equation (MF-GQME) approach is a non-perturbative and non-Markovian theory to treat open quantum systems without any restrictions on the form of the Hamiltonian that it can be applied to. By studying relaxation dynamics in a wide range of dynamical regimes, typical of charge and energy transfer, we show that MF-GQME provides a much higher accuracy than a direct application of mean field theory. In addition, these increases in accuracy are accompanied by computational speed-ups of between one and two orders of magnitude that become larger as the system becomes more nonadiabatic. This combination of quantum-classical theory and master equation techniques thus makes it possible to obtain the accuracy of much more computationally expensive approaches at a cost lower than even mean field dynamics, providing the ability to treat the quantum dynamics of atomistic condensed phase systems for long times.

Accurate nonadiabatic quantum dynamics on the cheap: making the most of mean field theory with master equations.

Science.gov (United States)

Kelly, Aaron; Brackbill, Nora; Markland, Thomas E

2015-03-07

In this article, we show how Ehrenfest mean field theory can be made both a more accurate and efficient method to treat nonadiabatic quantum dynamics by combining it with the generalized quantum master equation framework. The resulting mean field generalized quantum master equation (MF-GQME) approach is a non-perturbative and non-Markovian theory to treat open quantum systems without any restrictions on the form of the Hamiltonian that it can be applied to. By studying relaxation dynamics in a wide range of dynamical regimes, typical of charge and energy transfer, we show that MF-GQME provides a much higher accuracy than a direct application of mean field theory. In addition, these increases in accuracy are accompanied by computational speed-ups of between one and two orders of magnitude that become larger as the system becomes more nonadiabatic. This combination of quantum-classical theory and master equation techniques thus makes it possible to obtain the accuracy of much more computationally expensive approaches at a cost lower than even mean field dynamics, providing the ability to treat the quantum dynamics of atomistic condensed phase systems for long times.

Analytic and numerical calculations of quantum synchrotron spectra from relativistic electron distributions

International Nuclear Information System (INIS)

Brainerd, J.J.; Petrosian, V.

1987-01-01

Calculations are performed numerically and analytically of synchrotron spectra for thermal and power-law electron distributions using the single-particle synchrotron power spectrum derived from quantum electrodynamics. It is found that the photon energy at which quantum effects appear is proportional to temperature and independent of field strength for thermal spectra; quantum effects introduce an exponential roll-off away from the classical spectra. For power law spectra, the photon energy at which quantum effects appear is inversely proportional to the magnetic field strength; quantum effects produce a steeper power law than is found classically. The results are compared with spectra derived from the classical power spectrum with an energy cutoff ensuring conservation of energy. It is found that an energy cutoff is generally an inadequate approximation of quantum effects for low photon energies and for thermal spectra, but gives reasonable results for high-energy emission from power-law electron distributions. 17 references

The reaction rate for dissociative adsorption of N-2 on stepped Ru(0001): Six-dimensional quantum calculations

DEFF Research Database (Denmark)

van Harrevelt, Rob; Honkala, Johanna Karoliina; Nørskov, Jens Kehlet

2005-01-01

Quantum-mechanical calculations of the reaction rate for dissociative adsorption of N-2 on stepped Ru(0001) are presented. Converged six-dimensional quantum calculations for this heavy-atom reaction have been performed using the multiconfiguration time-dependent Hartree method. A potential...

An efficient and accurate method for calculating nonlinear diffraction beam fields

Energy Technology Data Exchange (ETDEWEB)

Jeong, Hyun Jo; Cho, Sung Jong; Nam, Ki Woong; Lee, Jang Hyun [Division of Mechanical and Automotive Engineering, Wonkwang University, Iksan (Korea, Republic of)

2016-04-15

This study develops an efficient and accurate method for calculating nonlinear diffraction beam fields propagating in fluids or solids. The Westervelt equation and quasilinear theory, from which the integral solutions for the fundamental and second harmonics can be obtained, are first considered. A computationally efficient method is then developed using a multi-Gaussian beam (MGB) model that easily separates the diffraction effects from the plane wave solution. The MGB models provide accurate beam fields when compared with the integral solutions for a number of transmitter-receiver geometries. These models can also serve as fast, powerful modeling tools for many nonlinear acoustics applications, especially in making diffraction corrections for the nonlinearity parameter determination, because of their computational efficiency and accuracy.

Quantum - statistical equation of state

International Nuclear Information System (INIS)

Kalitkin, N.N.; Kuz'mina, L.V.

1976-01-01

An atom model is considered which allows uniform description of the equation of an equilibrium plasma state in the range of densities from gas to superhigh ones and in the temperature range from 1-5 eV to a ten of keV. Quantum and exchange corrections to the Thomas-Fermi thermodynamic functions at non zero temperatures have been calculated. The calculated values have been compared with experimental data and with calculations performed by more accurate models. The differences result from the fact that a quantum approach does not allow for shell effects. The evaluation of these differences makes it possible to indicate the limits of applicability of the Thomas-Fermi model with quantum and exchange corrections. It turns out that if at zero temperature the model may be applied only for high compressions, at the temperature more than 1 eV it well describes the behaviour of plasma in a very wide range of densities and agrees satisfactorily with experiment even for non-ideal plasma

Achieving High Accuracy in Calculations of NMR Parameters

DEFF Research Database (Denmark)

Faber, Rasmus

quantum chemical methods have been developed, the calculation of NMR parameters with quantitative accuracy is far from trivial. In this thesis I address some of the issues that makes accurate calculation of NMR parameters so challenging, with the main focus on SSCCs. High accuracy quantum chemical......, but no programs were available to perform such calculations. As part of this thesis the CFOUR program has therefore been extended to allow the calculation of SSCCs using the CC3 method. CC3 calculations of SSCCs have then been performed for several molecules, including some difficult cases. These results show...... vibrations must be included. The calculation of vibrational corrections to NMR parameters has been reviewed as part of this thesis. A study of the basis set convergence of vibrational corrections to nuclear shielding constants has also been performed. The basis set error in vibrational correction...

Deterministic constant-temperature dynamics for dissipative quantum systems

International Nuclear Information System (INIS)

Sergi, Alessandro

2007-01-01

A novel method is introduced in order to treat the dissipative dynamics of quantum systems interacting with a bath of classical degrees of freedom. The method is based upon an extension of the Nose-Hoover chain (constant temperature) dynamics to quantum-classical systems. Both adiabatic and nonadiabatic numerical calculations on the relaxation dynamics of the spin-boson model show that the quantum-classical Nose-Hoover chain dynamics represents the thermal noise of the bath in an accurate and simple way. Numerical comparisons, both with the constant-energy calculation and with the quantum-classical Brownian motion treatment of the bath, show that the quantum-classical Nose-Hoover chain dynamics can be used to introduce dissipation in the evolution of a quantum subsystem even with just one degree of freedom for the bath. The algorithm can be computationally advantageous in modelling, within computer simulation, the dynamics of a quantum subsystem interacting with complex molecular environments. (fast track communication)

Vibrational cooling of spin-stretched dimer states by He buffer gas: quantum calculations for Li2(a 3Sigma(u)+) at ultralow energies.

Science.gov (United States)

Bovino, S; Bodo, E; Yurtsever, E; Gianturco, F A

2008-06-14

The interaction between the triplet state of the lithium dimer, (7)Li(2), with (4)He is obtained from accurate ab initio calculations where the vibrational dependence of the potential is newly computed. Vibrational quenching dynamics within a coupled-channel quantum treatment is carried out at ultralow energies, and large differences in efficiency as a function of the initial vibrational state of the targets are found as one compares the triplet results with those of the singlet state of the same target.

Accurate Calculation of Fringe Fields in the LHC Main Dipoles

CERN Document Server

Kurz, S; Siegel, N

2000-01-01

The ROXIE program developed at CERN for the design and optimization of the superconducting LHC magnets has been recently extended in a collaboration with the University of Stuttgart, Germany, with a field computation method based on the coupling between the boundary element (BEM) and the finite element (FEM) technique. This avoids the meshing of the coils and the air regions, and avoids the artificial far field boundary conditions. The method is therefore specially suited for the accurate calculation of fields in the superconducting magnets in which the field is dominated by the coil. We will present the fringe field calculations in both 2d and 3d geometries to evaluate the effect of connections and the cryostat on the field quality and the flux density to which auxiliary bus-bars are exposed.

Quantum statistical mechanics of dense partially ionized hydrogen.

Science.gov (United States)

Dewitt, H. E.; Rogers, F. J.

1972-01-01

The theory of dense hydrogenic plasmas beginning with the two component quantum grand partition function is reviewed. It is shown that ionization equilibrium and molecular dissociation equilibrium can be treated in the same manner with proper consideration of all two-body states. A quantum perturbation expansion is used to give an accurate calculation of the equation of state of the gas for any degree of dissociation and ionization. In this theory, the effective interaction between any two charges is the dynamic screened potential obtained from the plasma dielectric function. We make the static approximation; and we carry out detailed numerical calculations with the bound and scattering states of the Debye potential, using the Beth-Uhlenbeck form of the quantum second virial coefficient. We compare our results with calculations from the Saha equation.

Quantum computing applied to calculations of molecular energies: CH2 benchmark.

Science.gov (United States)

Veis, Libor; Pittner, Jiří

2010-11-21

Quantum computers are appealing for their ability to solve some tasks much faster than their classical counterparts. It was shown in [Aspuru-Guzik et al., Science 309, 1704 (2005)] that they, if available, would be able to perform the full configuration interaction (FCI) energy calculations with a polynomial scaling. This is in contrast to conventional computers where FCI scales exponentially. We have developed a code for simulation of quantum computers and implemented our version of the quantum FCI algorithm. We provide a detailed description of this algorithm and the results of the assessment of its performance on the four lowest lying electronic states of CH(2) molecule. This molecule was chosen as a benchmark, since its two lowest lying (1)A(1) states exhibit a multireference character at the equilibrium geometry. It has been shown that with a suitably chosen initial state of the quantum register, one is able to achieve the probability amplification regime of the iterative phase estimation algorithm even in this case.

Improved Patient Size Estimates for Accurate Dose Calculations in Abdomen Computed Tomography

Energy Technology Data Exchange (ETDEWEB)

Lee, Chang-Lae [Yonsei University, Wonju (Korea, Republic of)

2017-07-15

The radiation dose of CT (computed tomography) is generally represented by the CTDI (CT dose index). CTDI, however, does not accurately predict the actual patient doses for different human body sizes because it relies on a cylinder-shaped head (diameter : 16 cm) and body (diameter : 32 cm) phantom. The purpose of this study was to eliminate the drawbacks of the conventional CTDI and to provide more accurate radiation dose information. Projection radiographs were obtained from water cylinder phantoms of various sizes, and the sizes of the water cylinder phantoms were calculated and verified using attenuation profiles. The effective diameter was also calculated using the attenuation of the abdominal projection radiographs of 10 patients. When the results of the attenuation-based method and the geometry-based method shown were compared with the results of the reconstructed-axial-CT-image-based method, the effective diameter of the attenuation-based method was found to be similar to the effective diameter of the reconstructed-axial-CT-image-based method, with a difference of less than 3.8%, but the geometry-based method showed a difference of less than 11.4%. This paper proposes a new method of accurately computing the radiation dose of CT based on the patient sizes. This method computes and provides the exact patient dose before the CT scan, and can therefore be effectively used for imaging and dose control.

An Effective Method to Accurately Calculate the Phase Space Factors for β"-β"- Decay

International Nuclear Information System (INIS)

Horoi, Mihai; Neacsu, Andrei

2016-01-01

Accurate calculations of the electron phase space factors are necessary for reliable predictions of double-beta decay rates and for the analysis of the associated electron angular and energy distributions. We present an effective method to calculate these phase space factors that takes into account the distorted Coulomb field of the daughter nucleus, yet it allows one to easily calculate the phase space factors with good accuracy relative to the most exact methods available in the recent literature.

Chemical dynamics in the gas phase: Time-dependent quantum mechanics of chemical reactions

Energy Technology Data Exchange (ETDEWEB)

Gray, S.K. [Argonne National Laboratory, IL (United States)

1993-12-01

A major goal of this research is to obtain an understanding of the molecular reaction dynamics of three and four atom chemical reactions using numerically accurate quantum dynamics. This work involves: (i) the development and/or improvement of accurate quantum mechanical methods for the calculation and analysis of the properties of chemical reactions (e.g., rate constants and product distributions), and (ii) the determination of accurate dynamical results for selected chemical systems, which allow one to compare directly with experiment, determine the reliability of the underlying potential energy surfaces, and test the validity of approximate theories. This research emphasizes the use of recently developed time-dependent quantum mechanical methods, i.e. wave packet methods.

Exploiting Locality in Quantum Computation for Quantum Chemistry.

Science.gov (United States)

McClean, Jarrod R; Babbush, Ryan; Love, Peter J; Aspuru-Guzik, Alán

2014-12-18

Accurate prediction of chemical and material properties from first-principles quantum chemistry is a challenging task on traditional computers. Recent developments in quantum computation offer a route toward highly accurate solutions with polynomial cost; however, this solution still carries a large overhead. In this Perspective, we aim to bring together known results about the locality of physical interactions from quantum chemistry with ideas from quantum computation. We show that the utilization of spatial locality combined with the Bravyi-Kitaev transformation offers an improvement in the scaling of known quantum algorithms for quantum chemistry and provides numerical examples to help illustrate this point. We combine these developments to improve the outlook for the future of quantum chemistry on quantum computers.

Quantum mechanical methods for calculation of force constants

International Nuclear Information System (INIS)

Mullally, D.J.

1985-01-01

The focus of this thesis is upon the calculation of force constants; i.e., the second derivatives of the potential energy with respect to nuclear displacements. This information is useful for the calculation of molecular vibrational modes and frequencies. In addition, it may be used for the location and characterization of equilibrium and transition state geometries. The methods presented may also be applied to the calculation of electric polarizabilities and infrared and Raman vibrational intensities. Two approaches to this problem are studied and evaluated: finite difference methods and analytical techniques. The most suitable method depends on the type and level of theory used to calculate the electronic wave function. Double point displacement finite differencing is often required for accurate calculation of the force constant matrix. These calculations require energy and gradient calculations on both sides of the geometry of interest. In order to speed up these calculations, a novel method is presented that uses geometry dependent information about the wavefunction. A detailed derivation for the analytical evaluation of force constants with a complete active space multiconfiguration self consistent field wave function is presented

Fast and accurate calculation of the properties of water and steam for simulation

International Nuclear Information System (INIS)

Szegi, Zs.; Gacs, A.

1990-01-01

A basic principle simulator was developed at the CRIP, Budapest, for real time simulation of the transients of WWER-440 type nuclear power plants. Its integral part is the fast and accurate calculation of the thermodynamic properties of water and steam. To eliminate successive approximations, the model system of the secondary coolant circuit requires binary forms which are known as inverse functions, countinuous when crossing the saturation line, accurate and coherent for all argument combinations. A solution which reduces the computer memory and execution time demand is reported. (author) 36 refs.; 5 figs.; 3 tabs

Calculation of the Huang-Rhys parameter in spherical quantum dots: the optical deformation potential effect

International Nuclear Information System (INIS)

Hamma, M; Miranda, R P; Vasilevskiy, M I; Zorkani, I

2007-01-01

An accurate calculation of the exciton-phonon interaction matrix elements and Huang-Rhys parameter for nearly spherical nanocrystals (NCs) of polar semiconductor materials is presented. The theoretical approach is based on a continuum lattice dynamics model and the effective mass approximation for electronic states in the NCs. A strong confinement regime is considered for both excitons and optical phonons, taking into account both the Froehlich-type and optical deformation potential (ODP) mechanisms of the exciton-phonon interaction. The effects of exchange electron-hole interaction and possible hexagonal crystal structure of the underlying material are also taken into account. The theory is applied to CdSe and InP quantum dots. It is shown that the ODP mechanism, almost unimportant for CdSe, dominates the exciton-phonon coupling in small InP dots. The effect of the non-diagonal interaction, not included in the Huang-Rhys parameter, is briefly discussed

Biomolecular Structure Information from High-Speed Quantum Mechanical Electronic Spectra Calculation.

Science.gov (United States)

Seibert, Jakob; Bannwarth, Christoph; Grimme, Stefan

2017-08-30

A fully quantum mechanical (QM) treatment to calculate electronic absorption (UV-vis) and circular dichroism (CD) spectra of typical biomolecules with thousands of atoms is presented. With our highly efficient sTDA-xTB method, spectra averaged along structures from molecular dynamics (MD) simulations can be computed in a reasonable time frame on standard desktop computers. This way, nonequilibrium structure and conformational, as well as purely quantum mechanical effects like charge-transfer or exciton-coupling, are included. Different from other contemporary approaches, the entire system is treated quantum mechanically and neither fragmentation nor system-specific adjustment is necessary. Among the systems considered are a large DNA fragment, oligopeptides, and even entire proteins in an implicit solvent. We propose the method in tandem with experimental spectroscopy or X-ray studies for the elucidation of complex (bio)molecular structures including metallo-proteins like myoglobin.

Multi-fidelity machine learning models for accurate bandgap predictions of solids

International Nuclear Information System (INIS)

Pilania, Ghanshyam; Gubernatis, James E.; Lookman, Turab

2016-01-01

Here, we present a multi-fidelity co-kriging statistical learning framework that combines variable-fidelity quantum mechanical calculations of bandgaps to generate a machine-learned model that enables low-cost accurate predictions of the bandgaps at the highest fidelity level. Additionally, the adopted Gaussian process regression formulation allows us to predict the underlying uncertainties as a measure of our confidence in the predictions. In using a set of 600 elpasolite compounds as an example dataset and using semi-local and hybrid exchange correlation functionals within density functional theory as two levels of fidelities, we demonstrate the excellent learning performance of the method against actual high fidelity quantum mechanical calculations of the bandgaps. The presented statistical learning method is not restricted to bandgaps or electronic structure methods and extends the utility of high throughput property predictions in a significant way.

Direct Calculation of Permeability by High-Accurate Finite Difference and Numerical Integration Methods

KAUST Repository

Wang, Yi

2016-07-21

Velocity of fluid flow in underground porous media is 6~12 orders of magnitudes lower than that in pipelines. If numerical errors are not carefully controlled in this kind of simulations, high distortion of the final results may occur [1-4]. To fit the high accuracy demands of fluid flow simulations in porous media, traditional finite difference methods and numerical integration methods are discussed and corresponding high-accurate methods are developed. When applied to the direct calculation of full-tensor permeability for underground flow, the high-accurate finite difference method is confirmed to have numerical error as low as 10-5% while the high-accurate numerical integration method has numerical error around 0%. Thus, the approach combining the high-accurate finite difference and numerical integration methods is a reliable way to efficiently determine the characteristics of general full-tensor permeability such as maximum and minimum permeability components, principal direction and anisotropic ratio. Copyright © Global-Science Press 2016.

Quantum mechanical determination of atomic polarizabilities of ionic liquids.

Science.gov (United States)

Heid, Esther; Szabadi, András; Schröder, Christian

2018-04-25

The distribution of a molecule's polarizability to individual atomic sites is inevitable to develop accurate polarizable force fields. We present the direct quantum mechanical calculation of atomic polarizabilities of 27 common ionic liquids. The method is superior to previously published distribution routines based on large databases of the molecular polarizability, and enables the correct description of any ionic liquid and its peculiarities within the quantum mechanical framework.

Calculation of transition probabilities using the multiconfiguration Dirac-Fock method

International Nuclear Information System (INIS)

Kim, Yong Ki; Desclaux, Jean Paul; Indelicato, Paul

1998-01-01

The performance of the multiconfiguration Dirac-Fock (MCDF) method in calculating transition probabilities of atoms is reviewed. In general, the MCDF wave functions will lead to transition probabilities accurate to ∼ 10% or better for strong, electric-dipole allowed transitions for small atoms. However, it is more difficult to get reliable transition probabilities for weak transitions. Also, some MCDF wave functions for a specific J quantum number may not reduce to the appropriate L and S quantum numbers in the nonrelativistic limit. Transition probabilities calculated from such MCDF wave functions for nonrelativistically forbidden transitions are unreliable. Remedies for such cases are discussed

Analytic calculations of trial wave functions of the fractional quantum Hall effect on the sphere

Energy Technology Data Exchange (ETDEWEB)

Souza Batista, C.L. de [Centro Brasileiro de Pesquisas Fisicas (CBPF), Rio de Janeiro, RJ (Brazil); Dingping Li [Perugia Univ. (Italy). Dipt. di Fisica

1996-07-01

We present a framework for the analytic calculations of the hierarchical wave functions and the composite fermion wave functions in the fractional quantum Hall effect on the sphere by using projective coordinates. Then we calculate the overlaps between these two wave functions at various fillings and small numbers of electrons. We find that the overlaps are most equal to one. This gives a further evidence that two theories of the fractional quantum Hall effect, the hierarchical theory, are physically equivalent. (author). 31 refs., 2 tabs.

Procedures of grasp92 code to calculate accurate Dirac-Coulomb energy for the ground sate of helium atom

International Nuclear Information System (INIS)

Utsumi, Takayuki; Sasaki, Akira

2000-02-01

The procedures of grasp92 code to calculate accurate (relative error nearly equal 10 -7 ) eigenvalue for the ground sate of helium atom of the Dirac-Coulomb Hamiltonian are presented. The grasp92 code, based on the multi-configuration Dirac-Fock method, is widely used to calculate the atomic properties. However, the main part of the accurate calculations, extended optimal level calculation (EOL), suffer frequently numerical instabilities due to the lack of the confident procedures. The purpose of this report is to illustrate the guideline for stable EOL calculations by calculating the most fundamental atomic system, i.e. the ground sate of helium atom ls 2 1 S 2 . This procedure could be extended for the high-precise eigenfunction calculation of more complex atomic systems, for example highly ionized atoms and high-Z atoms. (author)

Opacity calculations for laser plasma applications

International Nuclear Information System (INIS)

Magee, N.H. Jr.

1986-01-01

The Los Alamos LTE light element detailed configuration opacity code (LEDCOP) has been revised to provide more accurate absorption coefficients and group means for modern radiation-hydrodynamic codes. The new group means will be especially useful for computing the transport of thermal radiation from laser deposition. The principal improvement is the inclusion of a complete set of accurate and internally consistent LS term energies and oscillator strengths in both the EOS and absorption coefficients. Selected energies and oscillator strengths were calculated from a Hartree-Fock code, then fitted by a quantum defect method. This allowed transitions at all wavelengths to be treated consistently and accurately instead of being limited to wavelength regions covered by experimental observations or isolated theoretical calculations. A second improvement is the use of more accurate photoionization cross sections for excited as well as ground state configurations. These cross sections are now more consistent with the bound-bound oscillator strengths, leading to a smooth transition across the continuum limit. Results will be presented showing the agreement of the LS term energies and oscillator strengths with observed values. The new absorption coefficients will be compared with previous calculations. 5 refs., 9 figs., 1 tab

"Shut up and calculate": the available discursive positions in quantum physics courses

Science.gov (United States)

Johansson, Anders; Andersson, Staffan; Salminen-Karlsson, Minna; Elmgren, Maja

2018-03-01

Educating new generations of physicists is often seen as a matter of attracting good students, teaching them physics and making sure that they stay at the university. Sometimes, questions are also raised about what could be done to increase diversity in recruitment. Using a discursive perspective, in this study of three introductory quantum physics courses at two Swedish universities, we instead ask what it means to become a physicist, and whether certain ways of becoming a physicist and doing physics is privileged in this process. Asking the question of what discursive positions are made accessible to students, we use observations of lectures and problem solving sessions together with interviews with students to characterize the discourse in the courses. Many students seem to have high expectations for the quantum physics course and generally express that they appreciate the course more than other courses. Nevertheless, our analysis shows that the ways of being a "good quantum physics student" are limited by the dominating focus on calculating quantum physics in the courses. We argue that this could have negative consequences both for the education of future physicists and the discipline of physics itself, in that it may reproduce an instrumental "shut up and calculate"-culture of physics, as well as an elitist physics education. Additionally, many students who take the courses are not future physicists, and the limitation of discursive positions may also affect these students significantly.

Accurate reactivity void coefficient calculation for the fast spectrum reactor FBR-IME

Energy Technology Data Exchange (ETDEWEB)

Lima, Fabiano P.C.; Vellozo, Sergio de O.; Velozo, Marta J., E-mail: fabianopetruceli@outlook.com, E-mail: vellozo@cbpf.br, E-mail: martajann@gmail.com [Instituto Militar de Engenharia (IME), Rio de Janeiro, RJ (Brazil). Secao de Engenharia Militar

2017-07-01

This paper aims to present an accurate calculation of the void reactivity coefficient for the FBR-IME, a fast spectrum reactor in development at the Engineering Military Institute (IME). The main design peculiarity lies in using mixed oxide [MOX - PuO{sub 2} + U(natural uranium)O{sub 2}] as fuel core. For this task, SCALE system was used to calculate the reactivity for several voids distributions generated by bubbles in the sodium beyond its boiling point. The results show that although the void reactivity coefficient is positive and location dependent, they are offset by other feedback effects, resulting in a negative overall coefficient. (author)

Accurate quantum yields by laser gain vs absorption spectroscopy - Investigation of Br/Br(asterisk) channels in photofragmentation of Br2 and IBr

Science.gov (United States)

Haugen, H. K.; Weitz, E.; Leone, S. R.

1985-01-01

Various techniques have been used to study photodissociation dynamics of the halogens and interhalogens. The quantum yields obtained by these techniques differ widely. The present investigation is concerned with a qualitatively new approach for obtaining highly accurate quantum yields for electronically excited states. This approach makes it possible to obtain an accuracy of 1 percent to 3 percent. It is shown that measurement of the initial transient gain/absorption vs the final absorption in a single time-resolved signal is a very accurate technique in the study of absolute branching fractions in photodissociation. The new technique is found to be insensitive to pulse and probe laser characteristics, molecular absorption cross sections, and absolute precursor density.

The use of bulk states to accelerate the band edge state calculation of a semiconductor quantum dot

International Nuclear Information System (INIS)

Voemel, Christof; Tomov, Stanimire Z.; Wang, Lin-Wang; Marques, Osni A.; Dongarra, Jack J.

2007-01-01

We present a new technique to accelerate the convergence of the folded spectrum method in empirical pseudopotential band edge state calculations for colloidal quantum dots. We use bulk band states of the materials constituent of the quantum dot to construct initial vectors and a preconditioner. We apply these to accelerate the convergence of the folded spectrum method for the interior states at the top of the valence and the bottom of the conduction band. For large CdSe quantum dots, the number of iteration steps until convergence decreases by about a factor of 4 compared to previous calculations

Quantum Monte Carlo calculations of van der Waals interactions between aromatic benzene rings

Science.gov (United States)

Azadi, Sam; Kühne, T. D.

2018-05-01

The magnitude of finite-size effects and Coulomb interactions in quantum Monte Carlo simulations of van der Waals interactions between weakly bonded benzene molecules are investigated. To that extent, two trial wave functions of the Slater-Jastrow and Backflow-Slater-Jastrow types are employed to calculate the energy-volume equation of state. We assess the impact of the backflow coordinate transformation on the nonlocal correlation energy. We found that the effect of finite-size errors in quantum Monte Carlo calculations on energy differences is particularly large and may even be more important than the employed trial wave function. In addition to the cohesive energy, the singlet excitonic energy gap and the energy gap renormalization of crystalline benzene at different densities are computed.

Biological Applications of Hybrid Quantum Mechanics/Molecular Mechanics Calculation

Directory of Open Access Journals (Sweden)

Jiyoung Kang

2012-01-01

Full Text Available Since in most cases biological macromolecular systems including solvent water molecules are remarkably large, the computational costs of performing ab initio calculations for the entire structures are prohibitive. Accordingly, QM calculations that are jointed with MM calculations are crucial to evaluate the long-range electrostatic interactions, which significantly affect the electronic structures of biological macromolecules. A UNIX-shell-based interface program connecting the quantum mechanics (QMs and molecular mechanics (MMs calculation engines, GAMESS and AMBER, was developed in our lab. The system was applied to a metalloenzyme, azurin, and PU.1-DNA complex; thereby, the significance of the environmental effects on the electronic structures of the site of interest was elucidated. Subsequently, hybrid QM/MM molecular dynamics (MD simulation using the calculation system was employed for investigation of mechanisms of hydrolysis (editing reaction in leucyl-tRNA synthetase complexed with the misaminoacylated tRNALeu, and a novel mechanism of the enzymatic reaction was revealed. Thus, our interface program can play a critical role as a powerful tool for state-of-the-art sophisticated hybrid ab initio QM/MM MD simulations of large systems, such as biological macromolecules.

Quantum phase space theory for the calculation of v·j vector correlations

International Nuclear Information System (INIS)

Hall, G.E.

1995-01-01

The quantum state-counting phase space theory commonly used to describe barrierless dissociation is recast in a helicity basis to calculate photofragment v·j correlations. Counting pairs of fragment states with specific angular momentum projection numbers on the relative velocity provides a simple connection between angular momentum conservation and the v·j correlation, which is not so evident in the conventional basis for phase space state counts. The upper bound on the orbital angular momentum, l, imposed by the centrifugal barrier cannot be included simply in the helicity basis, where l is not a good quantum number. Two approaches for a quantum calculation of the v·j correlation are described to address this point. An application to the photodissociation of NCCN is consistent with recent classical phase space calculations of Cline and Klippenstein. The observed vector correlation exceeds the phase space theory prediction. The authors take this as evidence of incomplete mixing of the K states of the linear parent molecule at the transition state, corresponding to an evolution of the body-fixed projection number K into the total helicity of the fragment pair state. The average over a thermal distribution of parent angular momentum in the special case of a linear molecule does not significantly reduce the v·j correlation below that computed for total J = 0

Calculation of accurate small angle X-ray scattering curves from coarse-grained protein models

Directory of Open Access Journals (Sweden)

Stovgaard Kasper

2010-08-01

Full Text Available Abstract Background Genome sequencing projects have expanded the gap between the amount of known protein sequences and structures. The limitations of current high resolution structure determination methods make it unlikely that this gap will disappear in the near future. Small angle X-ray scattering (SAXS is an established low resolution method for routinely determining the structure of proteins in solution. The purpose of this study is to develop a method for the efficient calculation of accurate SAXS curves from coarse-grained protein models. Such a method can for example be used to construct a likelihood function, which is paramount for structure determination based on statistical inference. Results We present a method for the efficient calculation of accurate SAXS curves based on the Debye formula and a set of scattering form factors for dummy atom representations of amino acids. Such a method avoids the computationally costly iteration over all atoms. We estimated the form factors using generated data from a set of high quality protein structures. No ad hoc scaling or correction factors are applied in the calculation of the curves. Two coarse-grained representations of protein structure were investigated; two scattering bodies per amino acid led to significantly better results than a single scattering body. Conclusion We show that the obtained point estimates allow the calculation of accurate SAXS curves from coarse-grained protein models. The resulting curves are on par with the current state-of-the-art program CRYSOL, which requires full atomic detail. Our method was also comparable to CRYSOL in recognizing native structures among native-like decoys. As a proof-of-concept, we combined the coarse-grained Debye calculation with a previously described probabilistic model of protein structure, TorusDBN. This resulted in a significant improvement in the decoy recognition performance. In conclusion, the presented method shows great promise for

Method to Calculate Accurate Top Event Probability in a Seismic PSA

Energy Technology Data Exchange (ETDEWEB)

Jung, Woo Sik [Sejong Univ., Seoul (Korea, Republic of)

2014-05-15

ACUBE(Advanced Cutset Upper Bound Estimator) calculates the top event probability and importance measures from cutsets by dividing cutsets into major and minor groups depending on the cutset probability, where the cutsets that have higher cutset probability are included in the major group and the others in minor cutsets, converting major cutsets into a Binary Decision Diagram (BDD). By applying the ACUBE algorithm to the seismic PSA cutsets, the accuracy of a top event probability and importance measures can be significantly improved. ACUBE works by dividing the cutsets into two groups (higher and lower cutset probability groups), calculating the top event probability and importance measures in each group, and combining the two results from the two groups. Here, ACUBE calculates the top event probability and importance measures of the higher cutset probability group exactly. On the other hand, ACUBE calculates these measures of the lower cutset probability group with an approximation such as MCUB. The ACUBE algorithm is useful for decreasing the conservatism that is caused by approximating the top event probability and importance measure calculations with given cutsets. By applying the ACUBE algorithm to the seismic PSA cutsets, the accuracy of a top event probability and importance measures can be significantly improved. This study shows that careful attention should be paid and an appropriate method be provided in order to avoid the significant overestimation of the top event probability calculation. Due to the strength of ACUBE that is explained in this study, the ACUBE became a vital tool for calculating more accurate CDF of the seismic PSA cutsets than the conventional probability calculation method.

Quantum-mechanical DFT calculation supported Raman spectroscopic study of some amino acids in bovine insulin.

Science.gov (United States)

Tah, Bidisha; Pal, Prabir; Roy, Sourav; Dutta, Debodyuti; Mishra, Sabyashachi; Ghosh, Manash; Talapatra, G B

2014-08-14

In this article Quantum mechanical (QM) calculations by Density Functional Theory (DFT) have been performed of all amino acids present in bovine insulin. Simulated Raman spectra of those amino acids are compared with their experimental spectra and the major bands are assigned. The results are in good agreement with experiment. We have also verified the DFT results with Quantum mechanical molecular mechanics (QM/MM) results for some amino acids. QM/MM results are very similar with the DFT results. Although the theoretical calculation of individual amino acids are feasible, but the calculated Raman spectrum of whole protein molecule is difficult or even quite impossible task, since it relies on lengthy and costly quantum-chemical computation. However, we have tried to simulate the Raman spectrum of whole protein by adding the proportionate contribution of the Raman spectra of each amino acid present in this protein. In DFT calculations, only the contributions of disulphide bonds between cysteines are included but the contribution of the peptide and hydrogen bonds have not been considered. We have recorded the Raman spectra of bovine insulin using micro-Raman set up. The experimental spectrum is found to be very similar with the resultant simulated Raman spectrum with some exceptions. Copyright © 2014 Elsevier B.V. All rights reserved.

Adaptation of quantum chemistry software for the electronic structure calculations on GPU for solid-state systems

International Nuclear Information System (INIS)

Gusakov, V.E.; Bel'ko, V.I.; Dorozhkin, N.N.

2015-01-01

We report on adaptation of quantum chemistry software - Quantum Espresso and LASTO - for the electronic structure calculations for the complex solid-state systems on the GeForce series GPUs using the nVIDIA CUDA technology. Specifically, protective covering based on transition metal nitrides are considered. (authors)

Quantum mechanical calculations of state-to-state cross sections and rate constants for the F + DCl → Cl + DF reaction.

Science.gov (United States)

Bulut, Niyazi; Kłos, Jacek; Roncero, Octavio

2015-06-07

We present accurate state-to-state quantum wave packet calculations of integral cross sections and rate constants for the title reaction. Calculations are carried out on the best available ground 1(2)A' global adiabatic potential energy surface of Deskevich et al. [J. Chem. Phys. 124, 224303 (2006)]. Converged state-to-state reaction cross sections have been calculated for collision energies up to 0.5 eV and different initial rotational and vibrational excitations, DCl(v = 0, j = 0 - 1; v = 1, j = 0). Also, initial-state resolved rate constants of the title reaction have been calculated in a temperature range of 100-400 K. It is found that the initial rotational excitation of the DCl molecule does not enhance reactivity, in contract to the reaction with the isotopologue HCl in which initial rotational excitation produces an important enhancement. These differences between the isotopologue reactions are analyzed in detail and attributed to the presence of resonances for HCl(v = 0, j), absent in the case of DCl(v = 0, j). For vibrational excited DCl(v = 1, j), however, the reaction cross section increases noticeably, what is also explained by another resonance.

Determination of quantum defects from the poles of the Schwinger T matrix

International Nuclear Information System (INIS)

Snitchler, G.L.

1987-01-01

Quantum defects are determined for lithium, sodium, potassium, and beryllium by searching for the poles of the Schwinger T matrix along the negative real-energy axis. This method takes advantage of the fundamental ideas of QDT by using a Coulomb Green's function to factor out most of the energy dependence. For the alkali atoms, a single-channel calculation is performed using model potentials to include the effects of core polarization and correlation. Quantum defects accurate to 1% are easily obtained with small grids and small fixed-basis sets for an entire Rydberg series up to principal quantum number, n, as high as 60. A multichannel extension of this method is used to determined neutral-beryllium quantum defects for the 1 P 0 , 3 P 0 , and 3 S Rydberg series. The 1 P 0 and 3 P 0 calculations are performed in a two-channel approximation using 1s 2 2p static-exchange cores. The 3 S calculation includes a third channel with a 1s 2 3s core. Accurate quantum defects are obtained with 4 to 6 basis functions per channel. The energies are variational and the wave functions have the correct asymptotic form enforced by the Coulomb Green's function. Tentative results for Be I 1 P 0 and 3 P 0 resonances below the 1s 2 2p 2 P threshold are presented. This calculation which is performed in a three-channel approximation uses a complex multichannel Coulomb Green's function to search for poles in the fourth quadrant of the complex-energy plane

Projected Dipole Model for Quantum Plasmonics

DEFF Research Database (Denmark)

Yan, Wei; Wubs, Martijn; Mortensen, N. Asger

2015-01-01

of classical electrodynamics, while quantum properties are described accurately through an infinitely thin layer of dipoles oriented normally to the metal surface. The nonlocal polarizability of the dipole layer-the only introduced parameter-is mapped from the free-electron distribution near the metal surface...... as obtained with 1D quantum calculations, such as time-dependent density-functional theory (TDDFT), and is determined once and for all. The model can be applied in two and three dimensions to any system size that is tractable within classical electrodynamics, while capturing quantum plasmonic aspects......Quantum effects of plasmonic phenomena have been explored through ab initio studies, but only for exceedingly small metallic nanostructures, leaving most experimentally relevant structures too large to handle. We propose instead an effective description with the computationally appealing features...

SU-E-T-191: First Principle Calculation of Quantum Yield in Photodynamic Therapy

Energy Technology Data Exchange (ETDEWEB)

Abolfath, R; Guo, F; Chen, Z; Nath, R [Yale New Haven Hospital, New Haven, CT (United States)

2014-06-01

Purpose: We present a first-principle method to calculate the spin transfer efficiency in oxygen induced by any photon fields especially in MeV energy range. The optical pumping is mediated through photosensitizers, e.g., porphyrin and/or ensemble of quantum dots. Methods: Under normal conditions, oxygen molecules are in the relatively non-reactive triplet state. In the presence of certain photosensitizer compounds such as porphyrins, electromagnetic radiation of specific wavelengths can excite oxygen to highly reactive singlet state. With selective uptake of photosensitizers by certain malignant cells, photon irradiation of phosensitized tumors can lead to selective killing of cancer cells. This is the basis of photodynamic therapy (PDT). Despite several attempts, PDT has not been clinically successful except in limited superficial cancers. Many parameters such as photon energy, conjugation with quantum dots etc. can be potentially combined with PDT in order to extend the role of PDT in cancer management. The key quantity for this optimization is the spin transfer efficiency in oxygen by any photon field. The first principle calculation model presented here, is an attempt to fill this need. We employ stochastic density matrix description of the quantum jumps and the rate equation methods in quantum optics based on Markov/Poisson processes and calculate time evolution of the population of the optically pumped singlet oxygen. Results: The results demonstrate the feasibility of our model in showing the dependence of the optical yield in generating spin-singlet oxygen on the experimental conditions. The adjustable variables can be tuned to maximize the population of the singlet oxygen hence the efficacy of the photodynamic therapy. Conclusion: The present model can be employed to fit and analyze the experimental data and possibly to assist researchers in optimizing the experimental conditions in photodynamic therapy.

Spin relaxation in quantum dots due to electron exchange with leads.

Science.gov (United States)

Vorontsov, A B; Vavilov, M G

2008-11-28

We calculate spin relaxation rates in lateral quantum dot systems due to electron exchange between dots and leads. Using rate equations, we develop a theoretical description of the experimentally observed electric current in the spin blockade regime of double quantum dots. A single expression fits the entire current profile and describes the structure of both the conduction peaks and the suppressed ("valley") region. Extrinsic rates calculated here have to be taken into account for accurate extraction of intrinsic relaxation rates due to the spin-orbit and hyperfine spin scattering mechanisms from spin blockade measurements.

Annular tautomerism: experimental observations and quantum mechanics calculations

Science.gov (United States)

Cruz-Cabeza, Aurora J.; Schreyer, Adrian; Pitt, William R.

2010-06-01

The use of MP2 level quantum mechanical (QM) calculations on isolated heteroaromatic ring systems for the prediction of the tautomeric propensities of whole molecules in a crystalline environment was examined. A Polarisable Continuum Model was used in the calculations to account for environment effects on the tautomeric relative stabilities. The calculated relative energies of tautomers were compared to relative abundances within the Cambridge Structural Database (CSD) and the Protein Data Bank (PDB). The work was focussed on 84 annular tautomeric forms of 34 common ring systems. Good agreement was found between the calculations and the experimental data even if the quantity of these data was limited in many cases. The QM results were compared to those produced by much faster semiempirical calculations. In a search for other sources of the useful experimental data, the relative numbers of known compounds in which prototropic positions were often substituted by heavy atoms were also analysed. A scheme which groups all annular tautomeric transformations into 10 classes was developed. The scheme was designed to encompass a comprehensive set of known and theoretically possible tautomeric ring systems generated as part of a previous study. General trends across analogous ring systems were detected as a result. The calculations and statistics collected on crystallographic data as well as the general trends observed should be useful for the better modelling of annular tautomerism in the applications such as computer-aided drug design, small molecule crystal structure prediction, the naming of compounds and the interpretation of protein—small molecule crystal structures.

The Excited Electronic States Calculated for Cd1−xZnxS Quantum Dots Grown by the Sol-Gel Technique

Directory of Open Access Journals (Sweden)

A. Sakly

2010-01-01

Full Text Available The present paper is aimed to investigate theoretically the quantum confinement in Cd1−xZnxS-related quantum dots with x the atomic fraction of Zn. For both electrons and holes, we have calculated the excited bound states with use of the spherical geometry model and assuming a finite potential at the boundary. For electrons, calculations were made by using Bessel function as an orthonormal basis. However, for holes, the confined subbands have been calculated based on squared quantum well envelope wave functions. The subband energies were evaluated for both electrons and holes versus zinc composition as well.

On calculations of the ground state energy in quantum mechanics

International Nuclear Information System (INIS)

Efimov, G.V.

1991-02-01

In nonrelativistic quantum mechanics the Wick-ordering method called the oscillator representation suggested to calculate the ground-state energy for a wide class of potentials allowing the existence of a bound state. The following examples are considered: the orbital excitations of the ground-state in the Coulomb plus linear potential, the Schroedinger equation with a ''relativistic'' kinetic energy √p 2 +m 2 , the Coulomb three-body problem. (author). 22 refs, 2 tabs

Accurate reconstruction of the jV-characteristic of organic solar cells from measurements of the external quantum efficiency

Science.gov (United States)

Meyer, Toni; Körner, Christian; Vandewal, Koen; Leo, Karl

2018-04-01

In two terminal tandem solar cells, the current density - voltage (jV) characteristic of the individual subcells is typically not directly measurable, but often required for a rigorous device characterization. In this work, we reconstruct the jV-characteristic of organic solar cells from measurements of the external quantum efficiency under applied bias voltages and illumination. We show that it is necessary to perform a bias irradiance variation at each voltage and subsequently conduct a mathematical correction of the differential to the absolute external quantum efficiency to obtain an accurate jV-characteristic. Furthermore, we show that measuring the external quantum efficiency as a function of voltage for a single bias irradiance of 0.36 AM1.5g equivalent sun provides a good approximation of the photocurrent density over voltage curve. The method is tested on a selection of efficient, common single-junctions. The obtained conclusions can easily be transferred to multi-junction devices with serially connected subcells.

Calculation of quantum-mechanical system energy spectra using path integrals

International Nuclear Information System (INIS)

Evseev, A.M.; Dmitriev, V.P.

1977-01-01

A solution of the Feynman quantum-mechanical integral connecting a wave function (psi (x, t)) at a moment t+tau (tau → 0) with the wave function at the moment t is provided by complex variable substitution and subsequent path integration. Time dependence of the wave function is calculated by the Monte Carlo method. The Fourier inverse transformation of the wave function by path integration calculated has been applied to determine the energy spectra. Energy spectra are presented of a hydrogen atom derived from wave function psi (x, t) at different x, as well as boson energy spectra of He, Li, and Be atoms obtained from psi (x, t) at X = O

Water dissociating on rigid Ni(100): A quantum dynamics study on a full-dimensional potential energy surface

Science.gov (United States)

Liu, Tianhui; Chen, Jun; Zhang, Zhaojun; Shen, Xiangjian; Fu, Bina; Zhang, Dong H.

2018-04-01

We constructed a nine-dimensional (9D) potential energy surface (PES) for the dissociative chemisorption of H2O on a rigid Ni(100) surface using the neural network method based on roughly 110 000 energies obtained from extensive density functional theory (DFT) calculations. The resulting PES is accurate and smooth, based on the small fitting errors and the good agreement between the fitted PES and the direct DFT calculations. Time dependent wave packet calculations also showed that the PES is very well converged with respect to the fitting procedure. The dissociation probabilities of H2O initially in the ground rovibrational state from 9D quantum dynamics calculations are quite different from the site-specific results from the seven-dimensional (7D) calculations, indicating the importance of full-dimensional quantum dynamics to quantitatively characterize this gas-surface reaction. It is found that the validity of the site-averaging approximation with exact potential holds well, where the site-averaging dissociation probability over 15 fixed impact sites obtained from 7D quantum dynamics calculations can accurately approximate the 9D dissociation probability for H2O in the ground rovibrational state.

Quantum Monte Carlo for vibrating molecules

International Nuclear Information System (INIS)

Brown, W.R.; Lawrence Berkeley National Lab., CA

1996-08-01

Quantum Monte Carlo (QMC) has successfully computed the total electronic energies of atoms and molecules. The main goal of this work is to use correlation function quantum Monte Carlo (CFQMC) to compute the vibrational state energies of molecules given a potential energy surface (PES). In CFQMC, an ensemble of random walkers simulate the diffusion and branching processes of the imaginary-time time dependent Schroedinger equation in order to evaluate the matrix elements. The program QMCVIB was written to perform multi-state VMC and CFQMC calculations and employed for several calculations of the H 2 O and C 3 vibrational states, using 7 PES's, 3 trial wavefunction forms, two methods of non-linear basis function parameter optimization, and on both serial and parallel computers. In order to construct accurate trial wavefunctions different wavefunctions forms were required for H 2 O and C 3 . In order to construct accurate trial wavefunctions for C 3 , the non-linear parameters were optimized with respect to the sum of the energies of several low-lying vibrational states. In order to stabilize the statistical error estimates for C 3 the Monte Carlo data was collected into blocks. Accurate vibrational state energies were computed using both serial and parallel QMCVIB programs. Comparison of vibrational state energies computed from the three C 3 PES's suggested that a non-linear equilibrium geometry PES is the most accurate and that discrete potential representations may be used to conveniently determine vibrational state energies

Evaluation of carbohydrate molecular mechanical force fields by quantum mechanical calculations

DEFF Research Database (Denmark)

Hemmingsen, Lars Bo Stegeager; Madsen, D.E.; Esbensen, A.L.

2004-01-01

of the (gg, gt and tg) rotamers of methyl alpha-D-glucopyranoside and methyl alpha-D-galactopyranoside are (0.13, 0.00, 0.15) and (0.64, 0.00, 0.77) kcal/mol. respectively. The results of the quantum mechanical calculations are compared with the results of calculations using the 20 second...... for monosaccharide carbohydrate benchmark systems. Selected results are: (i) The interaction energy of the alpha-D-alucopyranose-H2O heterodimer is estimated to be 4.9 kcal/mol, using a composite method including terms at highly correlated (CCSD(T)) level. Most molecular mechanics force fields are in error...

Accurate heterogeneous dose calculation for lung cancer patients without high‐resolution CT densities

Science.gov (United States)

Li, Jonathan G.; Liu, Chihray; Olivier, Kenneth R.; Dempsey, James F.

2009-01-01

The aim of this study was to investigate the relative accuracy of megavoltage photon‐beam dose calculations employing either five bulk densities or independent voxel densities determined by calibration of the CT Houndsfield number. Full‐resolution CT and bulk density treatment plans were generated for 70 lung or esophageal cancer tumors (66 cases) using a commercial treatment planning system with an adaptive convolution dose calculation algorithm (Pinnacle3, Philips Medicals Systems). Bulk densities were applied to segmented regions. Individual and population average densities were compared to the full‐resolution plan for each case. Monitor units were kept constant and no normalizations were employed. Dose volume histograms (DVH) and dose difference distributions were examined for all cases. The average densities of the segmented air, lung, fat, soft tissue, and bone for the entire set were found to be 0.14, 0.26, 0.89, 1.02, and 1.12 g/cm3, respectively. In all cases, the normal tissue DVH agreed to better than 2% in dose. In 62 of 70 DVHs of the planning target volume (PTV), agreement to better than 3% in dose was observed. Six cases demonstrated emphysema, one with bullous formations and one with a hiatus hernia having a large volume of gas. These required the additional assignment of density to the emphysemic lung and inflammatory changes to the lung, the regions of collapsed lung, the bullous formations, and the hernia gas. Bulk tissue density dose calculation provides an accurate method of heterogeneous dose calculation. However, patients with advanced emphysema may require high‐resolution CT studies for accurate treatment planning. PACS number: 87.53.Tf

ACCURATELY CALCULATING THE SOLAR ORIENTATION OF THE TIANGONG-2 ULTRAVIOLET FORWARD SPECTROMETER

Directory of Open Access Journals (Sweden)

Z. Liu

2018-04-01

Full Text Available The Ultraviolet Forward Spectrometer is a new type of spectrometer for monitoring the vertical distribution of atmospheric trace gases in the global middle atmosphere. It is on the TianGong-2 space laboratory, which was launched on 15 September 2016. The spectrometer uses a solar calibration mode to modify its irradiance. Accurately calculating the solar orientation is a prerequisite of spectral calibration for the Ultraviolet Forward Spectrometer. In this paper, a method of calculating the solar orientation is proposed according to the imaging geometric characteristics of the spectrometer. Firstly, the solar orientation in the horizontal rectangular coordinate system is calculated based on the solar declination angle algorithm proposed by Bourges and the solar hour angle algorithm proposed by Lamm. Then, the solar orientation in the sensor coordinate system is achieved through several coordinate system transforms. Finally, we calculate the solar orientation in the sensor coordinate system and evaluate its calculation accuracy using actual orbital data of TianGong-2. The results show that the accuracy is close to the simulation method with STK (Satellite Tool Kit, and the error is not more than 2 %. The algorithm we present does not need a lot of astronomical knowledge, but only needs some observation parameters provided by TianGong-2.

Density Functional Theory Calculations of the Quantum Capacitance of Graphene Oxide as a Supercapacitor Electrode.

Science.gov (United States)

Song, Ce; Wang, Jinyan; Meng, Zhaoliang; Hu, Fangyuan; Jian, Xigao

2018-03-31

Graphene oxide has become an attractive electrode-material candidate for supercapacitors thanks to its higher specific capacitance compared to graphene. The quantum capacitance makes relative contributions to the specific capacitance, which is considered as the major limitation of graphene electrodes, while the quantum capacitance of graphene oxide is rarely concerned. This study explores the quantum capacitance of graphene oxide, which bears epoxy and hydroxyl groups on its basal plane, by employing density functional theory (DFT) calculations. The results demonstrate that the total density of states near the Fermi level is significantly enhanced by introducing oxygen-containing groups, which is beneficial for the improvement of the quantum capacitance. Moreover, the quantum capacitances of the graphene oxide with different concentrations of these two oxygen-containing groups are compared, revealing that more epoxy and hydroxyl groups result in a higher quantum capacitance. Notably, the hydroxyl concentration has a considerable effect on the capacitive behavior. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Time-Dependent Wave Packet Dynamics Calculations of Cross Sections for Ultracold Scattering of Molecules

Science.gov (United States)

Huang, Jiayu; Liu, Shu; Zhang, Dong H.; Krems, Roman V.

2018-04-01

Because the de Broglie wavelength of ultracold molecules is very large, the cross sections for collisions of molecules at ultracold temperatures are always computed by the time-independent quantum scattering approach. Here, we report the first accurate time-dependent wave packet dynamics calculation for reactive scattering of ultracold molecules. Wave packet dynamics calculations can be applied to molecular systems with more dimensions and provide real-time information on the process of bond rearrangement and/or energy exchange in molecular collisions. Our work thus makes possible the extension of rigorous quantum calculations of ultracold reaction properties to polyatomic molecules and adds a new powerful tool for the study of ultracold chemistry.

Efficiency of free-energy calculations of spin lattices by spectral quantum algorithms

International Nuclear Information System (INIS)

Master, Cyrus P.; Yamaguchi, Fumiko; Yamamoto, Yoshihisa

2003-01-01

Ensemble quantum algorithms are well suited to calculate estimates of the energy spectra for spin-lattice systems. Based on the phase estimation algorithm, these algorithms efficiently estimate discrete Fourier coefficients of the density of states. Their efficiency in calculating the free energy per spin of general spin lattices to bounded error is examined. We find that the number of Fourier components required to bound the error in the free energy due to the broadening of the density of states scales polynomially with the number of spins in the lattice. However, the precision with which the Fourier components must be calculated is found to be an exponential function of the system size

Calculation of accurate albedo boundary conditions for three-dimensional nodal diffusion codes by the method of characteristics

International Nuclear Information System (INIS)

Petkov, Petko T.

2000-01-01

Most of the few-group three-dimensional nodal diffusion codes used for neutronics calculations of the WWER reactors use albedo type boundary conditions on the core-reflector boundary. The conventional albedo are group-to-group reflection probabilities, defined on each outer node face. The method of characteristics is used to calculate accurate albedo by the following procedure. A many-group two-dimensional heterogeneous core-reflector problem, including a sufficient part of the core and detailed description of the adjacent reflector, is solved first. From this solution the angular flux on the core-reflector boundary is calculated in all groups for all traced neutron directions. Accurate boundary conditions can be calculated for the radial, top and bottom reflectors as well as for the absorber part of the WWER-440 reactor control assemblies. The algorithm can be used to estimate also albedo, coupling outer node faces on the radial reflector in the axial direction. Numerical results for the WWER-440 reactor are presented. (Authors)

Dynamical basis sets for algebraic variational calculations in quantum-mechanical scattering theory

Science.gov (United States)

Sun, Yan; Kouri, Donald J.; Truhlar, Donald G.; Schwenke, David W.

1990-01-01

New basis sets are proposed for linear algebraic variational calculations of transition amplitudes in quantum-mechanical scattering problems. These basis sets are hybrids of those that yield the Kohn variational principle (KVP) and those that yield the generalized Newton variational principle (GNVP) when substituted in Schlessinger's stationary expression for the T operator. Trial calculations show that efficiencies almost as great as that of the GNVP and much greater than the KVP can be obtained, even for basis sets with the majority of the members independent of energy.

A more accurate scheme for calculating Earth's skin temperature

Science.gov (United States)

Tsuang, Ben-Jei; Tu, Chia-Ying; Tsai, Jeng-Lin; Dracup, John A.; Arpe, Klaus; Meyers, Tilden

2009-02-01

The theoretical framework of the vertical discretization of a ground column for calculating Earth’s skin temperature is presented. The suggested discretization is derived from the evenly heat-content discretization with the optimal effective thickness for layer-temperature simulation. For the same level number, the suggested discretization is more accurate in skin temperature as well as surface ground heat flux simulations than those used in some state-of-the-art models. A proposed scheme (“op(3,2,0)”) can reduce the normalized root-mean-square error (or RMSE/STD ratio) of the calculated surface ground heat flux of a cropland site significantly to 2% (or 0.9 W m-2), from 11% (or 5 W m-2) by a 5-layer scheme used in ECMWF, from 19% (or 8 W m-2) by a 5-layer scheme used in ECHAM, and from 74% (or 32 W m-2) by a single-layer scheme used in the UCLA GCM. Better accuracy can be achieved by including more layers to the vertical discretization. Similar improvements are expected for other locations with different land types since the numerical error is inherited into the models for all the land types. The proposed scheme can be easily implemented into state-of-the-art climate models for the temperature simulation of snow, ice and soil.

Vibrational spectra of halide-water dimers: Insights on ion hydration from full-dimensional quantum calculations on many-body potential energy surfaces

Science.gov (United States)

Bajaj, Pushp; Wang, Xiao-Gang; Carrington, Tucker; Paesani, Francesco

2018-03-01

Full-dimensional vibrational spectra are calculated for both X-(H2O) and X-(D2O) dimers (X = F, Cl, Br, I) at the quantum-mechanical level. The calculations are carried out on two sets of recently developed potential energy functions (PEFs), namely, Thole-type model energy (TTM-nrg) and many-body energy (MB-nrg), using the symmetry-adapted Lanczos algorithm with a product basis set including all six vibrational coordinates. Although both TTM-nrg and MB-nrg PEFs are derived from coupled-cluster single double triple-F12 data obtained in the complete basis set limit, they differ in how many-body effects are represented at short range. Specifically, while both models describe long-range interactions through the combination of two-body dispersion and many-body classical electrostatics, the relatively simple Born-Mayer functions employed in the TTM-nrg PEFs to represent short-range interactions are replaced in the MB-nrg PEFs by permutationally invariant polynomials to achieve chemical accuracy. For all dimers, the MB-nrg vibrational spectra are in close agreement with the available experimental data, correctly reproducing anharmonic and nuclear quantum effects. In contrast, the vibrational frequencies calculated with the TTM-nrg PEFs exhibit significant deviations from the experimental values. The comparison between the TTM-nrg and MB-nrg results thus reinforces the notion that an accurate representation of both short-range interactions associated with electron density overlap and long-range many-body electrostatic interactions is necessary for a correct description of hydration phenomena at the molecular level.

Highly Accurate Calculations of the Phase Diagram of Cold Lithium

Science.gov (United States)

Shulenburger, Luke; Baczewski, Andrew

The phase diagram of lithium is particularly complicated, exhibiting many different solid phases under the modest application of pressure. Experimental efforts to identify these phases using diamond anvil cells have been complemented by ab initio theory, primarily using density functional theory (DFT). Due to the multiplicity of crystal structures whose enthalpy is nearly degenerate and the uncertainty introduced by density functional approximations, we apply the highly accurate many-body diffusion Monte Carlo (DMC) method to the study of the solid phases at low temperature. These calculations span many different phases, including several with low symmetry, demonstrating the viability of DMC as a method for calculating phase diagrams for complex solids. Our results can be used as a benchmark to test the accuracy of various density functionals. This can strengthen confidence in DFT based predictions of more complex phenomena such as the anomalous melting behavior predicted for lithium at high pressures. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. DOE's National Nuclear Security Administration under contract DE-AC04-94AL85000.

The over-barrier resonant states and multi-channel scattering by a quantum well

Directory of Open Access Journals (Sweden)

Alexander F. Polupanov

2008-06-01

Full Text Available We demonstrate an explicit numerical method for accurate calculation ofthe analytic continuation of the scattering matrix, describing the multichannelscattering by a quantum well, to the unphysical region of complexvalues of the energy. Results of calculations show that one or severalpoles of the S-matrix exist, corresponding to the over-barrier resonantstates that are critical for the effect of the absolute reflection at scatteringof the heavy hole by a quantum well in the energy range where only theheavy hole may propagate over barriers in a quantum-well structure.Light- and heavy-hole states are described by the Luttinger Hamiltonianmatrix. The qualitative behaviour of the over-barrier scattering andresonant states is the same at variation of the shape of the quantum-wellpotential, however lifetimes of resonant states depend drastically on theshape and depth of a quantum well.

Young’s modulus calculations for cellulose Iß by MM3 and quantum mechanics

Science.gov (United States)

Quantum mechanics (QM) and molecular mechanics (MM) calculations were performed to elucidate Young’s moduli for a series of cellulose Iß models. Computations using the second generation empirical force field MM3 with a disaccharide cellulose model, 1,4'-O-dimethyl-ß-cellobioside (DMCB), and an analo...

Generalized Bloch Theorem for Complex Periodic Potentials - A Powerful Application to Quantum Transport Calculations

International Nuclear Information System (INIS)

Zhang, Xiaoguang; Varga, Kalman; Pantelides, Sokrates T

2007-01-01

Band-theoretic methods with periodically repeated supercells have been a powerful approach for ground-state electronic structure calculations, but have not so far been adapted for quantum transport problems with open boundary conditions. Here we introduce a generalized Bloch theorem for complex periodic potentials and use a transfer-matrix formulation to cast the transmission probability in a scattering problem with open boundary conditions in terms of the complex wave vectors of a periodic system with absorbing layers, allowing a band technique for quantum transport calculations. The accuracy and utility of the method is demonstrated by the model problems of the transmission of an electron over a square barrier and the scattering of a phonon in an inhomogeneous nanowire. Application to the resistance of a twin boundary in nanocrystalline copper yields excellent agreement with recent experimental data

An extrapolation scheme for solid-state NMR chemical shift calculations

Science.gov (United States)

Nakajima, Takahito

2017-06-01

Conventional quantum chemical and solid-state physical approaches include several problems to accurately calculate solid-state nuclear magnetic resonance (NMR) properties. We propose a reliable computational scheme for solid-state NMR chemical shifts using an extrapolation scheme that retains the advantages of these approaches but reduces their disadvantages. Our scheme can satisfactorily yield solid-state NMR magnetic shielding constants. The estimated values have only a small dependence on the low-level density functional theory calculation with the extrapolation scheme. Thus, our approach is efficient because the rough calculation can be performed in the extrapolation scheme.

Quantum Nuclear Extension of Electron Nuclear Dynamics on Folded Effective-Potential Surfaces

DEFF Research Database (Denmark)

Hall, B.; Deumens, E.; Ohrn, Y.

2014-01-01

A perennial problem in quantum scattering calculations is accurate theoretical treatment of low energy collisions. We propose a method of extracting a folded, nonadiabatic, effective potential energy surface from electron nuclear dynamics (END) trajectories; we then perform nuclear wave packet...

Optimization of extracranial stereotactic radiation therapy of small lung lesions using accurate dose calculation algorithms

International Nuclear Information System (INIS)

Dobler, Barbara; Walter, Cornelia; Knopf, Antje; Fabri, Daniella; Loeschel, Rainer; Polednik, Martin; Schneider, Frank; Wenz, Frederik; Lohr, Frank

2006-01-01

The aim of this study was to compare and to validate different dose calculation algorithms for the use in radiation therapy of small lung lesions and to optimize the treatment planning using accurate dose calculation algorithms. A 9-field conformal treatment plan was generated on an inhomogeneous phantom with lung mimics and a soft tissue equivalent insert, mimicking a lung tumor. The dose distribution was calculated with the Pencil Beam and Collapsed Cone algorithms implemented in Masterplan (Nucletron) and the Monte Carlo system XVMC and validated using Gafchromic EBT films. Differences in dose distribution were evaluated. The plans were then optimized by adding segments to the outer shell of the target in order to increase the dose near the interface to the lung. The Pencil Beam algorithm overestimated the dose by up to 15% compared to the measurements. Collapsed Cone and Monte Carlo predicted the dose more accurately with a maximum difference of -8% and -3% respectively compared to the film. Plan optimization by adding small segments to the peripheral parts of the target, creating a 2-step fluence modulation, allowed to increase target coverage and homogeneity as compared to the uncorrected 9 field plan. The use of forward 2-step fluence modulation in radiotherapy of small lung lesions allows the improvement of tumor coverage and dose homogeneity as compared to non-modulated treatment plans and may thus help to increase the local tumor control probability. While the Collapsed Cone algorithm is closer to measurements than the Pencil Beam algorithm, both algorithms are limited at tissue/lung interfaces, leaving Monte-Carlo the most accurate algorithm for dose prediction

Quantum-Mechanical Calculations on Molecular Substructures Involved in Nanosystems

Directory of Open Access Journals (Sweden)

Beata Szefler

2014-09-01

Full Text Available In this review article, four ideas are discussed: (a aromaticity of fullerenes patched with flowers of 6-and 8-membered rings, optimized at the HF and DFT levels of theory, in terms of HOMA and NICS criteria; (b polybenzene networks, from construction to energetic and vibrational spectra computations; (c quantum-mechanical calculations on the repeat units of various P-type crystal networks and (d construction and stability evaluation, at DFTB level of theory, of some exotic allotropes of diamond D5, involved in hyper-graphenes. The overall conclusion was that several of the yet hypothetical molecular nanostructures herein described are serious candidates to the status of real molecules.

Quantum synchrotron spectra from semirelativistic electrons in teragauss magnetic fields

International Nuclear Information System (INIS)

Brainerd, J.J.

1987-01-01

Synchrotron spectra are calculated from quantum electrodynamic transition rates for thermal and power-law electron distributions. It is shown that quantum effects appear in thermal spectra when the photon energy is greater than the electron temperature, and in power-law spectra when the electron energy in units of the electron rest mass times the magnetic field strength in units of the critical field strength is of order unity. These spectra are compared with spectra calculated from the ultrarelativistic approximation for synchrotron emission. It is found that the approximation for the power-law spectra is good, and the approximation for thermal spectra produces the shape of the spectrum accurately but fails to give the correct normalization. Single photon pair creation masks the quantum effects for power-law distributions, so only modifications to thermal spectra are important for gamma-ray bursts. 13 references

A matter of quantum voltages

Energy Technology Data Exchange (ETDEWEB)

Sellner, Bernhard; Kathmann, Shawn M., E-mail: Shawn.Kathmann@pnnl.gov [Physical Sciences Division, Pacific Northwest National Laboratory, Richland, Washington 99352 (United States)

2014-11-14

Voltages inside matter are relevant to crystallization, materials science, biology, catalysis, and aqueous chemistry. The variation of voltages in matter can be measured by experiment, however, modern supercomputers allow the calculation of accurate quantum voltages with spatial resolutions of bulk systems well beyond what can currently be measured provided a sufficient level of theory is employed. Of particular interest is the Mean Inner Potential (V{sub o}) – the spatial average of these quantum voltages referenced to the vacuum. Here we establish a protocol to reliably evaluate V{sub o} from quantum calculations. Voltages are very sensitive to the distribution of electrons and provide metrics to understand interactions in condensed phases. In the present study, we find excellent agreement with measurements of V{sub o} for vitrified water and salt crystals and demonstrate the impact of covalent and ionic bonding as well as intermolecular/atomic interactions. Certain aspects in this regard are highlighted making use of simple model systems/approximations. Furthermore, we predict V{sub o} as well as the fluctuations of these voltages in aqueous NaCl electrolytes and characterize the changes in their behavior as the resolution increases below the size of atoms.

Thermoelectric transport through quantum dots

Energy Technology Data Exchange (ETDEWEB)

Merker, Lukas Heinrich

2016-06-30

In this thesis the thermoelectric properties (electrical conductance, Seebeck coefficient and thermal conductance)of quantum dots described by the Anderson impurity model have been investigated by using the numerical renormalization group (NRG) method. In order to make accurate calculations for thermoelectric properties of quantum impurity systems, a number of recent developments and refinements of the NRG have been implemented. These include the z-averaging and Campo discretization scheme, which enable the evaluation of physical quantities on an arbitrary temperature grid and at large discretization parameter Λ and the full density matrix (FDM) approach, which allows a more accurate calculation of spectral functions and transport coefficients. The implementation of the z-averaging and Campo discretization scheme has been tested within a new method for specific heats of quantum impurities. The accuracy of this new method was established by comparison with the numerical solution of the Bethe-ansatz equations for the Anderson model. The FDM approach was implemented and tested within a new approach to the calculation of impurity contributions to the uniform susceptibilities. Within this method a non-negligible contribution from the ''environmental'' degrees of freedom needs to be taken into account to recover the correct susceptibility, as shown by comparison with the Bethe-ansatz approach. An accurate method to calculate the conductance of a quantum dot is implemented, enabling the extraction of the Fermi liquid scaling coefficients c{sub T} and c{sub B} to high accuracy, being able to verify the results of the renormalized super perturbation theory approach (within its regime of validity). The method was generalized to higher order moments of the local level spectral function. This, as well as reduction of the SU(2) code to the U(1) symmetry, enabled the investigation of the effect of a magnetic field on the thermoelectric properties of quantum

Lowest vibrational states of 4He3He+: Non-Born-Oppenheimer calculations

International Nuclear Information System (INIS)

Stanke, Monika; Bubin, Sergiy; Kedziera, Dariusz; Molski, Marcin; Adamowicz, Ludwik

2007-01-01

Very accurate quantum mechanical calculations of the first five vibrational states of the 4 He 3 He + molecular ion are reported. The calculations have been performed explicitly including the coupling of the electronic and nuclear motions [i.e., without assuming the Born-Oppenheimer (BO) approximation]. The nonrelativistic non-BO wave functions were used to calculate the α 2 relativistic mass velocity, Darwin, and spin-spin interaction corrections. For the lowest vibrational transition, whose experimental energy is established with high precision, the calculated and the experimental results differ by only 0.16 cm -1

Accurate Bit Error Rate Calculation for Asynchronous Chaos-Based DS-CDMA over Multipath Channel

Science.gov (United States)

Kaddoum, Georges; Roviras, Daniel; Chargé, Pascal; Fournier-Prunaret, Daniele

2009-12-01

An accurate approach to compute the bit error rate expression for multiuser chaosbased DS-CDMA system is presented in this paper. For more realistic communication system a slow fading multipath channel is considered. A simple RAKE receiver structure is considered. Based on the bit energy distribution, this approach compared to others computation methods existing in literature gives accurate results with low computation charge. Perfect estimation of the channel coefficients with the associated delays and chaos synchronization is assumed. The bit error rate is derived in terms of the bit energy distribution, the number of paths, the noise variance, and the number of users. Results are illustrated by theoretical calculations and numerical simulations which point out the accuracy of our approach.

Quantum density fluctuations in liquid neon from linearized path-integral calculations

International Nuclear Information System (INIS)

Poulsen, Jens Aage; Scheers, Johan; Nyman, Gunnar; Rossky, Peter J.

2007-01-01

The Feynman-Kleinert linearized path-integral [J. A. Poulsen et al., J. Chem. Phys. 119, 12179 (2003)] representation of quantum correlation functions is applied to compute the spectrum of density fluctuations for liquid neon at T=27.6 K, p=1.4 bar, and Q vector 1.55 Aa -1 . The calculated spectrum as well as the kinetic energy of the liquid are in excellent agreement with the experiment of Cunsolo et al. [Phys. Rev. B 67, 024507 (2003)

Accelerating atomistic calculations of quantum energy eigenstates on graphic cards

Science.gov (United States)

Rodrigues, Walter; Pecchia, A.; Lopez, M.; Auf der Maur, M.; Di Carlo, A.

2014-10-01

Electronic properties of nanoscale materials require the calculation of eigenvalues and eigenvectors of large matrices. This bottleneck can be overcome by parallel computing techniques or the introduction of faster algorithms. In this paper we report a custom implementation of the Lanczos algorithm with simple restart, optimized for graphical processing units (GPUs). The whole algorithm has been developed using CUDA and runs entirely on the GPU, with a specialized implementation that spares memory and reduces at most machine-to-device data transfers. Furthermore parallel distribution over several GPUs has been attained using the standard message passing interface (MPI). Benchmark calculations performed on a GaN/AlGaN wurtzite quantum dot with up to 600,000 atoms are presented. The empirical tight-binding (ETB) model with an sp3d5s∗+spin-orbit parametrization has been used to build the system Hamiltonian (H).

Toward an accurate description of solid-state properties of superheavy elements

Directory of Open Access Journals (Sweden)

Schwerdtfeger Peter

2016-01-01

Full Text Available In the last two decades cold and hot fusion experiments lead to the production of new elements for the Periodic Table up to nuclear charge 118. Recent developments in relativistic quantum theory have made it possible to obtain accurate electronic properties for the trans-actinide elements with the aim to predict their potential chemical and physical behaviour. Here we report on first results of solid-state calculations for Og (element 118 to support future atom-at-a-time gas-phase adsorption experiments on surfaces such as gold or quartz.

Correlation functions for fully or partially state-resolved reactive scattering calculations

International Nuclear Information System (INIS)

Manthe, Uwe; Welsch, Ralph

2014-01-01

Flux correlation functions and the quantum transition state concept are important tools for the accurate description of polyatomic reaction processes. Combined with the multi-configurational time-dependent Hartree approach, they facilitate rigorous full-dimensional calculations of cumulative and initial-state selected reaction probabilities for six atom reactions. In recent work [R. Welsch, F. Huarte-Larrañaga, and U. Manthe, J. Chem. Phys. 136, 064117 (2012)], an approach which allows one to calculate also state-to-state reaction probabilities within the quantum transition state concept has been introduced. This article presents further developments. Alternative generalized flux correlation functions are introduced and discussed. Equations for the calculation of fully state-resolved differential cross section using arbitrary definitions of the body fixed frame are derived. An approach for the efficient calculation of partially state-resolved observables as a function of the collision energy is introduced. Finally, numerical test studying the D + H 2 reaction illustrate important aspects of the formalism

Quantum Electrodynamical Shifts in Multivalent Heavy Ions.

Science.gov (United States)

Tupitsyn, I I; Kozlov, M G; Safronova, M S; Shabaev, V M; Dzuba, V A

2016-12-16

The quantum electrodynamics (QED) corrections are directly incorporated into the most accurate treatment of the correlation corrections for ions with complex electronic structure of interest to metrology and tests of fundamental physics. We compared the performance of four different QED potentials for various systems to access the accuracy of QED calculations and to make a prediction of highly charged ion properties urgently needed for planning future experiments. We find that all four potentials give consistent and reliable results for ions of interest. For the strongly bound electrons, the nonlocal potentials are more accurate than the local potential.

Quantum treatment of protons with the reduced explicitly correlated Hartree-Fock approach

Energy Technology Data Exchange (ETDEWEB)

Sirjoosingh, Andrew; Pak, Michael V.; Brorsen, Kurt R.; Hammes-Schiffer, Sharon, E-mail: shs3@illinois.edu [Department of Chemistry, University of Illinois at Urbana-Champaign, 600 South Mathews Ave., Urbana, Illinois 61801 (United States)

2015-06-07

The nuclear-electronic orbital (NEO) approach treats select nuclei quantum mechanically on the same level as the electrons and includes nonadiabatic effects between the electrons and the quantum nuclei. The practical implementation of this approach is challenging due to the significance of electron-nucleus dynamical correlation. Herein, we present a general extension of the previously developed reduced NEO explicitly correlated Hartree-Fock (RXCHF) approach, in which only select electronic orbitals are explicitly correlated to each quantum nuclear orbital via Gaussian-type geminal functions. Approximations of the electronic exchange between the geminal-coupled electronic orbitals and the other electronic orbitals are also explored. This general approach enables computationally tractable yet accurate calculations on molecular systems with quantum protons. The RXCHF method is applied to the hydrogen cyanide (HCN) and FHF{sup −} systems, where the proton and all electrons are treated quantum mechanically. For the HCN system, only the two electronic orbitals associated with the CH covalent bond are geminal-coupled to the proton orbital. For the FHF{sup −} system, only the four electronic orbitals associated with the two FH covalent bonds are geminal-coupled to the proton orbital. For both systems, the RXCHF method produces qualitatively accurate nuclear densities, in contrast to mean field-based NEO approaches. The development and implementation of the RXCHF method provide the framework to perform calculations on systems such as proton-coupled electron transfer reactions, where electron-proton nonadiabatic effects are important.

Quantum Computations: Fundamentals and Algorithms

International Nuclear Information System (INIS)

Duplij, S.A.; Shapoval, I.I.

2007-01-01

Basic concepts of quantum information theory, principles of quantum calculations and the possibility of creation on this basis unique on calculation power and functioning principle device, named quantum computer, are concerned. The main blocks of quantum logic, schemes of quantum calculations implementation, as well as some known today effective quantum algorithms, called to realize advantages of quantum calculations upon classical, are presented here. Among them special place is taken by Shor's algorithm of number factorization and Grover's algorithm of unsorted database search. Phenomena of decoherence, its influence on quantum computer stability and methods of quantum errors correction are described

Ab initio calculation of transport properties between PbSe quantum dots facets with iodide ligands

Science.gov (United States)

Wang, B.; Patterson, R.; Chen, W.; Zhang, Z.; Yang, J.; Huang, S.; Shrestha, S.; Conibeer, G.

2018-01-01

The transport properties between Lead Selenide (PbSe) quantum dots decorated with iodide ligands has been studied using density functional theory (DFT). Quantum conductance at each selected energy levels has been calculated along with total density of states and projected density of states. The DFT calculation is carried on using a grid-based planar augmented wave (GPAW) code incorporated with the linear combination of atomic orbital (LCAO) mode and Perdew Burke Ernzerhof (PBE) exchange-correlation functional. Three iodide ligand attached low index facets including (001), (011), (111) are investigated in this work. P-orbital of iodide ligand majorly contributes to density of state (DOS) at near top valence band resulting a significant quantum conductance, whereas DOS of Pb p-orbital shows minor influence. Various values of quantum conductance observed along different planes are possibly reasoned from a combined effect electrical field over topmost surface and total distance between adjacent facets. Ligands attached to (001) and (011) planes possess similar bond length whereas it is significantly shortened in (111) plane, whereas transport between (011) has an overall low value due to newly formed electric field. On the other hand, (111) plane with a net surface dipole perpendicular to surface layers leading to stronger electron coupling suggests an apparent increase of transport probability. Apart from previously mentioned, the maximum transport energy levels located several eVs (1 2 eVs) from the edge of valence band top.

Structural studies of crystals of organic and organoelement compounds using modern quantum chemical calculations within the framework of the density functional theory

International Nuclear Information System (INIS)

Korlyukov, Alexander A; Antipin, Mikhail Yu

2012-01-01

The review generalizes the results of structural studies of crystals of organic and organometallic compounds by modern quantum chemical calculations within the framework of the density functional theory reported in the last decade. Features of the software for such calculations are discussed. Examples of the use of quantum chemical calculations for the studies of the electronic structure, spectroscopic and other physicochemical properties of molecular crystals are presented. The bibliography includes 223 references.

A new model for the accurate calculation of natural gas viscosity

Directory of Open Access Journals (Sweden)

Xiaohong Yang

2017-03-01

Full Text Available Viscosity of natural gas is a basic and important parameter, of theoretical and practical significance in the domain of natural gas recovery, transmission and processing. In order to obtain the accurate viscosity data efficiently at a low cost, a new model and its corresponding functional relation are derived on the basis of the relationship among viscosity, temperature and density derived from the kinetic theory of gases. After the model parameters were optimized using a lot of experimental data, the diagram showing the variation of viscosity along with temperature and density is prepared, showing that: ① the gas viscosity increases with the increase of density as well as the increase of temperature in the low density region; ② the gas viscosity increases with the decrease of temperature in high density region. With this new model, the viscosity of 9 natural gas samples was calculated precisely. The average relative deviation between these calculated values and 1539 experimental data measured at 250–450 K and 0.10–140.0 MPa is less than 1.9%. Compared with the 793 experimental data with a measurement error less than 0.5%, the maximum relative deviation is less than 0.98%. It is concluded that this new model is more advantageous than the previous 8 models in terms of simplicity, accuracy, fast calculation, and direct applicability to the CO2 bearing gas samples.

Fluorescein isothiocyanate: Molecular characterization by theoretical calculations

Energy Technology Data Exchange (ETDEWEB)

Casanovas, Jordi [Departament de Quimica, Escola Politecnica Superior, Universitat de Lleida, c/Jaume II No 69, Lleida E-25001 (Spain); Jacquemin, Denis [Laboratoire de Chimie Theorique Appliquee, Facultes Universitaires Notre-Dame de la Paix, rue de Bruxelles, 61, B-5000 Namur (Belgium)], E-mail: denis.jacquemin@fundp.ac.be; Perpete, Eric A. [Laboratoire de Chimie Theorique Appliquee, Facultes Universitaires Notre-Dame de la Paix, rue de Bruxelles, 61, B-5000 Namur (Belgium); Aleman, Carlos [Departament d' Enginyeria Quimica, E. T. S. d' Enginyeria Industrial de Barcelona, Universitat Politecnica de Catalunya, Diagonal 647, Barcelona E-08028 (Spain)], E-mail: carlos.aleman@upc.edu

2008-12-10

Quantum mechanical calculations have been used to investigate the conformation, molecular geometry, basicity and spectroscopic properties of fluorescein isothiocyanate in both the gas-phase and aqueous solution. Specifically, calculations have been performed considering the neutral, monoanionic and dianionic forms of this important fluorescent compound. Results reveal that for the neutral form multiple conformational states are possible, all them with significant contributions, and the stability of the different conformers is similar in the gas-phase and aqueous solution. Calculation of the excitation energies revealed that spectroscopic properties are very sensitive to the relaxation effect in solution. A good agreement has been reached obtained between the experimental and theoretical values derived from time-dependent density functional theory methods for the neutral form, whereas for charged species the calculations fail to accurately reproduce the measured trends.

Strain-induced formation of fourfold symmetric SiGe quantum dot molecules.

Science.gov (United States)

Zinovyev, V A; Dvurechenskii, A V; Kuchinskaya, P A; Armbrister, V A

2013-12-27

The strain field distribution at the surface of a multilayer structure with disklike SiGe nanomounds formed by heteroepitaxy is exploited to arrange the symmetric quantum dot molecules typically consisting of four elongated quantum dots ordered along the [010] and [100] directions. The morphological transition from fourfold quantum dot molecules to continuous fortresslike quantum rings with an increasing amount of deposited Ge is revealed. We examine key mechanisms underlying the formation of lateral quantum dot molecules by using scanning tunneling microscopy and numerical calculations of the strain energy distribution on the top of disklike SiGe nanomounds. Experimental data are well described by a simple thermodynamic model based on the accurate evaluation of the strain dependent part of the surface chemical potential. The spatial arrangement of quantum dots inside molecules is attributed to the effect of elastic property anisotropy.

Quantum theory of gauge fields and rigid processes calculation

International Nuclear Information System (INIS)

Andreev, I.V.

1981-01-01

Elementary statement of the basic data on the nature of quark interactions and their role in the high energy processes is presented in the first part of the paper. The second part of the paper deals with gauge theory (GT) of strong interactions (chromodynamics (CD)) and its application in calculation of rigid processes with quark participation. It is based on the method of functional integration (MFI). A comparatively simple representation of the MFI in the quantum theory and formulation of the perturbation theory for gauge fields are given. A derivation of the rules of diagram technique is presented. Renormalization invariance of the theory and the basic for CD phenomenon of asymptotical freedom are discussed. Theory application in calculation of certain effects at high energies is considered. From the CD view point considered is a parton model on the base of which ''rigid'' stage of evolution of quark and gluon jets produced at high energies can be quantitatively described and some quantitative experimental tests of the CD are suggested [ru

Theoretical modeling of large molecular systems. Advances in the local self consistent field method for mixed quantum mechanics/molecular mechanics calculations.

Science.gov (United States)

Monari, Antonio; Rivail, Jean-Louis; Assfeld, Xavier

2013-02-19

Molecular mechanics methods can efficiently compute the macroscopic properties of a large molecular system but cannot represent the electronic changes that occur during a chemical reaction or an electronic transition. Quantum mechanical methods can accurately simulate these processes, but they require considerably greater computational resources. Because electronic changes typically occur in a limited part of the system, such as the solute in a molecular solution or the substrate within the active site of enzymatic reactions, researchers can limit the quantum computation to this part of the system. Researchers take into account the influence of the surroundings by embedding this quantum computation into a calculation of the whole system described at the molecular mechanical level, a strategy known as the mixed quantum mechanics/molecular mechanics (QM/MM) approach. The accuracy of this embedding varies according to the types of interactions included, whether they are purely mechanical or classically electrostatic. This embedding can also introduce the induced polarization of the surroundings. The difficulty in QM/MM calculations comes from the splitting of the system into two parts, which requires severing the chemical bonds that link the quantum mechanical subsystem to the classical subsystem. Typically, researchers replace the quantoclassical atoms, those at the boundary between the subsystems, with a monovalent link atom. For example, researchers might add a hydrogen atom when a C-C bond is cut. This Account describes another approach, the Local Self Consistent Field (LSCF), which was developed in our laboratory. LSCF links the quantum mechanical portion of the molecule to the classical portion using a strictly localized bond orbital extracted from a small model molecule for each bond. In this scenario, the quantoclassical atom has an apparent nuclear charge of +1. To achieve correct bond lengths and force constants, we must take into account the inner shell of

Quantum calculations of the IR spectrum of liquid water using ab initio and model potential and dipole moment surfaces and comparison with experiment

Energy Technology Data Exchange (ETDEWEB)

Liu, Hanchao; Wang, Yimin; Bowman, Joel M. [Cherry L. Emerson Center for Scientific Computation and Department of Chemistry, Emory University, Atlanta, Georgia 30322 (United States)

2015-05-21

The calculation and characterization of the IR spectrum of liquid water have remained a challenge for theory. In this paper, we address this challenge using a combination of ab initio approaches, namely, a quantum treatment of IR spectrum using the ab initio WHBB water potential energy surface and a refined ab initio dipole moment surface. The quantum treatment is based on the embedded local monomer method, in which the three intramolecular modes of each embedded H{sub 2}O monomer are fully coupled and also coupled singly to each of six intermolecular modes. The new dipole moment surface consists of a previous spectroscopically accurate 1-body dipole moment surface and a newly fitted ab initio intrinsic 2-body dipole moment. A detailed analysis of the new dipole moment surface in terms of the coordinate dependence of the effective atomic charges is done along with tests of it for the water dimer and prism hexamer double-harmonic spectra against direct ab initio calculations. The liquid configurations are taken from previous molecular dynamics calculations of Skinner and co-workers, using the TIP4P plus E3B rigid monomer water potential. The IR spectrum of water at 300 K in the range of 0–4000 cm{sup −1} is calculated and compared with experiment, using the ab initio WHBB potential and new ab initio dipole moment, the q-TIP4P/F potential, which has a fixed-charged description of the dipole moment, and the TTM3-F potential and dipole moment surfaces. The newly calculated ab initio spectrum is in very good agreement with experiment throughout the above spectral range, both in band positions and intensities. This contrasts to results with the other potentials and dipole moments, especially the fixed-charge q-TIP4P/F model, which gives unrealistic intensities. The calculated ab initio spectrum is analyzed by examining the contribution of various transitions to each band.

Quantum calculations of the IR spectrum of liquid water using ab initio and model potential and dipole moment surfaces and comparison with experiment

International Nuclear Information System (INIS)

Liu, Hanchao; Wang, Yimin; Bowman, Joel M.

2015-01-01

The calculation and characterization of the IR spectrum of liquid water have remained a challenge for theory. In this paper, we address this challenge using a combination of ab initio approaches, namely, a quantum treatment of IR spectrum using the ab initio WHBB water potential energy surface and a refined ab initio dipole moment surface. The quantum treatment is based on the embedded local monomer method, in which the three intramolecular modes of each embedded H 2 O monomer are fully coupled and also coupled singly to each of six intermolecular modes. The new dipole moment surface consists of a previous spectroscopically accurate 1-body dipole moment surface and a newly fitted ab initio intrinsic 2-body dipole moment. A detailed analysis of the new dipole moment surface in terms of the coordinate dependence of the effective atomic charges is done along with tests of it for the water dimer and prism hexamer double-harmonic spectra against direct ab initio calculations. The liquid configurations are taken from previous molecular dynamics calculations of Skinner and co-workers, using the TIP4P plus E3B rigid monomer water potential. The IR spectrum of water at 300 K in the range of 0–4000 cm −1 is calculated and compared with experiment, using the ab initio WHBB potential and new ab initio dipole moment, the q-TIP4P/F potential, which has a fixed-charged description of the dipole moment, and the TTM3-F potential and dipole moment surfaces. The newly calculated ab initio spectrum is in very good agreement with experiment throughout the above spectral range, both in band positions and intensities. This contrasts to results with the other potentials and dipole moments, especially the fixed-charge q-TIP4P/F model, which gives unrealistic intensities. The calculated ab initio spectrum is analyzed by examining the contribution of various transitions to each band

Cold and ultracold dynamics of the barrierless D{sup +} + H{sub 2} reaction: Quantum reactive calculations for ∼R{sup −4} long range interaction potentials

Energy Technology Data Exchange (ETDEWEB)

Lara, Manuel, E-mail: manuel.lara@uam.es [Departamento de Química Física Aplicada, Facultad de Ciencias, Universidad Autónoma de Madrid, 28049 Madrid (Spain); Jambrina, P. G.; Aoiz, F. J. [Departamento de Química Física, Facultad de Química, Universidad Complutense, 28040 Madrid (Spain); Launay, J.-M. [Institut de Physique de Rennes, UMR CNRS 6251, Université de Rennes I, F-35042 Rennes (France)

2015-11-28

Quantum reactive and elastic cross sections and rate coefficients have been calculated for D{sup +} + H{sub 2} (v = 0, j = 0) collisions in the energy range from 10{sup −8} K (deep ultracold regime), where only one partial wave is open, to 150 K (Langevin regime) where many of them contribute. In systems involving ions, the ∼R{sup −4} behavior extends the interaction up to extremely long distances, requiring a special treatment. To this purpose, we have used a modified version of the hyperspherical quantum reactive scattering method, which allows the propagations up to distances of 10{sup 5} a{sub 0} needed to converge the elastic cross sections. Interpolation procedures are also proposed which may reduce the cost of exact dynamical calculations at such low energies. Calculations have been carried out on the PES by Velilla et al. [J. Chem. Phys. 129, 084307 (2008)] which accurately reproduces the long range interactions. Results on its prequel, the PES by Aguado et al. [J. Chem. Phys. 112, 1240 (2000)], are also shown in order to emphasize the significance of the inclusion of the long range interactions. The calculated reaction rate coefficient changes less than one order of magnitude in a collision energy range of ten orders of magnitude, and it is found in very good agreement with the available experimental data in the region where they exist (10-100 K). State-to-state reaction probabilities are also provided which show that for each partial wave, the distribution of HD final states remains essentially constant below 1 K.

Assignment of absolute stereostructures through quantum mechanics electronic and vibrational circular dichroism calculations.

Science.gov (United States)

Dai, Peng; Jiang, Nan; Tan, Ren-Xiang

2016-01-01

Elucidation of absolute configuration of chiral molecules including structurally complex natural products remains a challenging problem in organic chemistry. A reliable method for assigning the absolute stereostructure is to combine the experimental circular dichroism (CD) techniques such as electronic and vibrational CD (ECD and VCD), with quantum mechanics (QM) ECD and VCD calculations. The traditional QM methods as well as their continuing developments make them more applicable with accuracy. Taking some chiral natural products with diverse conformations as examples, this review describes the basic concepts and new developments of QM approaches for ECD and VCD calculations in solution and solid states.

Recent Progress in Treating Protein-Ligand Interactions with Quantum-Mechanical Methods.

Science.gov (United States)

Yilmazer, Nusret Duygu; Korth, Martin

2016-05-16

We review the first successes and failures of a "new wave" of quantum chemistry-based approaches to the treatment of protein/ligand interactions. These approaches share the use of "enhanced", dispersion (D), and/or hydrogen-bond (H) corrected density functional theory (DFT) or semi-empirical quantum mechanical (SQM) methods, in combination with ensemble weighting techniques of some form to capture entropic effects. Benchmark and model system calculations in comparison to high-level theoretical as well as experimental references have shown that both DFT-D (dispersion-corrected density functional theory) and SQM-DH (dispersion and hydrogen bond-corrected semi-empirical quantum mechanical) perform much more accurately than older DFT and SQM approaches and also standard docking methods. In addition, DFT-D might soon become and SQM-DH already is fast enough to compute a large number of binding modes of comparably large protein/ligand complexes, thus allowing for a more accurate assessment of entropic effects.

Recent Progress in Treating Protein–Ligand Interactions with Quantum-Mechanical Methods

Directory of Open Access Journals (Sweden)

Nusret Duygu Yilmazer

2016-05-01

Full Text Available We review the first successes and failures of a “new wave” of quantum chemistry-based approaches to the treatment of protein/ligand interactions. These approaches share the use of “enhanced”, dispersion (D, and/or hydrogen-bond (H corrected density functional theory (DFT or semi-empirical quantum mechanical (SQM methods, in combination with ensemble weighting techniques of some form to capture entropic effects. Benchmark and model system calculations in comparison to high-level theoretical as well as experimental references have shown that both DFT-D (dispersion-corrected density functional theory and SQM-DH (dispersion and hydrogen bond-corrected semi-empirical quantum mechanical perform much more accurately than older DFT and SQM approaches and also standard docking methods. In addition, DFT-D might soon become and SQM-DH already is fast enough to compute a large number of binding modes of comparably large protein/ligand complexes, thus allowing for a more accurate assessment of entropic effects.

An accurate algorithm to calculate the Hurst exponent of self-similar processes

International Nuclear Information System (INIS)

Fernández-Martínez, M.; Sánchez-Granero, M.A.; Trinidad Segovia, J.E.; Román-Sánchez, I.M.

2014-01-01

In this paper, we introduce a new approach which generalizes the GM2 algorithm (introduced in Sánchez-Granero et al. (2008) [52]) as well as fractal dimension algorithms (FD1, FD2 and FD3) (first appeared in Sánchez-Granero et al. (2012) [51]), providing an accurate algorithm to calculate the Hurst exponent of self-similar processes. We prove that this algorithm performs properly in the case of short time series when fractional Brownian motions and Lévy stable motions are considered. We conclude the paper with a dynamic study of the Hurst exponent evolution in the S and P500 index stocks. - Highlights: • We provide a new approach to properly calculate the Hurst exponent. • This generalizes FD algorithms and GM2, introduced previously by the authors. • This method (FD4) results especially appropriate for short time series. • FD4 may be used in both unifractal and multifractal contexts. • As an empirical application, we show that S and P500 stocks improved their efficiency

An accurate algorithm to calculate the Hurst exponent of self-similar processes

Energy Technology Data Exchange (ETDEWEB)

Fernández-Martínez, M., E-mail: fmm124@ual.es [Department of Mathematics, Faculty of Science, Universidad de Almería, 04120 Almería (Spain); Sánchez-Granero, M.A., E-mail: misanche@ual.es [Department of Mathematics, Faculty of Science, Universidad de Almería, 04120 Almería (Spain); Trinidad Segovia, J.E., E-mail: jetrini@ual.es [Department of Accounting and Finance, Faculty of Economics and Business, Universidad de Almería, 04120 Almería (Spain); Román-Sánchez, I.M., E-mail: iroman@ual.es [Department of Accounting and Finance, Faculty of Economics and Business, Universidad de Almería, 04120 Almería (Spain)

2014-06-27

In this paper, we introduce a new approach which generalizes the GM2 algorithm (introduced in Sánchez-Granero et al. (2008) [52]) as well as fractal dimension algorithms (FD1, FD2 and FD3) (first appeared in Sánchez-Granero et al. (2012) [51]), providing an accurate algorithm to calculate the Hurst exponent of self-similar processes. We prove that this algorithm performs properly in the case of short time series when fractional Brownian motions and Lévy stable motions are considered. We conclude the paper with a dynamic study of the Hurst exponent evolution in the S and P500 index stocks. - Highlights: • We provide a new approach to properly calculate the Hurst exponent. • This generalizes FD algorithms and GM2, introduced previously by the authors. • This method (FD4) results especially appropriate for short time series. • FD4 may be used in both unifractal and multifractal contexts. • As an empirical application, we show that S and P500 stocks improved their efficiency.

Calculation of accurate small angle X-ray scattering curves from coarse-grained protein models

DEFF Research Database (Denmark)

Stovgaard, Kasper; Andreetta, Christian; Ferkinghoff-Borg, Jesper

2010-01-01

, which is paramount for structure determination based on statistical inference. Results: We present a method for the efficient calculation of accurate SAXS curves based on the Debye formula and a set of scattering form factors for dummy atom representations of amino acids. Such a method avoids......DBN. This resulted in a significant improvement in the decoy recognition performance. In conclusion, the presented method shows great promise for use in statistical inference of protein structures from SAXS data....

Accurate Determination of the Quasiparticle and Scaling Properties Surrounding the Quantum Critical Point of Disordered Three-Dimensional Dirac Semimetals.

Science.gov (United States)

Fu, Bo; Zhu, Wei; Shi, Qinwei; Li, Qunxiang; Yang, Jinlong; Zhang, Zhenyu

2017-04-07

Exploiting the enabling power of the Lanczos method in momentum space, we determine accurately the quasiparticle and scaling properties of disordered three-dimensional Dirac semimetals surrounding the quantum critical point separating the semimetal and diffusive metal regimes. We unveil that the imaginary part of the quasiparticle self-energy obeys a common power law before, at, and after the quantum phase transition, but the power law is nonuniversal, whose exponent is dependent on the disorder strength. More intriguingly, whereas a common power law is also found for the real part of the self-energy before and after the phase transition, a distinctly different behavior is identified at the critical point, characterized by the existence of a nonanalytic logarithmic singularity. This nonanalytical correction serves as the very basis for the unusual power-law behaviors of the quasiparticles and many other physical properties surrounding the quantum critical point. Our approach also allows the ready and reliable determination of the scaling properties of the correlation length and dynamical exponents. We further show that the central findings are valid for both uncorrelated and correlated disorder distributions and should be directly comparable with future experimental observations.

An approximate framework for quantum transport calculation with model order reduction

Energy Technology Data Exchange (ETDEWEB)

Chen, Quan, E-mail: quanchen@eee.hku.hk [Department of Electrical and Electronic Engineering, The University of Hong Kong (Hong Kong); Li, Jun [Department of Chemistry, The University of Hong Kong (Hong Kong); Yam, Chiyung [Beijing Computational Science Research Center (China); Zhang, Yu [Department of Chemistry, The University of Hong Kong (Hong Kong); Wong, Ngai [Department of Electrical and Electronic Engineering, The University of Hong Kong (Hong Kong); Chen, Guanhua [Department of Chemistry, The University of Hong Kong (Hong Kong)

2015-04-01

A new approximate computational framework is proposed for computing the non-equilibrium charge density in the context of the non-equilibrium Green's function (NEGF) method for quantum mechanical transport problems. The framework consists of a new formulation, called the X-formulation, for single-energy density calculation based on the solution of sparse linear systems, and a projection-based nonlinear model order reduction (MOR) approach to address the large number of energy points required for large applied biases. The advantages of the new methods are confirmed by numerical experiments.

Green's function approach to calculate spin injection in quantum dot

International Nuclear Information System (INIS)

Tan, S.G.; Jalil, M.B.A.; Liew, Thomas; Teo, K.L.

2006-01-01

We present a theoretical model to study spin injection (η) through a quantum dot system sandwiched by two ferromagnetic contacts. The effect of contact magnetization on η was studied using Green's function descriptions of the density of states. Green's function models have the advantages that coherent effects of temperature, electron occupation in the QD, and lead perturbation on the state wave function and hence the current can be formally included in the calculations. In addition, self-consistent treatment of current with applied electrochemical potential or lead conductivity, a necessary step which has not been considered in previous works, has also been implemented in our model

Conjugate-gradient optimization method for orbital-free density functional calculations.

Science.gov (United States)

Jiang, Hong; Yang, Weitao

2004-08-01

Orbital-free density functional theory as an extension of traditional Thomas-Fermi theory has attracted a lot of interest in the past decade because of developments in both more accurate kinetic energy functionals and highly efficient numerical methodology. In this paper, we developed a conjugate-gradient method for the numerical solution of spin-dependent extended Thomas-Fermi equation by incorporating techniques previously used in Kohn-Sham calculations. The key ingredient of the method is an approximate line-search scheme and a collective treatment of two spin densities in the case of spin-dependent extended Thomas-Fermi problem. Test calculations for a quartic two-dimensional quantum dot system and a three-dimensional sodium cluster Na216 with a local pseudopotential demonstrate that the method is accurate and efficient. (c) 2004 American Institute of Physics.

Accurate Holdup Calculations with Predictive Modeling & Data Integration

Energy Technology Data Exchange (ETDEWEB)

Azmy, Yousry [North Carolina State Univ., Raleigh, NC (United States). Dept. of Nuclear Engineering; Cacuci, Dan [Univ. of South Carolina, Columbia, SC (United States). Dept. of Mechanical Engineering

2017-04-03

In facilities that process special nuclear material (SNM) it is important to account accurately for the fissile material that enters and leaves the plant. Although there are many stages and processes through which materials must be traced and measured, the focus of this project is material that is “held-up” in equipment, pipes, and ducts during normal operation and that can accumulate over time into significant quantities. Accurately estimating the holdup is essential for proper SNM accounting (vis-à-vis nuclear non-proliferation), criticality and radiation safety, waste management, and efficient plant operation. Usually it is not possible to directly measure the holdup quantity and location, so these must be inferred from measured radiation fields, primarily gamma and less frequently neutrons. Current methods to quantify holdup, i.e. Generalized Geometry Holdup (GGH), primarily rely on simple source configurations and crude radiation transport models aided by ad hoc correction factors. This project seeks an alternate method of performing measurement-based holdup calculations using a predictive model that employs state-of-the-art radiation transport codes capable of accurately simulating such situations. Inverse and data assimilation methods use the forward transport model to search for a source configuration that best matches the measured data and simultaneously provide an estimate of the level of confidence in the correctness of such configuration. In this work the holdup problem is re-interpreted as an inverse problem that is under-determined, hence may permit multiple solutions. A probabilistic approach is applied to solving the resulting inverse problem. This approach rates possible solutions according to their plausibility given the measurements and initial information. This is accomplished through the use of Bayes’ Theorem that resolves the issue of multiple solutions by giving an estimate of the probability of observing each possible solution. To use

Accurate convolution/superposition for multi-resolution dose calculation using cumulative tabulated kernels

International Nuclear Information System (INIS)

Lu Weiguo; Olivera, Gustavo H; Chen Mingli; Reckwerdt, Paul J; Mackie, Thomas R

2005-01-01

is demonstrated to be the most accurate one for multi-resolution dose calculations

A comparative study of different methods for calculating electronic transition rates

Science.gov (United States)

Kananenka, Alexei A.; Sun, Xiang; Schubert, Alexander; Dunietz, Barry D.; Geva, Eitan

2018-03-01

We present a comprehensive comparison of the following mixed quantum-classical methods for calculating electronic transition rates: (1) nonequilibrium Fermi's golden rule, (2) mixed quantum-classical Liouville method, (3) mean-field (Ehrenfest) mixed quantum-classical method, and (4) fewest switches surface-hopping method (in diabatic and adiabatic representations). The comparison is performed on the Garg-Onuchic-Ambegaokar benchmark charge-transfer model, over a broad range of temperatures and electronic coupling strengths, with different nonequilibrium initial states, in the normal and inverted regimes. Under weak to moderate electronic coupling, the nonequilibrium Fermi's golden rule rates are found to be in good agreement with the rates obtained via the mixed quantum-classical Liouville method that coincides with the fully quantum-mechanically exact results for the model system under study. Our results suggest that the nonequilibrium Fermi's golden rule can serve as an inexpensive yet accurate alternative to Ehrenfest and the fewest switches surface-hopping methods.

Reducing Projection Calculation in Quantum Teleportation by Virtue of the IWOP Technique and Schmidt Decomposition of |η〉 State

Institute of Scientific and Technical Information of China (English)

FAN Hong-Yi; FAN Yue

2002-01-01

By virtue of the technique of integration within an ordered product of operators and the Schmidt decomposition of the entangled state |η〉, we reduce the general projection calculation in the theory of quantum teleportation to a as simple as possible form and present a general formalism for teleportating quantum states of continuous variable.

Linear and Non-Linear Dielectric Response of Periodic Systems from Quantum Monte Carlo

Science.gov (United States)

Umari, Paolo

2006-03-01

We present a novel approach that allows to calculate the dielectric response of periodic systems in the quantum Monte Carlo formalism. We employ a many-body generalization for the electric enthalpy functional, where the coupling with the field is expressed via the Berry-phase formulation for the macroscopic polarization. A self-consistent local Hamiltonian then determines the ground-state wavefunction, allowing for accurate diffusion quantum Monte Carlo calculations where the polarization's fixed point is estimated from the average on an iterative sequence. The polarization is sampled through forward-walking. This approach has been validated for the case of the polarizability of an isolated hydrogen atom, and then applied to a periodic system. We then calculate the linear susceptibility and second-order hyper-susceptibility of molecular-hydrogen chains whith different bond-length alternations, and assess the quality of nodal surfaces derived from density-functional theory or from Hartree-Fock. The results found are in excellent agreement with the best estimates obtained from the extrapolation of quantum-chemistry calculations.P. Umari, A.J. Williamson, G. Galli, and N. MarzariPhys. Rev. Lett. 95, 207602 (2005).

Quantum dynamics in open quantum-classical systems.

Science.gov (United States)

Kapral, Raymond

2015-02-25

Often quantum systems are not isolated and interactions with their environments must be taken into account. In such open quantum systems these environmental interactions can lead to decoherence and dissipation, which have a marked influence on the properties of the quantum system. In many instances the environment is well-approximated by classical mechanics, so that one is led to consider the dynamics of open quantum-classical systems. Since a full quantum dynamical description of large many-body systems is not currently feasible, mixed quantum-classical methods can provide accurate and computationally tractable ways to follow the dynamics of both the system and its environment. This review focuses on quantum-classical Liouville dynamics, one of several quantum-classical descriptions, and discusses the problems that arise when one attempts to combine quantum and classical mechanics, coherence and decoherence in quantum-classical systems, nonadiabatic dynamics, surface-hopping and mean-field theories and their relation to quantum-classical Liouville dynamics, as well as methods for simulating the dynamics.

QmeQ 1.0: An open-source Python package for calculations of transport through quantum dot devices

Science.gov (United States)

Kiršanskas, Gediminas; Pedersen, Jonas Nyvold; Karlström, Olov; Leijnse, Martin; Wacker, Andreas

2017-12-01

QmeQ is an open-source Python package for numerical modeling of transport through quantum dot devices with strong electron-electron interactions using various approximate master equation approaches. The package provides a framework for calculating stationary particle or energy currents driven by differences in chemical potentials or temperatures between the leads which are tunnel coupled to the quantum dots. The electronic structures of the quantum dots are described by their single-particle states and the Coulomb matrix elements between the states. When transport is treated perturbatively to lowest order in the tunneling couplings, the possible approaches are Pauli (classical), first-order Redfield, and first-order von Neumann master equations, and a particular form of the Lindblad equation. When all processes involving two-particle excitations in the leads are of interest, the second-order von Neumann approach can be applied. All these approaches are implemented in QmeQ. We here give an overview of the basic structure of the package, give examples of transport calculations, and outline the range of applicability of the different approximate approaches.

Protein structure validation and refinement using amide proton chemical shifts derived from quantum mechanics

DEFF Research Database (Denmark)

Christensen, Anders Steen; Linnet, Troels Emtekær; Borg, Mikael

2013-01-01

We present the ProCS method for the rapid and accurate prediction of protein backbone amide proton chemical shifts - sensitive probes of the geometry of key hydrogen bonds that determine protein structure. ProCS is parameterized against quantum mechanical (QM) calculations and reproduces high level...

Comparison of different boost transformations for the calculation of form factors in relativistic quantum mechanics

International Nuclear Information System (INIS)

Theussl, L.; Noguera, S.; Amghar, A.; Desplanques, B.

2003-01-01

The effect of different boost expressions, pertinent to the instant, front and point forms of relativistic quantum mechanics, is considered for the calculation of the ground-state form factor of a two-body system in simple scalar models. Results with a Galilean boost as well as an explicitly covariant calculation based on the Bethe-Salpeter approach are given for comparison. It is found that the present so-called point-form calculations of form factors strongly deviate from all the other ones. This suggests that the formalism which underlies them requires further elaboration. A proposition in this sense is made. (author)

Quantum thermodynamics of general quantum processes.

Science.gov (United States)

Binder, Felix; Vinjanampathy, Sai; Modi, Kavan; Goold, John

2015-03-01

Accurately describing work extraction from a quantum system is a central objective for the extension of thermodynamics to individual quantum systems. The concepts of work and heat are surprisingly subtle when generalizations are made to arbitrary quantum states. We formulate an operational thermodynamics suitable for application to an open quantum system undergoing quantum evolution under a general quantum process by which we mean a completely positive and trace-preserving map. We derive an operational first law of thermodynamics for such processes and show consistency with the second law. We show that heat, from the first law, is positive when the input state of the map majorizes the output state. Moreover, the change in entropy is also positive for the same majorization condition. This makes a strong connection between the two operational laws of thermodynamics.

Electron states in semiconductor quantum dots

International Nuclear Information System (INIS)

Dhayal, Suman S.; Ramaniah, Lavanya M.; Ruda, Harry E.; Nair, Selvakumar V.

2014-01-01

In this work, the electronic structures of quantum dots (QDs) of nine direct band gap semiconductor materials belonging to the group II-VI and III-V families are investigated, within the empirical tight-binding framework, in the effective bond orbital model. This methodology is shown to accurately describe these systems, yielding, at the same time, qualitative insights into their electronic properties. Various features of the bulk band structure such as band-gaps, band curvature, and band widths around symmetry points affect the quantum confinement of electrons and holes. These effects are identified and quantified. A comparison with experimental data yields good agreement with the calculations. These theoretical results would help quantify the optical response of QDs of these materials and provide useful input for applications

Discovery of a general method of solving the Schrödinger and dirac equations that opens a way to accurately predictive quantum chemistry.

Science.gov (United States)

Nakatsuji, Hiroshi

2012-09-18

Just as Newtonian law governs classical physics, the Schrödinger equation (SE) and the relativistic Dirac equation (DE) rule the world of chemistry. So, if we can solve these equations accurately, we can use computation to predict chemistry precisely. However, for approximately 80 years after the discovery of these equations, chemists believed that they could not solve SE and DE for atoms and molecules that included many electrons. This Account reviews ideas developed over the past decade to further the goal of predictive quantum chemistry. Between 2000 and 2005, I discovered a general method of solving the SE and DE accurately. As a first inspiration, I formulated the structure of the exact wave function of the SE in a compact mathematical form. The explicit inclusion of the exact wave function's structure within the variational space allows for the calculation of the exact wave function as a solution of the variational method. Although this process sounds almost impossible, it is indeed possible, and I have published several formulations and applied them to solve the full configuration interaction (CI) with a very small number of variables. However, when I examined analytical solutions for atoms and molecules, the Hamiltonian integrals in their secular equations diverged. This singularity problem occurred in all atoms and molecules because it originates from the singularity of the Coulomb potential in their Hamiltonians. To overcome this problem, I first introduced the inverse SE and then the scaled SE. The latter simpler idea led to immediate and surprisingly accurate solution for the SEs of the hydrogen atom, helium atom, and hydrogen molecule. The free complement (FC) method, also called the free iterative CI (free ICI) method, was efficient for solving the SEs. In the FC method, the basis functions that span the exact wave function are produced by the Hamiltonian of the system and the zeroth-order wave function. These basis functions are called complement

Accurate van der Waals force field for gas adsorption in porous materials.

Science.gov (United States)

Sun, Lei; Yang, Li; Zhang, Ya-Dong; Shi, Qi; Lu, Rui-Feng; Deng, Wei-Qiao

2017-09-05

An accurate van der Waals force field (VDW FF) was derived from highly precise quantum mechanical (QM) calculations. Small molecular clusters were used to explore van der Waals interactions between gas molecules and porous materials. The parameters of the accurate van der Waals force field were determined by QM calculations. To validate the force field, the prediction results from the VDW FF were compared with standard FFs, such as UFF, Dreiding, Pcff, and Compass. The results from the VDW FF were in excellent agreement with the experimental measurements. This force field can be applied to the prediction of the gas density (H 2 , CO 2 , C 2 H 4 , CH 4 , N 2 , O 2 ) and adsorption performance inside porous materials, such as covalent organic frameworks (COFs), zeolites and metal organic frameworks (MOFs), consisting of H, B, N, C, O, S, Si, Al, Zn, Mg, Ni, and Co. This work provides a solid basis for studying gas adsorption in porous materials. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.

Quantum-Mechanical Calculation of Ionization-Potential Lowering in Dense Plasmas

Directory of Open Access Journals (Sweden)

Sang-Kil Son (손상길

2014-07-01

Full Text Available The charged environment within a dense plasma leads to the phenomenon of ionization-potential depression (IPD for ions embedded in the plasma. Accurate predictions of the IPD effect are of crucial importance for modeling atomic processes occurring within dense plasmas. Several theoretical models have been developed to describe the IPD effect, with frequently discrepant predictions. Only recently, first experiments on IPD in Al plasma have been performed with an x-ray free-electron laser, where their results were found to be in disagreement with the widely used IPD model by Stewart and Pyatt. Another experiment on Al, at the Orion laser, showed disagreement with the model by Ecker and Kröll. This controversy shows a strong need for a rigorous and consistent theoretical approach to calculate the IPD effect. Here, we propose such an approach: a two-step Hartree-Fock-Slater model. With this parameter-free model, we can accurately and efficiently describe the experimental Al data and validate the accuracy of standard IPD models. Our model can be a useful tool for calculating atomic properties within dense plasmas with wide-ranging applications to studies on warm dense matter, shock experiments, planetary science, inertial confinement fusion, and nonequilibrium plasmas created with x-ray free-electron lasers.

QMCPACK: an open source ab initio quantum Monte Carlo package for the electronic structure of atoms, molecules and solids

Science.gov (United States)

Kim, Jeongnim; Baczewski, Andrew D.; Beaudet, Todd D.; Benali, Anouar; Chandler Bennett, M.; Berrill, Mark A.; Blunt, Nick S.; Josué Landinez Borda, Edgar; Casula, Michele; Ceperley, David M.; Chiesa, Simone; Clark, Bryan K.; Clay, Raymond C., III; Delaney, Kris T.; Dewing, Mark; Esler, Kenneth P.; Hao, Hongxia; Heinonen, Olle; Kent, Paul R. C.; Krogel, Jaron T.; Kylänpää, Ilkka; Li, Ying Wai; Lopez, M. Graham; Luo, Ye; Malone, Fionn D.; Martin, Richard M.; Mathuriya, Amrita; McMinis, Jeremy; Melton, Cody A.; Mitas, Lubos; Morales, Miguel A.; Neuscamman, Eric; Parker, William D.; Pineda Flores, Sergio D.; Romero, Nichols A.; Rubenstein, Brenda M.; Shea, Jacqueline A. R.; Shin, Hyeondeok; Shulenburger, Luke; Tillack, Andreas F.; Townsend, Joshua P.; Tubman, Norm M.; Van Der Goetz, Brett; Vincent, Jordan E.; ChangMo Yang, D.; Yang, Yubo; Zhang, Shuai; Zhao, Luning

2018-05-01

QMCPACK is an open source quantum Monte Carlo package for ab initio electronic structure calculations. It supports calculations of metallic and insulating solids, molecules, atoms, and some model Hamiltonians. Implemented real space quantum Monte Carlo algorithms include variational, diffusion, and reptation Monte Carlo. QMCPACK uses Slater–Jastrow type trial wavefunctions in conjunction with a sophisticated optimizer capable of optimizing tens of thousands of parameters. The orbital space auxiliary-field quantum Monte Carlo method is also implemented, enabling cross validation between different highly accurate methods. The code is specifically optimized for calculations with large numbers of electrons on the latest high performance computing architectures, including multicore central processing unit and graphical processing unit systems. We detail the program’s capabilities, outline its structure, and give examples of its use in current research calculations. The package is available at http://qmcpack.org.

Relaxation of a kinetic hole due to carrier-carrier scattering in multisubband single-quantum-well semiconductors

DEFF Research Database (Denmark)

Dery, H.; Tromborg, Bjarne; Eisenstein, G.

2003-01-01

We describe a theoretical model for carrier-carrier scattering in an inverted semiconductor quantum well structure using a multisubband diagram. The model includes all possible nonvanishing interaction terms within the static screening approximation, and it enables one to calculate accurately...

Accurate calculation of field and carrier distributions in doped semiconductors

Directory of Open Access Journals (Sweden)

Wenji Yang

2012-06-01

Full Text Available We use the numerical squeezing algorithm(NSA combined with the shooting method to accurately calculate the built-in fields and carrier distributions in doped silicon films (SFs in the micron and sub-micron thickness range and results are presented in graphical form for variety of doping profiles under different boundary conditions. As a complementary approach, we also present the methods and the results of the inverse problem (IVP - finding out the doping profile in the SFs for given field distribution. The solution of the IVP provides us the approach to arbitrarily design field distribution in SFs - which is very important for low dimensional (LD systems and device designing. Further more, the solution of the IVP is both direct and much easy for all the one-, two-, and three-dimensional semiconductor systems. With current efforts focused on the LD physics, knowing of the field and carrier distribution details in the LD systems will facilitate further researches on other aspects and hence the current work provides a platform for those researches.

Calculation of the dependence on the Moon and Mars γ-quantum flux on the relief and distance to the surface

International Nuclear Information System (INIS)

Surkov, Yu.A.; Noskaleva, L.P.; Manvelyan, O.S.

1978-01-01

The dependence of the gamma quantum flux on height over a planet, area over which the gamma radiation is ''collected'', and surface relief is calculated. The effect of the planet atmosphere on detected gamma radiation is considered. If the specific power of gamma-quantum sources is known, the results obtained allow to determine for any height over a planet the gamma-quantum flux due to the planet rock and its atmosphere radiations, as well as the detector spatial resolution

Silicon Oxysulfide, OSiS: Rotational Spectrum, Quantum-Chemical Calculations, and Equilibrium Structure.

Science.gov (United States)

Thorwirth, Sven; Mück, Leonie Anna; Gauss, Jürgen; Tamassia, Filippo; Lattanzi, Valerio; McCarthy, Michael C

2011-06-02

Silicon oxysulfide, OSiS, and seven of its minor isotopic species have been characterized for the first time in the gas phase at high spectral resolution by means of Fourier transform microwave spectroscopy. The equilibrium structure of OSiS has been determined from the experimental data using calculated vibration-rotation interaction constants. The structural parameters (rO-Si = 1.5064 Å and rSi-S = 1.9133 Å) are in very good agreement with values from high-level quantum chemical calculations using coupled-cluster techniques together with sophisticated additivity and extrapolation schemes. The bond distances in OSiS are very short in comparison with those in SiO and SiS. This unexpected finding is explained by the partial charges calculated for OSiS via a natural population analysis. The results suggest that electrostatic effects rather than multiple bonding are the key factors in determining bonding in this triatomic molecule. The data presented provide the spectroscopic information needed for radio astronomical searches for OSiS.

Towards quantum chemistry on a quantum computer.

Science.gov (United States)

Lanyon, B P; Whitfield, J D; Gillett, G G; Goggin, M E; Almeida, M P; Kassal, I; Biamonte, J D; Mohseni, M; Powell, B J; Barbieri, M; Aspuru-Guzik, A; White, A G

2010-02-01

Exact first-principles calculations of molecular properties are currently intractable because their computational cost grows exponentially with both the number of atoms and basis set size. A solution is to move to a radically different model of computing by building a quantum computer, which is a device that uses quantum systems themselves to store and process data. Here we report the application of the latest photonic quantum computer technology to calculate properties of the smallest molecular system: the hydrogen molecule in a minimal basis. We calculate the complete energy spectrum to 20 bits of precision and discuss how the technique can be expanded to solve large-scale chemical problems that lie beyond the reach of modern supercomputers. These results represent an early practical step toward a powerful tool with a broad range of quantum-chemical applications.

The electronic band parameters calculated by the Kronig-Penney method for Cd1-xZnxS quantum dot superlattices

International Nuclear Information System (INIS)

Sakly, A.; Safta, N.; Mejri, H.; Lamine, A. Ben

2009-01-01

This work reports on a theoretical study of superlattices based on Cd 1-x Zn x S quantum dots embedded in an insulating material. We show, in particular, how this system can be assumed to a series of flattened cylindrical quantum dots with a finite barrier height at the boundary. In this paper, are also reviewed the approximations needed to calculate the band edges of the Cd 1-x Zn x S superlattices with use of the Kronig-Penney model. The electronic states and the electron effective masses of both Γ 1 - and Γ 2 -minibands have been computed as a function of zinc composition for different inter-quantum dot separations. As is found, the CdS system is appropriate to give rise a superlattice behavior for conduction electrons in a relatively large range of inter-sheet separations. An attempt to explain the electron band parameters calculated will be presented.

Quantum robots and quantum computers

Energy Technology Data Exchange (ETDEWEB)

Benioff, P.

1998-07-01

Validation of a presumably universal theory, such as quantum mechanics, requires a quantum mechanical description of systems that carry out theoretical calculations and systems that carry out experiments. The description of quantum computers is under active development. No description of systems to carry out experiments has been given. A small step in this direction is taken here by giving a description of quantum robots as mobile systems with on board quantum computers that interact with different environments. Some properties of these systems are discussed. A specific model based on the literature descriptions of quantum Turing machines is presented.

Recent Advances in Development and Applications of the Mixed Quantum/Classical Theory for Inelastic Scattering.

Science.gov (United States)

Babikov, Dmitri; Semenov, Alexander

2016-01-28

A mixed quantum/classical approach to inelastic scattering (MQCT) is developed in which the relative motion of two collision partners is treated classically, and the rotational and vibrational motion of each molecule is treated quantum mechanically. The cases of molecule + atom and molecule + molecule are considered including diatomics, symmetric-top rotors, and asymmetric-top rotor molecules. Phase information is taken into consideration, permitting calculations of elastic and inelastic, total and differential cross sections for excitation and quenching. The method is numerically efficient and intrinsically parallel. The scaling law of MQCT is favorable, which enables calculations at high collision energies and for complicated molecules. Benchmark studies are carried out for several quite different molecular systems (N2 + Na, H2 + He, CO + He, CH3 + He, H2O + He, HCOOCH3 + He, and H2 + N2) in a broad range of collision energies, which demonstrates that MQCT is a viable approach to inelastic scattering. At higher collision energies it can confidently replace the computationally expensive full-quantum calculations. At low collision energies and for low-mass systems results of MQCT are less accurate but are still reasonable. A proposal is made for blending MQCT calculations at higher energies with full-quantum calculations at low energies.

Quantum critical dynamics for a prototype class of insulating antiferromagnets

Science.gov (United States)

Wu, Jianda; Yang, Wang; Wu, Congjun; Si, Qimiao

2018-06-01

Quantum criticality is a fundamental organizing principle for studying strongly correlated systems. Nevertheless, understanding quantum critical dynamics at nonzero temperatures is a major challenge of condensed-matter physics due to the intricate interplay between quantum and thermal fluctuations. The recent experiments with the quantum spin dimer material TlCuCl3 provide an unprecedented opportunity to test the theories of quantum criticality. We investigate the nonzero-temperature quantum critical spin dynamics by employing an effective O (N ) field theory. The on-shell mass and the damping rate of quantum critical spin excitations as functions of temperature are calculated based on the renormalized coupling strength and are in excellent agreement with experiment observations. Their T lnT dependence is predicted to be dominant at very low temperatures, which will be tested in future experiments. Our work provides confidence that quantum criticality as a theoretical framework, which is being considered in so many different contexts of condensed-matter physics and beyond, is indeed grounded in materials and experiments accurately. It is also expected to motivate further experimental investigations on the applicability of the field theory to related quantum critical systems.

Magnetism of iron and nickel from rotationally invariant Hirsch-Fye quantum Monte Carlo calculations

Science.gov (United States)

Belozerov, A. S.; Leonov, I.; Anisimov, V. I.

2013-03-01

We present a rotationally invariant Hirsch-Fye quantum Monte Carlo algorithm in which the spin rotational invariance of Hund's exchange is approximated by averaging over all possible directions of the spin quantization axis. We employ this technique to perform benchmark calculations for the two- and three-band Hubbard models on the infinite-dimensional Bethe lattice. Our results agree quantitatively well with those obtained using the continuous-time quantum Monte Carlo method with rotationally invariant Coulomb interaction. The proposed approach is employed to compute the electronic and magnetic properties of paramagnetic α iron and nickel. The obtained Curie temperatures agree well with experiment. Our results indicate that the magnetic transition temperature is significantly overestimated by using the density-density type of Coulomb interaction.

Size-dependent optical properties of colloidal PbS quantum dots.

Science.gov (United States)

Moreels, Iwan; Lambert, Karel; Smeets, Dries; De Muynck, David; Nollet, Tom; Martins, José C; Vanhaecke, Frank; Vantomme, André; Delerue, Christophe; Allan, Guy; Hens, Zeger

2009-10-27

We quantitatively investigate the size-dependent optical properties of colloidal PbS nanocrystals or quantum dots (Qdots), by combining the Qdot absorbance spectra with detailed elemental analysis of the Qdot suspensions. At high energies, the molar extinction coefficient epsilon increases with the Qdot volume d(3) and agrees with theoretical calculations using the Maxwell-Garnett effective medium theory and bulk values for the Qdot dielectric function. This demonstrates that quantum confinement has no influence on epsilon in this spectral range, and it provides an accurate method to calculate the Qdot concentration. Around the band gap, epsilon only increases with d(1.3), and values are comparable to the epsilon of PbSe Qdots. The data are related to the oscillator strength f(if) of the band gap transition and results agree well with theoretical tight-binding calculations, predicting a linear dependence of f(if) on d. For both PbS and PbSe Qdots, the exciton lifetime tau is calculated from f(if). We find values ranging between 1 and 3 mus, in agreement with experimental literature data from time-resolved luminescence spectroscopy. Our results provide a thorough general framework to calculate and understand the optical properties of suspended colloidal quantum dots. Most importantly, it highlights the significance of the local field factor in these systems.

Semiempirical Quantum Chemical Calculations Accelerated on a Hybrid Multicore CPU-GPU Computing Platform.

Science.gov (United States)

Wu, Xin; Koslowski, Axel; Thiel, Walter

2012-07-10

In this work, we demonstrate that semiempirical quantum chemical calculations can be accelerated significantly by leveraging the graphics processing unit (GPU) as a coprocessor on a hybrid multicore CPU-GPU computing platform. Semiempirical calculations using the MNDO, AM1, PM3, OM1, OM2, and OM3 model Hamiltonians were systematically profiled for three types of test systems (fullerenes, water clusters, and solvated crambin) to identify the most time-consuming sections of the code. The corresponding routines were ported to the GPU and optimized employing both existing library functions and a GPU kernel that carries out a sequence of noniterative Jacobi transformations during pseudodiagonalization. The overall computation times for single-point energy calculations and geometry optimizations of large molecules were reduced by one order of magnitude for all methods, as compared to runs on a single CPU core.

Accurate deuterium spectroscopy for fundamental studies

Science.gov (United States)

Wcisło, P.; Thibault, F.; Zaborowski, M.; Wójtewicz, S.; Cygan, A.; Kowzan, G.; Masłowski, P.; Komasa, J.; Puchalski, M.; Pachucki, K.; Ciuryło, R.; Lisak, D.

2018-07-01

We present an accurate measurement of the weak quadrupole S(2) 2-0 line in self-perturbed D2 and theoretical ab initio calculations of both collisional line-shape effects and energy of this rovibrational transition. The spectra were collected at the 247-984 Torr pressure range with a frequency-stabilized cavity ring-down spectrometer linked to an optical frequency comb (OFC) referenced to a primary time standard. Our line-shape modeling employed quantum calculations of molecular scattering (the pressure broadening and shift and their speed dependencies were calculated, while the complex frequency of optical velocity-changing collisions was fitted to experimental spectra). The velocity-changing collisions are handled with the hard-sphere collisional kernel. The experimental and theoretical pressure broadening and shift are consistent within 5% and 27%, respectively (the discrepancy for shift is 8% when referred not to the speed averaged value, which is close to zero, but to the range of variability of the speed-dependent shift). We use our high pressure measurement to determine the energy, ν0, of the S(2) 2-0 transition. The ab initio line-shape calculations allowed us to mitigate the expected collisional systematics reaching the 410 kHz accuracy of ν0. We report theoretical determination of ν0 taking into account relativistic and QED corrections up to α5. Our estimation of the accuracy of the theoretical ν0 is 1.3 MHz. We observe 3.4σ discrepancy between experimental and theoretical ν0.

Precise Determination of Quantum Critical Points by the Violation of the Entropic Area Law

OpenAIRE

Xavier, J. C.; Alcaraz, F. C.

2011-01-01

Finite-size scaling analysis turns out to be a powerful tool to calculate the phase diagram as well as the critical properties of two dimensional classical statistical mechanics models and quantum Hamiltonians in one dimension. The most used method to locate quantum critical points is the so called crossing method, where the estimates are obtained by comparing the mass gaps of two distinct lattice sizes. The success of this method is due to its simplicity and the ability to provide accurate r...

Rotational spectra of rare isotopic species of fluoroiodomethane: determination of the equilibrium structure from rotational spectroscopy and quantum-chemical calculations.

Science.gov (United States)

Puzzarini, Cristina; Cazzoli, Gabriele; López, Juan Carlos; Alonso, José Luis; Baldacci, Agostino; Baldan, Alessandro; Stopkowicz, Stella; Cheng, Lan; Gauss, Jürgen

2012-07-14

Supported by accurate quantum-chemical calculations, the rotational spectra of the mono- and bi-deuterated species of fluoroiodomethane, CHDFI and CD(2)FI, as well as of the (13)C-containing species, (13)CH(2)FI, were recorded for the first time. Three different spectrometers were employed, a Fourier-transform microwave spectrometer, a millimeter/submillimter-wave spectrometer, and a THz spectrometer, thus allowing to record a huge portion of the rotational spectrum, from 5 GHz up to 1.05 THz, and to accurately determine the ground-state rotational and centrifugal-distortion constants. Sub-Doppler measurements allowed to resolve the hyperfine structure of the rotational spectrum and to determine the complete iodine quadrupole-coupling tensor as well as the diagonal elements of the iodine spin-rotation tensor. The present investigation of rare isotopic species of CH(2)FI together with the results previously obtained for the main isotopologue [C. Puzzarini, G. Cazzoli, J. C. López, J. L. Alonso, A. Baldacci, A. Baldan, S. Stopkowicz, L. Cheng, and J. Gauss, J. Chem. Phys. 134, 174312 (2011); G. Cazzoli, A. Baldacci, A. Baldan, and C. Puzzarini, Mol. Phys. 109, 2245 (2011)] enabled us to derive a semi-experimental equilibrium structure for fluoroiodomethane by means of a least-squares fit procedure using the available experimental ground-state rotational constants together with computed vibrational corrections. Problems related to the missing isotopic substitution of fluorine and iodine were overcome thanks to the availability of an accurate theoretical equilibrium geometry (computed at the coupled-cluster singles and doubles level augmented by a perturbative treatment of triple excitations).

Theoretical calculations of physico-chemical and spectroscopic properties of bioinorganic systems: current limits and perspectives.

Science.gov (United States)

Rokob, Tibor András; Srnec, Martin; Rulíšek, Lubomír

2012-05-21

In the last decade, we have witnessed substantial progress in the development of quantum chemical methodologies. Simultaneously, robust solvation models and various combined quantum and molecular mechanical (QM/MM) approaches have become an integral part of quantum chemical programs. Along with the steady growth of computer power and, more importantly, the dramatic increase of the computer performance to price ratio, this has led to a situation where computational chemistry, when exercised with the proper amount of diligence and expertise, reproduces, predicts, and complements the experimental data. In this perspective, we review some of the latest achievements in the field of theoretical (quantum) bioinorganic chemistry, concentrating mostly on accurate calculations of the spectroscopic and physico-chemical properties of open-shell bioinorganic systems by wave-function (ab initio) and DFT methods. In our opinion, the one-to-one mapping between the calculated properties and individual molecular structures represents a major advantage of quantum chemical modelling since this type of information is very difficult to obtain experimentally. Once (and only once) the physico-chemical, thermodynamic and spectroscopic properties of complex bioinorganic systems are quantitatively reproduced by theoretical calculations may we consider the outcome of theoretical modelling, such as reaction profiles and the various decompositions of the calculated parameters into individual spatial or physical contributions, to be reliable. In an ideal situation, agreement between theory and experiment may imply that the practical problem at hand, such as the reaction mechanism of the studied metalloprotein, can be considered as essentially solved.

Low-pressure phase diagram of crystalline benzene from quantum Monte Carlo

Energy Technology Data Exchange (ETDEWEB)

Azadi, Sam, E-mail: s.azadi@ucl.ac.uk [Departments of Physics and Astronomy, University College London, Thomas Young Center, London Centre for Nanotechnology, London WC1E 6BT (United Kingdom); Cohen, R. E. [Extreme Materials Initiative, Geophysical Laboratory, Carnegie Institution for Science, Washington, DC 20015 (United States); Department of Earth- and Environmental Sciences, Ludwig Maximilians Universität, Munich 80333 (Germany); Department of Physics and Astronomy, University College London, London WC1E 6BT (United Kingdom)

2016-08-14

We studied the low-pressure (0–10 GPa) phase diagram of crystalline benzene using quantum Monte Carlo and density functional theory (DFT) methods. We performed diffusion quantum Monte Carlo (DMC) calculations to obtain accurate static phase diagrams as benchmarks for modern van der Waals density functionals. Using density functional perturbation theory, we computed the phonon contributions to the free energies. Our DFT enthalpy-pressure phase diagrams indicate that the Pbca and P2{sub 1}/c structures are the most stable phases within the studied pressure range. The DMC Gibbs free-energy calculations predict that the room temperature Pbca to P2{sub 1}/c phase transition occurs at 2.1(1) GPa. This prediction is consistent with available experimental results at room temperature. Our DMC calculations give 50.6 ± 0.5 kJ/mol for crystalline benzene lattice energy.

Quantum-chemical calculations and electron diffraction study of the equilibrium molecular structure of vitamin K3

Science.gov (United States)

Khaikin, L. S.; Tikhonov, D. S.; Grikina, O. E.; Rykov, A. N.; Stepanov, N. F.

2014-05-01

The equilibrium molecular structure of 2-methyl-1,4-naphthoquinone (vitamin K3) having C s symmetry is experimentally characterized for the first time by means of gas-phase electron diffraction using quantum-chemical calculations and data on the vibrational spectra of related compounds.

Quantum mechanical calculation of electric fields and vibrational Stark shifts at active site of human aldose reductase.

Science.gov (United States)

Wang, Xianwei; Zhang, John Z H; He, Xiao

2015-11-14

Recent advance in biophysics has made it possible to directly measure site-specific electric field at internal sites of proteins using molecular probes with C = O or C≡N groups in the context of vibrational Stark effect. These measurements directly probe changes of electric field at specific protein sites due to, e.g., mutation and are very useful in protein design. Computational simulation of the Stark effect based on force fields such as AMBER and OPLS, while providing good insight, shows large errors in comparison to experimental measurement due to inherent difficulties associated with point charge based representation of force fields. In this study, quantum mechanical calculation of protein's internal electrostatic properties and vibrational Stark shifts was carried out by using electrostatically embedded generalized molecular fractionation with conjugate caps method. Quantum calculated change of mutation-induced electric field and vibrational Stark shift is reported at the internal probing site of enzyme human aldose reductase. The quantum result is in much better agreement with experimental data than those predicted by force fields, underscoring the deficiency of traditional point charge models describing intra-protein electrostatic properties.

Quantum mechanical calculation of electric fields and vibrational Stark shifts at active site of human aldose reductase

Energy Technology Data Exchange (ETDEWEB)

Wang, Xianwei [Center for Optics and Optoelectronics Research, College of Science, Zhejiang University of Technology, Hangzhou, Zhejiang 310023 (China); State Key Laboratory of Precision Spectroscopy, Institute of Theoretical and Computational Science, East China Normal University, Shanghai 200062 (China); Zhang, John Z. H.; He, Xiao, E-mail: xiaohe@phy.ecnu.edu.cn [State Key Laboratory of Precision Spectroscopy, Institute of Theoretical and Computational Science, East China Normal University, Shanghai 200062 (China); NYU-ECNU Center for Computational Chemistry at NYU Shanghai, Shanghai 200062 (China)

2015-11-14

Recent advance in biophysics has made it possible to directly measure site-specific electric field at internal sites of proteins using molecular probes with C = O or C≡N groups in the context of vibrational Stark effect. These measurements directly probe changes of electric field at specific protein sites due to, e.g., mutation and are very useful in protein design. Computational simulation of the Stark effect based on force fields such as AMBER and OPLS, while providing good insight, shows large errors in comparison to experimental measurement due to inherent difficulties associated with point charge based representation of force fields. In this study, quantum mechanical calculation of protein’s internal electrostatic properties and vibrational Stark shifts was carried out by using electrostatically embedded generalized molecular fractionation with conjugate caps method. Quantum calculated change of mutation-induced electric field and vibrational Stark shift is reported at the internal probing site of enzyme human aldose reductase. The quantum result is in much better agreement with experimental data than those predicted by force fields, underscoring the deficiency of traditional point charge models describing intra-protein electrostatic properties.

Virial theorem in the Kohn-Sham density-functional theory formalism: Accurate calculation of the atomic quantum theory of atoms in molecules energies

NARCIS (Netherlands)

Rodriguez, A.; Ayers, P.W.; Gotz, A.W.; Castillo-Alvarado, F.L.

2009-01-01

A new approach for computing the atom-in-molecule [quantum theory of atoms in molecule (QTAIM)] energies in Kohn-Sham density-functional theory is presented and tested by computing QTAIM energies for a set of representative molecules. In the new approach, the contribution for the correlation-kinetic

Quantum dynamics of quantum bits

International Nuclear Information System (INIS)

Nguyen, Bich Ha

2011-01-01

The theory of coherent oscillations of the matrix elements of the density matrix of the two-state system as a quantum bit is presented. Different calculation methods are elaborated in the case of a free quantum bit. Then the most appropriate methods are applied to the study of the density matrices of the quantum bits interacting with a classical pumping radiation field as well as with the quantum electromagnetic field in a single-mode microcavity. The theory of decoherence of a quantum bit in Markovian approximation is presented. The decoherence of a quantum bit interacting with monoenergetic photons in a microcavity is also discussed. The content of the present work can be considered as an introduction to the study of the quantum dynamics of quantum bits. (review)

A quantum accurate waveform synthesizer as a voltage reference for an electronic primary thermometer

Science.gov (United States)

Pollarolo, Alessio; Benz, Samuel; Rogalla, Horst; Dresselhaus, Paul

2014-03-01

We are using a quantum voltage noise source (QVNS) for use as an intrinsically accurate voltage reference for a new type of electronic temperature standard. In Johnson Noise Thermometry (JNT) the noise of a resistor is used to measure temperature or Boltzmann's constant k, because the Nyquist equation =4kTR Δf shows that the power spectral density is proportional to k, temperature T, resistance R and measurement bandwidth Δf . The QVNS is a digital to analog converter used to synthesize a voltage waveform that resembles pseudo-random noise comparable in amplitude to the resistor noise. The signal generated is a frequency comb of harmonics tones that are equally spaced in frequency, all having identical amplitudes but random phases. The QVNS is an array superconducting Josephson junctions that are biased with a pulsed waveform clocked at 10 GHz. The accuracy of the voltage waveform derives from the identical voltage pulses produced by each junction that are perfectly quantized because their time-integrals are always equal to flux quantum h/2 e. The time-dependent output voltage waveform is determined by the number of pulses and their density in time. The measurement electronics exploits cross-correlation techniques to reduce the uncorrelated measurement noise so as to reveal the resistor noise, both of which are on the order of 2 nV/ √Hz. With this technique we have measured k with an uncertainty of about one part in 105, which we hope to improve by another order of magnitude with further research.

Spectral response, dark current, and noise analyses in resonant tunneling quantum dot infrared photodetectors.

Science.gov (United States)

Jahromi, Hamed Dehdashti; Mahmoodi, Ali; Sheikhi, Mohammad Hossein; Zarifkar, Abbas

2016-10-20

Reduction of dark current at high-temperature operation is a great challenge in conventional quantum dot infrared photodetectors, as the rate of thermal excitations resulting in the dark current increases exponentially with temperature. A resonant tunneling barrier is the best candidate for suppression of dark current, enhancement in signal-to-noise ratio, and selective extraction of different wavelength response. In this paper, we use a physical model developed by the authors recently to design a proper resonant tunneling barrier for quantum infrared photodetectors and to study and analyze the spectral response of these devices. The calculated transmission coefficient of electrons by this model and its dependency on bias voltage are in agreement with experimental results. Furthermore, based on the calculated transmission coefficient, the dark current of a quantum dot infrared photodetector with a resonant tunneling barrier is calculated and compared with the experimental data. The validity of our model is proven through this comparison. Theoretical dark current by our model shows better agreement with the experimental data and is more accurate than the previously developed model. Moreover, noise in the device is calculated. Finally, the effect of different parameters, such as temperature, size of quantum dots, and bias voltage, on the performance of the device is simulated and studied.

Quantum calculations of the carrier mobility: Methodology, Matthiessen's rule, and comparison with semi-classical approaches

Energy Technology Data Exchange (ETDEWEB)

Niquet, Yann-Michel, E-mail: yniquet@cea.fr; Nguyen, Viet-Hung; Duchemin, Ivan [L-Sim, SP2M, UMR-E CEA/UJF-Grenoble 1, INAC, Grenoble (France); Triozon, François [CEA, LETI-MINATEC, Grenoble (France); Nier, Olivier; Rideau, Denis [ST Microelectronics, Crolles (France)

2014-02-07

We discuss carrier mobilities in the quantum Non-Equilibrium Green's Functions (NEGF) framework. We introduce a method for the extraction of the mobility that is free from contact resistance contamination and with minimal needs for ensemble averages. We focus on silicon thin films as an illustration, although the method can be applied to various materials such as semiconductor nanowires or carbon nanostructures. We then introduce a new paradigm for the definition of the partial mobility μ{sub M} associated with a given elastic scattering mechanism “M,” taking phonons (PH) as a reference (μ{sub M}{sup −1}=μ{sub PH+M}{sup −1}−μ{sub PH}{sup −1}). We argue that this definition makes better sense in a quantum transport framework as it is free from long range interference effects that can appear in purely ballistic calculations. As a matter of fact, these mobilities satisfy Matthiessen's rule for three mechanisms [e.g., surface roughness (SR), remote Coulomb scattering (RCS) and phonons] much better than the usual, single mechanism calculations. We also discuss the problems raised by the long range spatial correlations in the RCS disorder. Finally, we compare semi-classical Kubo-Greenwood (KG) and quantum NEGF calculations. We show that KG and NEGF are in reasonable agreement for phonon and RCS, yet not for SR. We discuss the reasons for these discrepancies.

On the acceptor-related photoluminescence spectra of GaAs quantum-wire microcrystals: A model calculation

International Nuclear Information System (INIS)

Oliveira, L.E.; Porras Montenegro, N.; Latge, A.

1992-07-01

The acceptor-related photoluminescence spectrum of a GaAs quantum-wire microcrystal is theoretically investigated via a model calculation within the effective-mass approximation, with the acceptor envelope wave functions and binding energies calculated through a variational procedure. Typical theoretical photoluminescence spectra show two peaks associated to transitions from the n = 1 conduction subband electron gas to acceptors at the on-center and on-edge positions in the wire in good agreement with the recent experimental results by Hirum et al. (Appl. Phys. Lett. 59, 431 (1991)). (author). 14 refs, 3 figs

Application of the CRAY-1 for quantum chemistry calculations

International Nuclear Information System (INIS)

Saunders, V.R.; Guest, M.F.

1982-01-01

The following steps in a typical quantum chemistry calculation will be considered: 1. Gaussian integrals evaluation. 2. Hartree-Fock computation of an uncorrelated wavefunction. 3. 4-index transformation of two-electron integrals. 4. Configuration interaction calculations of a correlated wavefunction. In all the above steps we have found that algorithms may be devised which formulate the problem as being dominated by a series of matrix multiplications: R=AB, where A (or B) is sparse. A routine for performing the sparse matrix multiply has been prepared with a maximum measured performance of 147 M flops. When this routine is used in our applications packages, overall performance of approximately 50, 100 and 120 M flops are observed for steps 1, 3 and 4, respectively. The result in step 2 is not so successful, as effective implementation of the matrix multiplication requires efficient performance of data gather and scatter sequences (not vectorisable on the CRAY-1), and a performance of 10 M flops is observed. The importance of gather/scatter sequences in such operations as file sorting is pointed out. The present performance is compared with that previously obtained on CDC 7600 equipment and from this data we deduce the cost-effectiveness of the CRAY-1 in our field. (orig.)

Piezo-optic tensor of crystals from quantum-mechanical calculations.

Science.gov (United States)

Erba, A; Ruggiero, M T; Korter, T M; Dovesi, R

2015-10-14

An automated computational strategy is devised for the ab initio determination of the full fourth-rank piezo-optic tensor of crystals belonging to any space group of symmetry. Elastic stiffness and compliance constants are obtained as numerical first derivatives of analytical energy gradients with respect to the strain and photo-elastic constants as numerical derivatives of analytical dielectric tensor components, which are in turn computed through a Coupled-Perturbed-Hartree-Fock/Kohn-Sham approach, with respect to the strain. Both point and translation symmetries are exploited at all steps of the calculation, within the framework of periodic boundary conditions. The scheme is applied to the determination of the full set of ten symmetry-independent piezo-optic constants of calcium tungstate CaWO4, which have recently been experimentally reconstructed. Present calculations unambiguously determine the absolute sign (positive) of the π61 constant, confirm the reliability of 6 out of 10 experimentally determined constants and provide new, more accurate values for the remaining 4 constants.

The molecular structure of 4-methylpyridine-N-oxide: Gas-phase electron diffraction and quantum chemical calculations

Science.gov (United States)

Belova, Natalya V.; Girichev, Georgiy V.; Kotova, Vitaliya E.; Korolkova, Kseniya A.; Trang, Nguyen Hoang

2018-03-01

The molecular structure of 4-methylpiridine-N-oxide, 4-MePyO, has been studied by gas-phase electron diffraction monitored by mass spectrometry (GED/MS) and quantum chemical (DFT) calculations. Both, quantum chemistry and GED analyses resulted in CS molecular symmetry with the planar pyridine ring. Obtained molecular parameters confirm the hyperconjugation in the pyridine ring and the sp2 hybridization concept of the nitrogen and carbon atoms in the ring. The experimental geometric parameters are in a good agreement with the parameters for non-substituted N-oxide and reproduced very closely by DFT calculations. The presence of the electron-donating CH3 substituent in 4-MePyO leads to a decrease of the ipso-angle and to an increase of r(N→O) in comparison with the non-substituted PyO. Electron density distribution analysis has been performed in terms of natural bond orbitals (NBO) scheme. The nature of the semipolar N→O bond is discussed.

Accurate line intensities of methane from first-principles calculations

Science.gov (United States)

Nikitin, Andrei V.; Rey, Michael; Tyuterev, Vladimir G.

2017-10-01

In this work, we report first-principle theoretical predictions of methane spectral line intensities that are competitive with (and complementary to) the best laboratory measurements. A detailed comparison with the most accurate data shows that discrepancies in integrated polyad intensities are in the range of 0.4%-2.3%. This corresponds to estimations of the best available accuracy in laboratory Fourier Transform spectra measurements for this quantity. For relatively isolated strong lines the individual intensity deviations are in the same range. A comparison with the most precise laser measurements of the multiplet intensities in the 2ν3 band gives an agreement within the experimental error margins (about 1%). This is achieved for the first time for five-atomic molecules. In the Supplementary Material we provide the lists of theoretical intensities at 269 K for over 5000 strongest transitions in the range below 6166 cm-1. The advantage of the described method is that this offers a possibility to generate fully assigned exhaustive line lists at various temperature conditions. Extensive calculations up to 12,000 cm-1 including high-T predictions will be made freely available through the TheoReTS information system (http://theorets.univ-reims.fr, http://theorets.tsu.ru) that contains ab initio born line lists and provides a user-friendly graphical interface for a fast simulation of the absorption cross-sections and radiance.

Quantum Dynamical Behaviour in Complex Systems - A Semiclassical Approach

Energy Technology Data Exchange (ETDEWEB)

Ananth, Nandini [Univ. of California, Berkeley, CA (United States)

2008-01-01

One of the biggest challenges in Chemical Dynamics is describing the behavior of complex systems accurately. Classical MD simulations have evolved to a point where calculations involving thousands of atoms are routinely carried out. Capturing coherence, tunneling and other such quantum effects for these systems, however, has proven considerably harder. Semiclassical methods such as the Initial Value Representation (SC-IVR) provide a practical way to include quantum effects while still utilizing only classical trajectory information. For smaller systems, this method has been proven to be most effective, encouraging the hope that it can be extended to deal with a large number of degrees of freedom. Several variations upon the original idea of the SCIVR have been developed to help make these larger calculations more tractable; these range from the simplest, classical limit form, the Linearized IVR (LSC-IVR) to the quantum limit form, the Exact Forward-Backward version (EFB-IVR). In this thesis a method to tune between these limits is described which allows us to choose exactly which degrees of freedom we wish to treat in a more quantum mechanical fashion and to what extent. This formulation is called the Tuning IVR (TIVR). We further describe methodology being developed to evaluate the prefactor term that appears in the IVR formalism. The regular prefactor is composed of the Monodromy matrices (jacobians of the transformation from initial to finial coordinates and momenta) which are time evolved using the Hessian. Standard MD simulations require the potential surfaces and their gradients, but very rarely is there any information on the second derivative. We would like to be able to carry out the SC-IVR calculation without this information too. With this in mind a finite difference scheme to obtain the Hessian on-the-fly is proposed. Wealso apply the IVR formalism to a few problems of current interest. A method to obtain energy eigenvalues accurately for complex

QmeQ 1.0: An open-source Python package for calculations of transport through quantum dot devices

DEFF Research Database (Denmark)

Kiršanskas, Gediminas; Pedersen, Jonas Nyvold; Karlström, Olov

2017-01-01

QmeQ is an open-source Python package for numerical modeling of transport through quantum dot devices with strong electron–electron interactions using various approximate master equation approaches. The package provides a framework for calculating stationary particle or energy currents driven...

Expectation values of $r^{q}$ between Dirac and quasirelativistic wave functions in the quantum-defect approximation

CERN Document Server

Kwato-Njock, M G; Oumarou, B

2002-01-01

A search is conducted for the determination of expectation values of $r^q$ between Dirac and quasirelativistic radial wave functions in the quantum-defect approximation. The phenomenological and supersymmetry-inspired quantum-defect models which have proven so far to yield accurate results are used. The recursive structure of formulae derived on the basis of the hypervirial theorem enables us to develop explicit relations for arbitrary values of $q$. Detailed numerical calculations concerning alkali-metal-like ions of the Li-, Na- and Cu-iso electronic sequences confirm the superiority of supersymmetry-based quantum-defect theory over quantum-defect orbital and exact orbital quantum number approximations. It is also shown that relativistic rather than quasirelativistic treatment may be used for consistent inclusion of relativistic effects.

Calculation of molecular free energies in classical potentials

International Nuclear Information System (INIS)

Farhi, Asaf; Singh, Bipin

2016-01-01

Free energies of molecules can be calculated by quantum chemistry computations or by normal mode classical calculations. However, the first can be computationally impractical for large molecules and the second is based on the assumption of harmonic dynamics. We present a novel, accurate and complete calculation of molecular free energies in standard classical potentials. In this method we transform the molecule by relaxing potential terms which depend on the coordinates of a group of atoms in that molecule and calculate the free energy difference associated with the transformation. Then, since the transformed molecule can be treated as non-interacting systems, the free energy associated with these atoms is analytically or numerically calculated. This two-step calculation can be applied to calculate free energies of molecules or free energy difference between (possibly large) molecules in a general environment. We demonstrate the method in free energy calculations for methanethiol and butane molecules in vacuum and solvent. We suggest the potential application of free energy calculation of chemical reactions in classical molecular simulations. (paper)

Direct Quantum Dynamics Using Grid-Based Wave Function Propagation and Machine-Learned Potential Energy Surfaces.

Science.gov (United States)

Richings, Gareth W; Habershon, Scott

2017-09-12

We describe a method for performing nuclear quantum dynamics calculations using standard, grid-based algorithms, including the multiconfiguration time-dependent Hartree (MCTDH) method, where the potential energy surface (PES) is calculated "on-the-fly". The method of Gaussian process regression (GPR) is used to construct a global representation of the PES using values of the energy at points distributed in molecular configuration space during the course of the wavepacket propagation. We demonstrate this direct dynamics approach for both an analytical PES function describing 3-dimensional proton transfer dynamics in malonaldehyde and for 2- and 6-dimensional quantum dynamics simulations of proton transfer in salicylaldimine. In the case of salicylaldimine we also perform calculations in which the PES is constructed using Hartree-Fock calculations through an interface to an ab initio electronic structure code. In all cases, the results of the quantum dynamics simulations are in excellent agreement with previous simulations of both systems yet do not require prior fitting of a PES at any stage. Our approach (implemented in a development version of the Quantics package) opens a route to performing accurate quantum dynamics simulations via wave function propagation of many-dimensional molecular systems in a direct and efficient manner.

Preface: Special Topic: From Quantum Mechanics to Force Fields

Science.gov (United States)

Piquemal, Jean-Philip; Jordan, Kenneth D.

2017-10-01

This Special Topic issue entitled "From Quantum Mechanics to Force Fields" is dedicated to the ongoing efforts of the theoretical chemistry community to develop a new generation of accurate force fields based on data from high-level electronic structure calculations and to develop faster electronic structure methods for testing and designing force fields as well as for carrying out simulations. This issue includes a collection of 35 original research articles that illustrate recent theoretical advances in the field. It provides a timely snapshot of recent developments in the generation of approaches to enable more accurate molecular simulations of processes important in chemistry, physics, biophysics, and materials science.

Ab initio quantum chemical calculation as a tool of evaluating diamagnetic susceptibility of magnetically levitating substances

International Nuclear Information System (INIS)

Fujiwara, Y; Tanimoto, Y

2009-01-01

On magnetic force evaluation necessary for magnetically levitated diamagnetic substances, isotropic diamagnetic susceptibility estimation by the ab initio quantum chemical calculation using Gaussian03W was verified for more than 300 molecules in a viewpoint of the accuracy in the absolute value and the calculation level affording good cost performance. From comparison, the method of B3PW91 / 6-311+G(d,p) was found to give the adequate absolute value by the relation of (observed) = (1.03 ± 0.005) x (calculated) - (1.22 ± 0.60) x 10 -6 in a unit of cm 3 mol -1 and good cost performance.

Ab initio quantum chemical calculation as a tool of evaluating diamagnetic susceptibility of magnetically levitating substances

Energy Technology Data Exchange (ETDEWEB)

Fujiwara, Y [Department of Mathematical and Life Sciences, Graduate School of Science, Hiroshima University, Higashi-Hiroshima, Hiroshima 739-8526 (Japan); Tanimoto, Y [Faculty of Pharmacy, Osaka Ohtani University, Nishikiorikita, Tondabayashi 584-8540 (Japan)], E-mail: fuji0710@sci.hiroshima-u.ac.jp

2009-03-01

On magnetic force evaluation necessary for magnetically levitated diamagnetic substances, isotropic diamagnetic susceptibility estimation by the ab initio quantum chemical calculation using Gaussian03W was verified for more than 300 molecules in a viewpoint of the accuracy in the absolute value and the calculation level affording good cost performance. From comparison, the method of B3PW91 / 6-311+G(d,p) was found to give the adequate absolute value by the relation of (observed) = (1.03 {+-} 0.005) x (calculated) - (1.22 {+-} 0.60) x 10{sup -6} in a unit of cm{sup 3} mol{sup -1} and good cost performance.

High-fidelity quantum driving

DEFF Research Database (Denmark)

Bason, Mark George; Viteau, Matthieu; Malossi, Nicola

2011-01-01

Accurately controlling a quantum system is a fundamental requirement in quantum information processing and the coherent manipulation of molecular systems. The ultimate goal in quantum control is to prepare a desired state with the highest fidelity allowed by the available resources...... and the experimental constraints. Here we experimentally implement two optimal high-fidelity control protocols using a two-level quantum system comprising Bose–Einstein condensates in optical lattices. The first is a short-cut protocol that reaches the maximum quantum-transformation speed compatible...

Expectation values of r sup q between Dirac and quasirelativistic wave functions in the quantum-defect approximation

CERN Document Server

Kwato-Njock, K

2002-01-01

A search is conducted for the determination of expectation values of r sup q between Dirac and quasirelativistic radial wave functions in the quantum-defect approximation. The phenomenological and supersymmetry-inspired quantum-defect models which have proven so far to yield accurate results are used. The recursive structure of formulae derived on the basis of the hypervirial theorem enables us to develop explicit relations for arbitrary values of q. Detailed numerical calculations concerning alkali-metal-like ions of the Li-, Na- and Cu-iso electronic sequences confirm the superiority of supersymmetry-based quantum-defect theory over quantum-defect orbital and exact orbital quantum number approximations. It is also shown that relativistic rather than quasirelativistic treatment may be used for consistent inclusion of relativistic effects.

Density-functional theory simulation of large quantum dots

Science.gov (United States)

Jiang, Hong; Baranger, Harold U.; Yang, Weitao

2003-10-01

Kohn-Sham spin-density functional theory provides an efficient and accurate model to study electron-electron interaction effects in quantum dots, but its application to large systems is a challenge. Here an efficient method for the simulation of quantum dots using density-function theory is developed; it includes the particle-in-the-box representation of the Kohn-Sham orbitals, an efficient conjugate-gradient method to directly minimize the total energy, a Fourier convolution approach for the calculation of the Hartree potential, and a simplified multigrid technique to accelerate the convergence. We test the methodology in a two-dimensional model system and show that numerical studies of large quantum dots with several hundred electrons become computationally affordable. In the noninteracting limit, the classical dynamics of the system we study can be continuously varied from integrable to fully chaotic. The qualitative difference in the noninteracting classical dynamics has an effect on the quantum properties of the interacting system: integrable classical dynamics leads to higher-spin states and a broader distribution of spacing between Coulomb blockade peaks.

A programmable quantum current standard from the Josephson and the quantum Hall effects

Energy Technology Data Exchange (ETDEWEB)

Poirier, W., E-mail: wilfrid.poirier@lne.fr; Lafont, F.; Djordjevic, S.; Schopfer, F.; Devoille, L. [Quantum metrology group, Laboratoire National de métrologie et d' Essais, 29 avenue Roger Hennequin, 78197 Trappes (France)

2014-01-28

We propose a way to realize a programmable quantum current standard (PQCS) from the Josephson voltage standard and the quantum Hall resistance standard (QHR) exploiting the multiple connection technique provided by the quantum Hall effect (QHE) and the exactness of the cryogenic current comparator. The PQCS could lead to breakthroughs in electrical metrology like the realization of a programmable quantum current source, a quantum ampere-meter, and a simplified closure of the quantum metrological triangle. Moreover, very accurate universality tests of the QHE could be performed by comparing PQCS based on different QHRs.

Extension of PT-symmetric quantum mechanics to quantum field theory with cubic interaction

International Nuclear Information System (INIS)

Bender, Carl M.; Brody, Dorje C.; Jones, Hugh F.

2004-01-01

It has recently been shown that a non-Hermitian Hamiltonian H possessing an unbroken PT symmetry (i) has a real spectrum that is bounded below, and (ii) defines a unitary theory of quantum mechanics with positive norm. The proof of unitarity requires a linear operator C, which was originally defined as a sum over the eigenfunctions of H. However, using this definition to calculate C is cumbersome in quantum mechanics and impossible in quantum field theory. An alternative method is devised here for calculating C directly in terms of the operator dynamical variables of the quantum theory. This method is general and applies to a variety of quantum mechanical systems having several degrees of freedom. More importantly, this method is used to calculate the C operator in quantum field theory. The C operator is a time-independent observable in PT-symmetric quantum field theory

Cation solvation with quantum chemical effects modeled by a size-consistent multi-partitioning quantum mechanics/molecular mechanics method.

Science.gov (United States)

Watanabe, Hiroshi C; Kubillus, Maximilian; Kubař, Tomáš; Stach, Robert; Mizaikoff, Boris; Ishikita, Hiroshi

2017-07-21

In the condensed phase, quantum chemical properties such as many-body effects and intermolecular charge fluctuations are critical determinants of the solvation structure and dynamics. Thus, a quantum mechanical (QM) molecular description is required for both solute and solvent to incorporate these properties. However, it is challenging to conduct molecular dynamics (MD) simulations for condensed systems of sufficient scale when adapting QM potentials. To overcome this problem, we recently developed the size-consistent multi-partitioning (SCMP) quantum mechanics/molecular mechanics (QM/MM) method and realized stable and accurate MD simulations, using the QM potential to a benchmark system. In the present study, as the first application of the SCMP method, we have investigated the structures and dynamics of Na + , K + , and Ca 2+ solutions based on nanosecond-scale sampling, a sampling 100-times longer than that of conventional QM-based samplings. Furthermore, we have evaluated two dynamic properties, the diffusion coefficient and difference spectra, with high statistical certainty. Furthermore the calculation of these properties has not previously been possible within the conventional QM/MM framework. Based on our analysis, we have quantitatively evaluated the quantum chemical solvation effects, which show distinct differences between the cations.

Preparation of freezing quantum state for quantum coherence

Science.gov (United States)

Yang, Lian-Wu; Man, Zhong-Xiao; Zhang, Ying-Jie; Han, Feng; Du, Shao-jiang; Xia, Yun-Jie

2018-06-01

We provide a method to prepare the freezing quantum state for quantum coherence via unitary operations. The initial product state consists of the control qubit and target qubit; when it satisfies certain conditions, the initial product state converts into the particular Bell diagonal state under the unitary operations, which have the property of freezing of quantum coherence under quantum channels. We calculate the frozen quantum coherence and corresponding quantum correlations, and find that the quantities are determined by the control qubit only when the freezing phenomena occur.

Modeling classical and quantum radiation from laser-plasma accelerators

Directory of Open Access Journals (Sweden)

M. Chen

2013-03-01

Full Text Available The development of models and the “Virtual Detector for Synchrotron Radiation” (vdsr code that accurately describe the production of synchrotron radiation are described. These models and code are valid in the classical and linear (single-scattering quantum regimes and are capable of describing radiation produced from laser-plasma accelerators (LPAs through a variety of mechanisms including betatron radiation, undulator radiation, and Thomson/Compton scattering. Previous models of classical synchrotron radiation, such as those typically used for undulator radiation, are inadequate in describing the radiation spectra from electrons undergoing small numbers of oscillations. This is due to an improper treatment of a mathematical evaluation at the end points of an integration that leads to an unphysical plateau in the radiation spectrum at high frequencies, the magnitude of which increases as the number of oscillation periods decreases. This is important for betatron radiation from LPAs, in which the betatron strength parameter is large but the number of betatron periods is small. The code vdsr allows the radiation to be calculated in this regime by full integration over each electron trajectory, including end-point effects, and this code is used to calculate betatron radiation for cases of experimental interest. Radiation from Thomson scattering and Compton scattering is also studied with vdsr. For Thomson scattering, radiation reaction is included by using the Sokolov method for the calculation of the electron dynamics. For Compton scattering, quantum recoil effects are considered in vdsr by using Monte Carlo methods. The quantum calculation has been benchmarked with the classical calculation in a classical regime.

Tensor-decomposed vibrational coupled-cluster theory: Enabling large-scale, highly accurate vibrational-structure calculations

Science.gov (United States)

Madsen, Niels Kristian; Godtliebsen, Ian H.; Losilla, Sergio A.; Christiansen, Ove

2018-01-01

A new implementation of vibrational coupled-cluster (VCC) theory is presented, where all amplitude tensors are represented in the canonical polyadic (CP) format. The CP-VCC algorithm solves the non-linear VCC equations without ever constructing the amplitudes or error vectors in full dimension but still formally includes the full parameter space of the VCC[n] model in question resulting in the same vibrational energies as the conventional method. In a previous publication, we have described the non-linear-equation solver for CP-VCC calculations. In this work, we discuss the general algorithm for evaluating VCC error vectors in CP format including the rank-reduction methods used during the summation of the many terms in the VCC amplitude equations. Benchmark calculations for studying the computational scaling and memory usage of the CP-VCC algorithm are performed on a set of molecules including thiadiazole and an array of polycyclic aromatic hydrocarbons. The results show that the reduced scaling and memory requirements of the CP-VCC algorithm allows for performing high-order VCC calculations on systems with up to 66 vibrational modes (anthracene), which indeed are not possible using the conventional VCC method. This paves the way for obtaining highly accurate vibrational spectra and properties of larger molecules.

Quantum Dot Systems : A versatile platform for quantum simulations

NARCIS (Netherlands)

Barthelemy, P.J.C.; Vandersypen, L.M.K.

2013-01-01

Quantum mechanics often results in extremely complex phenomena, especially when the quantum system under consideration is composed of many interacting particles. The states of these many-body systems live in a space so large that classical numerical calculations cannot compute them. Quantum

Accurate calculation of high harmonics generated by relativistic Thomson scattering

International Nuclear Information System (INIS)

Popa, Alexandru

2008-01-01

The recent emergence of the field of ultraintense laser pulses, corresponding to beam intensities higher than 10 18 W cm -2 , brings about the problem of the high harmonic generation (HHG) by the relativistic Thomson scattering of the electromagnetic radiation by free electrons. Starting from the equations of the relativistic motion of the electron in the electromagnetic field, we give an exact solution of this problem. Taking into account the Lienard-Wiechert equations, we obtain a periodic scattered electromagnetic field. Without loss of generality, the solution is strongly simplified by observing that the electromagnetic field is always normal to the direction electron-detector. The Fourier series expansion of this field leads to accurate expressions of the high harmonics generated by the Thomson scattering. Our calculations lead to a discrete HHG spectrum, whose shape and angular distribution are in agreement with the experimental data from the literature. Since no approximations were made, our approach is also valid in the ultrarelativistic regime, corresponding to intensities higher than 10 23 W cm -2 , where it predicts a strong increase of the HHG intensities and of the order of harmonics. In this domain, the nonlinear Thomson scattering could be an efficient source of hard x-rays

Accurate DFT-D3 Calculations in a Small Basis Set

Czech Academy of Sciences Publication Activity Database

Hostaš, Jiří; Řezáč, Jan

2017-01-01

Roč. 13, č. 8 (2017), s. 3575-3585 ISSN 1549-9618 R&D Projects: GA ČR(CZ) GJ16-11321Y Institutional support: RVO:61388963 Keywords : density functional theory * molecular orbital methods * quantum chemical methods Subject RIV: CF - Physical ; Theoretical Chemistry OBOR OECD: Physical chemistry Impact factor: 5.245, year: 2016

Geometric constraints in semiclassical initial value representation calculations in Cartesian coordinates: accurate reduction in zero-point energy.

Science.gov (United States)

Issack, Bilkiss B; Roy, Pierre-Nicholas

2005-08-22

An approach for the inclusion of geometric constraints in semiclassical initial value representation calculations is introduced. An important aspect of the approach is that Cartesian coordinates are used throughout. We devised an algorithm for the constrained sampling of initial conditions through the use of multivariate Gaussian distribution based on a projected Hessian. We also propose an approach for the constrained evaluation of the so-called Herman-Kluk prefactor in its exact log-derivative form. Sample calculations are performed for free and constrained rare-gas trimers. The results show that the proposed approach provides an accurate evaluation of the reduction in zero-point energy. Exact basis set calculations are used to assess the accuracy of the semiclassical results. Since Cartesian coordinates are used, the approach is general and applicable to a variety of molecular and atomic systems.

Pseudopotentials for quantum-Monte-Carlo-calculations; Pseudopotentiale fuer Quanten-Monte-Carlo-Rechnungen

Energy Technology Data Exchange (ETDEWEB)

Burkatzki, Mark Thomas

2008-07-01

The author presents scalar-relativistic energy-consistent Hartree-Fock pseudopotentials for the main-group and 3d-transition-metal elements. The pseudopotentials do not exhibit a singularity at the nucleus and are therefore suitable for quantum Monte Carlo (QMC) calculations. The author demonstrates their transferability through extensive benchmark calculations of atomic excitation spectra as well as molecular properties. In particular, the author computes the vibrational frequencies and binding energies of 26 first- and second-row diatomic molecules using post Hartree-Fock methods, finding excellent agreement with the corresponding all-electron values. The author shows that the presented pseudopotentials give superior accuracy than other existing pseudopotentials constructed specifically for QMC. The localization error and the efficiency in QMC are discussed. The author also presents QMC calculations for selected atomic and diatomic 3d-transitionmetal systems. Finally, valence basis sets of different sizes (VnZ with n=D,T,Q,5 for 1st and 2nd row; with n=D,T for 3rd to 5th row; with n=D,T,Q for the 3d transition metals) optimized for the pseudopotentials are presented. (orig.)

Controllable conditional quantum oscillations and quantum gate operations in superconducting flux qubits

International Nuclear Information System (INIS)

Chen Aimin; Cho Samyoung

2011-01-01

Conditional quantum oscillations are investigated for quantum gate operations in superconducting flux qubits. We present an effective Hamiltonian which describes a conditional quantum oscillation in two-qubit systems. Rabi-type quantum oscillations are discussed in implementing conditional quantum oscillations to quantum gate operations. Two conditional quantum oscillations depending on the states of control qubit can be synchronized to perform controlled-gate operations by varying system parameters. It is shown that the conditional quantum oscillations with their frequency synchronization make it possible to operate the controlled-NOT and -U gates with a very accurate gate performance rate in interacting qubit systems. Further, this scheme can be applicable to realize a controlled multi-qubit operation in various solid-state qubit systems. (author)

Canonical partition functions: ideal quantum gases, interacting classical gases, and interacting quantum gases

Science.gov (United States)

Zhou, Chi-Chun; Dai, Wu-Sheng

2018-02-01

In statistical mechanics, for a system with a fixed number of particles, e.g. a finite-size system, strictly speaking, the thermodynamic quantity needs to be calculated in the canonical ensemble. Nevertheless, the calculation of the canonical partition function is difficult. In this paper, based on the mathematical theory of the symmetric function, we suggest a method for the calculation of the canonical partition function of ideal quantum gases, including ideal Bose, Fermi, and Gentile gases. Moreover, we express the canonical partition functions of interacting classical and quantum gases given by the classical and quantum cluster expansion methods in terms of the Bell polynomial in mathematics. The virial coefficients of ideal Bose, Fermi, and Gentile gases are calculated from the exact canonical partition function. The virial coefficients of interacting classical and quantum gases are calculated from the canonical partition function by using the expansion of the Bell polynomial, rather than calculated from the grand canonical potential.

Accurate thermodynamic relations of the melting temperature of nanocrystals with different shapes and pure theoretical calculation

Energy Technology Data Exchange (ETDEWEB)

Zhu, Jinhua; Fu, Qingshan; Xue, Yongqiang, E-mail: xyqlw@126.com; Cui, Zixiang

2017-05-01

Based on the surface pre-melting model, accurate thermodynamic relations of the melting temperature of nanocrystals with different shapes (tetrahedron, cube, octahedron, dodecahedron, icosahedron, nanowire) were derived. The theoretically calculated melting temperatures are in relative good agreements with experimental, molecular dynamic simulation and other theoretical results for nanometer Au, Ag, Al, In and Pb. It is found that the particle size and shape have notable effects on the melting temperature of nanocrystals, and the smaller the particle size, the greater the effect of shape. Furthermore, at the same equivalent radius, the more the shape deviates from sphere, the lower the melting temperature is. The value of melting temperature depression of cylindrical nanowire is just half of that of spherical nanoparticle with an identical radius. The theoretical relations enable one to quantitatively describe the influence regularities of size and shape on the melting temperature and to provide an effective way to predict and interpret the melting temperature of nanocrystals with different sizes and shapes. - Highlights: • Accurate relations of T{sub m} of nanocrystals with various shapes are derived. • Calculated T{sub m} agree with literature results for nano Au, Ag, Al, In and Pb. • ΔT{sub m} (nanowire) = 0.5ΔT{sub m} (spherical nanocrystal). • The relations apply to predict and interpret the melting behaviors of nanocrystals.

Parallelizing the QUDA Library for Multi-GPU Calculations in Lattice Quantum Chromodynamics

Energy Technology Data Exchange (ETDEWEB)

Ronald Babich, Michael Clark, Balint Joo

2010-11-01

Graphics Processing Units (GPUs) are having a transformational effect on numerical lattice quantum chromodynamics (LQCD) calculations of importance in nuclear and particle physics. The QUDA library provides a package of mixed precision sparse matrix linear solvers for LQCD applications, supporting single GPUs based on NVIDIA's Compute Unified Device Architecture (CUDA). This library, interfaced to the QDP++/Chroma framework for LQCD calculations, is currently in production use on the "9g" cluster at the Jefferson Laboratory, enabling unprecedented price/performance for a range of problems in LQCD. Nevertheless, memory constraints on current GPU devices limit the problem sizes that can be tackled. In this contribution we describe the parallelization of the QUDA library onto multiple GPUs using MPI, including strategies for the overlapping of communication and computation. We report on both weak and strong scaling for up to 32 GPUs interconnected by InfiniBand, on which we sustain in excess of 4 Tflops.

Parallelizing the QUDA Library for Multi-GPU Calculations in Lattice Quantum Chromodynamics

International Nuclear Information System (INIS)

Babich, Ronald; Clark, Michael; Joo, Balint

2010-01-01

Graphics Processing Units (GPUs) are having a transformational effect on numerical lattice quantum chromodynamics (LQCD) calculations of importance in nuclear and particle physics. The QUDA library provides a package of mixed precision sparse matrix linear solvers for LQCD applications, supporting single GPUs based on NVIDIA's Compute Unified Device Architecture (CUDA). This library, interfaced to the QDP++/Chroma framework for LQCD calculations, is currently in production use on the '9g' cluster at the Jefferson Laboratory, enabling unprecedented price/performance for a range of problems in LQCD. Nevertheless, memory constraints on current GPU devices limit the problem sizes that can be tackled. In this contribution we describe the parallelization of the QUDA library onto multiple GPUs using MPI, including strategies for the overlapping of communication and computation. We report on both weak and strong scaling for up to 32 GPUs interconnected by InfiniBand, on which we sustain in excess of 4 Tflops.

The Over-Barrier Resonant States and Multi-Channel Scattering in Multiple Quantum Wells

Directory of Open Access Journals (Sweden)

A Polupanov

2016-09-01

Full Text Available We demonstrate an explicit numerical method for accurate calculation of the scattering matrix and its poles, and apply this method to describe the multi-channel scattering in the multiple quantum-wells structures. The S-matrix is continued analytically to the unphysical region of complex energy values. Results of calculations show that there exist one or more S-matrix poles, corresponding to the over-barrier resonant states critical for the effect of the absolute reflection of holes in the energy range where only the heavy ones may propagate over barriers in a structure. Light- and heavy-hole states are described by the Luttinger Hamiltonian matrix. In contrast to the single quantum-well case, at some parameters of a multiple quantum-wells structure the number of S-matrix poles may exceed that of the absolute reflection peaks, and at different values of parameters the absolute reflection peak corresponds to different resonant states. The imaginary parts of the S-matrix poles and hence the lifetimes of resonant states as well as the widths of resonant peaks of absolute reflection depend drastically on the quantum-well potential depth. In the case of shallow quantum wells there is in fact a long-living over-barrier resonant hole state.

Kohn-Sham orbitals and potentials from quantum Monte Carlo molecular densities

International Nuclear Information System (INIS)

Varsano, Daniele; Barborini, Matteo; Guidoni, Leonardo

2014-01-01

In this work we show the possibility to extract Kohn-Sham orbitals, orbital energies, and exchange correlation potentials from accurate Quantum Monte Carlo (QMC) densities for atoms (He, Be, Ne) and molecules (H 2 , Be 2 , H 2 O, and C 2 H 4 ). The Variational Monte Carlo (VMC) densities based on accurate Jastrow Antisymmetrised Geminal Power wave functions are calculated through different estimators. Using these reference densities, we extract the Kohn-Sham quantities with the method developed by Zhao, Morrison, and Parr (ZMP) [Phys. Rev. A 50, 2138 (1994)]. We compare these extracted quantities with those obtained form CISD densities and with other data reported in the literature, finding a good agreement between VMC and other high-level quantum chemistry methods. Our results demonstrate the applicability of the ZMP procedure to QMC molecular densities, that can be used for the testing and development of improved functionals and for the implementation of embedding schemes based on QMC and Density Functional Theory

Quantum-information processing in disordered and complex quantum systems

International Nuclear Information System (INIS)

Sen, Aditi; Sen, Ujjwal; Ahufinger, Veronica; Briegel, Hans J.; Sanpera, Anna; Lewenstein, Maciej

2006-01-01

We study quantum information processing in complex disordered many body systems that can be implemented by using lattices of ultracold atomic gases and trapped ions. We demonstrate, first in the short range case, the generation of entanglement and the local realization of quantum gates in a disordered magnetic model describing a quantum spin glass. We show that in this case it is possible to achieve fidelities of quantum gates higher than in the classical case. Complex systems with long range interactions, such as ions chains or dipolar atomic gases, can be used to model neural network Hamiltonians. For such systems, where both long range interactions and disorder appear, it is possible to generate long range bipartite entanglement. We provide an efficient analytical method to calculate the time evolution of a given initial state, which in turn allows us to calculate its quantum correlations

Comment on "Modified quantum-speed-limit bounds for open quantum dynamics in quantum channels"

Science.gov (United States)

Mirkin, Nicolás; Toscano, Fabricio; Wisniacki, Diego A.

2018-04-01

In a recent paper [Phys. Rev. A 95, 052118 (2017), 10.1103/PhysRevA.95.052118], the authors claim that our criticism, in Phys. Rev. A 94, 052125 (2016), 10.1103/PhysRevA.94.052125, to some quantum speed limit bounds for open quantum dynamics that appeared recently in literature are invalid. According to the authors, the problem with our analysis would be generated by an artifact of the finite-precision numerical calculations. We analytically show here that it is not possible to have any inconsistency associated with the numerical precision of calculations. Therefore, our criticism of the quantum speed limit bounds continues to be valid.

Antenna modeling considerations for accurate SAR calculations in human phantoms in close proximity to GSM cellular base station antennas.

Science.gov (United States)

van Wyk, Marnus J; Bingle, Marianne; Meyer, Frans J C

2005-09-01

International bodies such as International Commission on Non-Ionizing Radiation Protection (ICNIRP) and the Institute for Electrical and Electronic Engineering (IEEE) make provision for human exposure assessment based on SAR calculations (or measurements) and basic restrictions. In the case of base station exposure this is mostly applicable to occupational exposure scenarios in the very near field of these antennas where the conservative reference level criteria could be unnecessarily restrictive. This study presents a variety of critical aspects that need to be considered when calculating SAR in a human body close to a mobile phone base station antenna. A hybrid FEM/MoM technique is proposed as a suitable numerical method to obtain accurate results. The verification of the FEM/MoM implementation has been presented in a previous publication; the focus of this study is an investigation into the detail that must be included in a numerical model of the antenna, to accurately represent the real-world scenario. This is accomplished by comparing numerical results to measurements for a generic GSM base station antenna and appropriate, representative canonical and human phantoms. The results show that it is critical to take the disturbance effect of the human phantom (a large conductive body) on the base station antenna into account when the antenna-phantom spacing is less than 300 mm. For these small spacings, the antenna structure must be modeled in detail. The conclusion is that it is feasible to calculate, using the proposed techniques and methodology, accurate occupational compliance zones around base station antennas based on a SAR profile and basic restriction guidelines. (c) 2005 Wiley-Liss, Inc.

Sign Learning Kink-based (SiLK) Quantum Monte Carlo for molecular systems

Energy Technology Data Exchange (ETDEWEB)

Ma, Xiaoyao [Department of Physics and Astronomy, Louisiana State University, Baton Rouge, Louisiana 70803 (United States); Hall, Randall W. [Department of Natural Sciences and Mathematics, Dominican University of California, San Rafael, California 94901 (United States); Department of Chemistry, Louisiana State University, Baton Rouge, Louisiana 70803 (United States); Löffler, Frank [Center for Computation and Technology, Louisiana State University, Baton Rouge, Louisiana 70803 (United States); Kowalski, Karol [William R. Wiley Environmental Molecular Sciences Laboratory, Battelle, Pacific Northwest National Laboratory, Richland, Washington 99352 (United States); Bhaskaran-Nair, Kiran; Jarrell, Mark; Moreno, Juana [Department of Physics and Astronomy, Louisiana State University, Baton Rouge, Louisiana 70803 (United States); Center for Computation and Technology, Louisiana State University, Baton Rouge, Louisiana 70803 (United States)

2016-01-07

The Sign Learning Kink (SiLK) based Quantum Monte Carlo (QMC) method is used to calculate the ab initio ground state energies for multiple geometries of the H{sub 2}O, N{sub 2}, and F{sub 2} molecules. The method is based on Feynman’s path integral formulation of quantum mechanics and has two stages. The first stage is called the learning stage and reduces the well-known QMC minus sign problem by optimizing the linear combinations of Slater determinants which are used in the second stage, a conventional QMC simulation. The method is tested using different vector spaces and compared to the results of other quantum chemical methods and to exact diagonalization. Our findings demonstrate that the SiLK method is accurate and reduces or eliminates the minus sign problem.

Sign Learning Kink-based (SiLK) Quantum Monte Carlo for molecular systems

Energy Technology Data Exchange (ETDEWEB)

Ma, Xiaoyao [Department of Physics and Astronomy, Louisiana State University, Baton Rouge, Louisiana 70803, USA; Hall, Randall W. [Department of Natural Sciences and Mathematics, Dominican University of California, San Rafael, California 94901, USA; Department of Chemistry, Louisiana State University, Baton Rouge, Louisiana 70803, USA; Löffler, Frank [Center for Computation and Technology, Louisiana State University, Baton Rouge, Louisiana 70803, USA; Kowalski, Karol [William R. Wiley Environmental Molecular Sciences Laboratory, Battelle, Pacific Northwest National Laboratory, Richland, Washington 99352, USA; Bhaskaran-Nair, Kiran [Department of Physics and Astronomy, Louisiana State University, Baton Rouge, Louisiana 70803, USA; Center for Computation and Technology, Louisiana State University, Baton Rouge, Louisiana 70803, USA; Jarrell, Mark [Department of Physics and Astronomy, Louisiana State University, Baton Rouge, Louisiana 70803, USA; Center for Computation and Technology, Louisiana State University, Baton Rouge, Louisiana 70803, USA; Moreno, Juana [Department of Physics and Astronomy, Louisiana State University, Baton Rouge, Louisiana 70803, USA; Center for Computation and Technology, Louisiana State University, Baton Rouge, Louisiana 70803, USA

2016-01-07

The Sign Learning Kink (SiLK) based Quantum Monte Carlo (QMC) method is used to calculate the ab initio ground state energies for multiple geometries of the H2O, N2, and F2 molecules. The method is based on Feynman’s path integral formulation of quantum mechanics and has two stages. The first stage is called the learning stage and reduces the well-known QMC minus sign problem by optimizing the linear combinations of Slater determinants which are used in the second stage, a conventional QMC simulation. The method is tested using different vector spaces and compared to the results of other quantum chemical methods and to exact diagonalization. Our findings demonstrate that the SiLK method is accurate and reduces or eliminates the minus sign problem.

Sign Learning Kink-based (SiLK) Quantum Monte Carlo for molecular systems

International Nuclear Information System (INIS)

Ma, Xiaoyao; Hall, Randall W.; Löffler, Frank; Kowalski, Karol; Bhaskaran-Nair, Kiran; Jarrell, Mark; Moreno, Juana

2016-01-01

The Sign Learning Kink (SiLK) based Quantum Monte Carlo (QMC) method is used to calculate the ab initio ground state energies for multiple geometries of the H 2 O, N 2 , and F 2 molecules. The method is based on Feynman’s path integral formulation of quantum mechanics and has two stages. The first stage is called the learning stage and reduces the well-known QMC minus sign problem by optimizing the linear combinations of Slater determinants which are used in the second stage, a conventional QMC simulation. The method is tested using different vector spaces and compared to the results of other quantum chemical methods and to exact diagonalization. Our findings demonstrate that the SiLK method is accurate and reduces or eliminates the minus sign problem

Calculation of protein-ligand binding affinities.

Science.gov (United States)

Gilson, Michael K; Zhou, Huan-Xiang

2007-01-01

Accurate methods of computing the affinity of a small molecule with a protein are needed to speed the discovery of new medications and biological probes. This paper reviews physics-based models of binding, beginning with a summary of the changes in potential energy, solvation energy, and configurational entropy that influence affinity, and a theoretical overview to frame the discussion of specific computational approaches. Important advances are reported in modeling protein-ligand energetics, such as the incorporation of electronic polarization and the use of quantum mechanical methods. Recent calculations suggest that changes in configurational entropy strongly oppose binding and must be included if accurate affinities are to be obtained. The linear interaction energy (LIE) and molecular mechanics Poisson-Boltzmann surface area (MM-PBSA) methods are analyzed, as are free energy pathway methods, which show promise and may be ready for more extensive testing. Ultimately, major improvements in modeling accuracy will likely require advances on multiple fronts, as well as continued validation against experiment.

Relativistic quantum mechanic calculation of photoionization cross-section of hydrogenic and non-hydrogenic states using analytical potentials

International Nuclear Information System (INIS)

Rodriguez, R.; Gil, J.M.; Rubiano, J.G.; Florido, R.; Martel, P.; Minguez, E.

2005-01-01

Photoionization process is a subject of special importance in many areas of physics. Numerical methods must be used in order to obtain photoionization cross-sections for non-hydrogenic levels. The atomic data required to calculate them is huge so self-consistent calculations increase computing time considerably. Analytical potentials are a useful alternative because they avoid the iterative procedures typical in self-consistent models. In this work, we present a relativistic quantum calculation of photoionization cross-sections for isolated ions based on an analytical potential to obtain the required atomic data, which is valid both for hydrogenic and non-hydrogenic ions. Comparisons between our results and others obtained using either widely used analytical expressions for the cross-sections or more sophisticated calculations are done

Quantum mechanical calculations of vibrational population inversion in chemical reactions - Numerically exact L-squared-amplitude-density study of the H2Br reactive system

Science.gov (United States)

Zhang, Y. C.; Zhang, J. Z. H.; Kouri, D. J.; Haug, K.; Schwenke, D. W.

1988-01-01

Numerically exact, fully three-dimensional quantum mechanicl reactive scattering calculations are reported for the H2Br system. Both the exchange (H + H-prime Br to H-prime + HBr) and abstraction (H + HBR to H2 + Br) reaction channels are included in the calculations. The present results are the first completely converged three-dimensional quantum calculations for a system involving a highly exoergic reaction channel (the abstraction process). It is found that the production of vibrationally hot H2 in the abstraction reaction, and hence the extent of population inversion in the products, is a sensitive function of initial HBr rotational state and collision energy.

Digital Quantum Simulation of Spin Models with Circuit Quantum Electrodynamics

OpenAIRE

Salathé, Y.; Mondal, M.; Oppliger, M.; Heinsoo, J.; Kurpiers, P.; Potočnik, A.; Mezzacapo, Antonio; Las Heras García, Urtzi; Lamata Manuel, Lucas; Solano Villanueva, Enrique Leónidas; Filipp, S.; Wallraff, A.

2015-01-01

Systems of interacting quantum spins show a rich spectrum of quantum phases and display interesting many-body dynamics. Computing characteristics of even small systems on conventional computers poses significant challenges. A quantum simulator has the potential to outperform standard computers in calculating the evolution of complex quantum systems. Here, we perform a digital quantum simulation of the paradigmatic Heisenberg and Ising interacting spin models using a two transmon-qubit circuit...

Classical calculation of radiative lifetimes of atomic hydrogen in a homogeneous magnetic field

International Nuclear Information System (INIS)

Horbatsch, M.W.; Hessels, E.A.; Horbatsch, M.

2005-01-01

Radiative lifetimes of hydrogenic atoms in a homogeneous magnetic field of moderate strength are calculated on the basis of classical radiation. The modifications of the Keplerian orbits due to the magnetic field are incorporated by classical perturbation theory. The model is complemented by a classical radiative decay calculation using the radiated Larmor power. A recently derived highly accurate formula for the transition rate of a field-free hydrogenic state is averaged over the angular momentum oscillations caused by the magnetic field. The resulting radiative lifetimes for diamagnetic eigenstates classified by n,m and the diamagnetic energy shift C compare well with quantum results

The rigorous stochastic matrix multiplication scheme for the calculations of reduced equilibrium density matrices of open multilevel quantum systems

International Nuclear Information System (INIS)

Chen, Xin

2014-01-01

Understanding the roles of the temporary and spatial structures of quantum functional noise in open multilevel quantum molecular systems attracts a lot of theoretical interests. I want to establish a rigorous and general framework for functional quantum noises from the constructive and computational perspectives, i.e., how to generate the random trajectories to reproduce the kernel and path ordering of the influence functional with effective Monte Carlo methods for arbitrary spectral densities. This construction approach aims to unify the existing stochastic models to rigorously describe the temporary and spatial structure of Gaussian quantum noises. In this paper, I review the Euclidean imaginary time influence functional and propose the stochastic matrix multiplication scheme to calculate reduced equilibrium density matrices (REDM). In addition, I review and discuss the Feynman-Vernon influence functional according to the Gaussian quadratic integral, particularly its imaginary part which is critical to the rigorous description of the quantum detailed balance. As a result, I establish the conditions under which the influence functional can be interpreted as the average of exponential functional operator over real-valued Gaussian processes for open multilevel quantum systems. I also show the difference between the local and nonlocal phonons within this framework. With the stochastic matrix multiplication scheme, I compare the normalized REDM with the Boltzmann equilibrium distribution for open multilevel quantum systems

Accurate Determination of Tunneling-Affected Rate Coefficients: Theory Assessing Experiment.

Science.gov (United States)

Zuo, Junxiang; Xie, Changjian; Guo, Hua; Xie, Daiqian

2017-07-20

The thermal rate coefficients of a prototypical bimolecular reaction are determined on an accurate ab initio potential energy surface (PES) using ring polymer molecular dynamics (RPMD). It is shown that quantum effects such as tunneling and zero-point energy (ZPE) are of critical importance for the HCl + OH reaction at low temperatures, while the heavier deuterium substitution renders tunneling less facile in the DCl + OH reaction. The calculated RPMD rate coefficients are in excellent agreement with experimental data for the HCl + OH reaction in the entire temperature range of 200-1000 K, confirming the accuracy of the PES. On the other hand, the RPMD rate coefficients for the DCl + OH reaction agree with some, but not all, experimental values. The self-consistency of the theoretical results thus allows a quality assessment of the experimental data.

Quantum Criticality

Science.gov (United States)

Drummond, P. D.; Chaturvedi, S.; Dechoum, K.; Comey, J.

2001-02-01

We investigate the theory of quantum fluctuations in non-equilibrium systems having large crit­ical fluctuations. This allows us to treat the limits imposed by nonlinearities to quantum squeezing and noise reduction, and also to envisage future tests of quantum theory in regions of macroscopic quantum fluctuations. A long-term objective of this research is to identify suitable physical sys­tems in which macroscopic 'Schrödinger cat'-like behaviour may be observed. We investigate two systems in particular of much current experimental interest, namely the degenerate parametric oscillator near threshold, and the evaporatively cooled (BEC). We compare the results obtained in the positive-P representation, as a fully quantum mechanical calculation, with the truncated Wigner phase space equation, also known as semi-classical theory. We show when these results agree and differ in calculations taken beyond the linearized approximation. In the region where the largest quantum fluctuations and Schrödinger cat-like behaviour might be expected, we find that the quantum predictions correspond very closely to the semi-classical theory. Nature abhors observing a Schrödinger cat. -Pacs: 03.65.Bz

Achieving the Heisenberg limit in quantum metrology using quantum error correction.

Science.gov (United States)

Zhou, Sisi; Zhang, Mengzhen; Preskill, John; Jiang, Liang

2018-01-08

Quantum metrology has many important applications in science and technology, ranging from frequency spectroscopy to gravitational wave detection. Quantum mechanics imposes a fundamental limit on measurement precision, called the Heisenberg limit, which can be achieved for noiseless quantum systems, but is not achievable in general for systems subject to noise. Here we study how measurement precision can be enhanced through quantum error correction, a general method for protecting a quantum system from the damaging effects of noise. We find a necessary and sufficient condition for achieving the Heisenberg limit using quantum probes subject to Markovian noise, assuming that noiseless ancilla systems are available, and that fast, accurate quantum processing can be performed. When the sufficient condition is satisfied, a quantum error-correcting code can be constructed that suppresses the noise without obscuring the signal; the optimal code, achieving the best possible precision, can be found by solving a semidefinite program.

Development of a method to accurately calculate the Dpb and quickly predict the strength of a chemical bond

International Nuclear Information System (INIS)

Du, Xia; Zhao, Dong-Xia; Yang, Zhong-Zhi

2013-01-01

Highlights: ► A method from new respect to characterize and measure the bond strength is proposed. ► We calculate the D pb of a series of various bonds to justify our approach. ► A quite good linear relationship of the D pb with the bond lengths for series of various bonds is shown. ► Take the prediction of strengths of C–H and N–H bonds for base pairs in DNA as a practical application of our method. - Abstract: A new approach to characterize and measure bond strength has been developed. First, we propose a method to accurately calculate the potential acting on an electron in a molecule (PAEM) at the saddle point along a chemical bond in situ, denoted by D pb . Then, a direct method to quickly evaluate bond strength is established. We choose some familiar molecules as models for benchmarking this method. As a practical application, the D pb of base pairs in DNA along C–H and N–H bonds are obtained for the first time. All results show that C 7 –H of A–T and C 8 –H of G–C are the relatively weak bonds that are the injured positions in DNA damage. The significance of this work is twofold: (i) A method is developed to calculate D pb of various sizable molecules in situ quickly and accurately; (ii) This work demonstrates the feasibility to quickly predict the bond strength in macromolecules

Accurate pKa calculation of the conjugate acids of alkanolamines, alkaloids and nucleotide bases by quantum chemical methods.

Science.gov (United States)

Gangarapu, Satesh; Marcelis, Antonius T M; Zuilhof, Han

2013-04-02

The pKa of the conjugate acids of alkanolamines, neurotransmitters, alkaloid drugs and nucleotide bases are calculated with density functional methods (B3LYP, M08-HX and M11-L) and ab initio methods (SCS-MP2, G3). Implicit solvent effects are included with a conductor-like polarizable continuum model (CPCM) and universal solvation models (SMD, SM8). G3, SCS-MP2 and M11-L methods coupled with SMD and SM8 solvation models perform well for alkanolamines with mean unsigned errors below 0.20 pKa units, in all cases. Extending this method to the pKa calculation of 35 nitrogen-containing compounds spanning 12 pKa units showed an excellent correlation between experimental and computational pKa values of these 35 amines with the computationally low-cost SM8/M11-L density functional approach. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

New mixed quantum/semiclassical propagation method

International Nuclear Information System (INIS)

Antoniou, Dimitri; Gelman, David; Schwartz, Steven D.

2007-01-01

The authors developed a new method for calculating the quantum evolution of multidimensional systems, for cases in which the system can be assumed to consist of a quantum subsystem and a bath subsystem of heavier atoms. The method combines two ideas: starting from a simple frozen Gaussian description of the bath subsystem, then calculate quantum corrections to the propagation of the quantum subsystem. This follows from recent work by one of them, showing how one can calculate corrections to approximate evolution schemes, even when the Hamiltonian that corresponds to these approximate schemes is unknown. Then, they take the limit in which the width of the frozen Gaussians approaches zero, which makes the corrections to the evolution of the quantum subsystem depend only on classical bath coordinates. The test calculations they present use low-dimensional systems, in which comparison to exact quantum dynamics is feasible

Calculation of wave-functions with frozen orbitals in mixed quantum mechanics/molecular mechanics methods. II. Application of the local basis equation.

Science.gov (United States)

Ferenczy, György G

2013-04-05

The application of the local basis equation (Ferenczy and Adams, J. Chem. Phys. 2009, 130, 134108) in mixed quantum mechanics/molecular mechanics (QM/MM) and quantum mechanics/quantum mechanics (QM/QM) methods is investigated. This equation is suitable to derive local basis nonorthogonal orbitals that minimize the energy of the system and it exhibits good convergence properties in a self-consistent field solution. These features make the equation appropriate to be used in mixed QM/MM and QM/QM methods to optimize orbitals in the field of frozen localized orbitals connecting the subsystems. Calculations performed for several properties in divers systems show that the method is robust with various choices of the frozen orbitals and frontier atom properties. With appropriate basis set assignment, it gives results equivalent with those of a related approach [G. G. Ferenczy previous paper in this issue] using the Huzinaga equation. Thus, the local basis equation can be used in mixed QM/MM methods with small size quantum subsystems to calculate properties in good agreement with reference Hartree-Fock-Roothaan results. It is shown that bond charges are not necessary when the local basis equation is applied, although they are required for the self-consistent field solution of the Huzinaga equation based method. Conversely, the deformation of the wave-function near to the boundary is observed without bond charges and this has a significant effect on deprotonation energies but a less pronounced effect when the total charge of the system is conserved. The local basis equation can also be used to define a two layer quantum system with nonorthogonal localized orbitals surrounding the central delocalized quantum subsystem. Copyright © 2013 Wiley Periodicals, Inc.

A New Quantum Watermarking Based on Quantum Wavelet Transforms

International Nuclear Information System (INIS)

Heidari, Shahrokh; Pourarian, Mohammad Rasoul; Naseri, Mosayeb; Gheibi, Reza; Baghfalaki, Masoud; Farouk, Ahmed

2017-01-01

Quantum watermarking is a technique to embed specific information, usually the owner’s identification, into quantum cover data such for copyright protection purposes. In this paper, a new scheme for quantum watermarking based on quantum wavelet transforms is proposed which includes scrambling, embedding and extracting procedures. The invisibility and robustness performances of the proposed watermarking method is confirmed by simulation technique. The invisibility of the scheme is examined by the peak-signal-to-noise ratio (PSNR) and the histogram calculation. Furthermore the robustness of the scheme is analyzed by the Bit Error Rate (BER) and the Correlation Two-Dimensional (Corr 2-D) calculation. The simulation results indicate that the proposed watermarking scheme indicate not only acceptable visual quality but also a good resistance against different types of attack. (paper)

Automatic generation of active coordinates for quantum dynamics calculations: Application to the dynamics of benzene photochemistry

International Nuclear Information System (INIS)

Lasorne, Benjamin; Sicilia, Fabrizio; Bearpark, Michael J.; Robb, Michael A.; Worth, Graham A.; Blancafort, Lluis

2008-01-01

A new practical method to generate a subspace of active coordinates for quantum dynamics calculations is presented. These reduced coordinates are obtained as the normal modes of an analytical quadratic representation of the energy difference between excited and ground states within the complete active space self-consistent field method. At the Franck-Condon point, the largest negative eigenvalues of this Hessian correspond to the photoactive modes: those that reduce the energy difference and lead to the conical intersection; eigenvalues close to 0 correspond to bath modes, while modes with large positive eigenvalues are photoinactive vibrations, which increase the energy difference. The efficacy of quantum dynamics run in the subspace of the photoactive modes is illustrated with the photochemistry of benzene, where theoretical simulations are designed to assist optimal control experiments

Practical Quantum Realization of the Ampere from the Elementary Charge

Science.gov (United States)

Brun-Picard, J.; Djordjevic, S.; Leprat, D.; Schopfer, F.; Poirier, W.

2016-10-01

One major change of the future revision of the International System of Units is a new definition of the ampere based on the elementary charge e . Replacing the former definition based on Ampère's force law will allow one to fully benefit from quantum physics to realize the ampere. However, a quantum realization of the ampere from e , accurate to within 10-8 in relative value and fulfilling traceability needs, is still missing despite the many efforts made for the development of single-electron tunneling devices. Starting again with Ohm's law, applied here in a quantum circuit combining the quantum Hall resistance and Josephson voltage standards with a superconducting cryogenic amplifier, we report on a practical and universal programmable quantum current generator. We demonstrate that currents generated in the milliampere range are accurately quantized in terms of e fJ (fJ is the Josephson frequency) with measurement uncertainty of 10-8. This new quantum current source, which is able to deliver such accurate currents down to the microampere range, can greatly improve the current measurement traceability, as demonstrated with the calibrations of digital ammeters. In addition, it opens the way to further developments in metrology and in fundamental physics, such as a quantum multimeter or new accurate comparisons to single-electron pumps.

Decoherence and Entanglement Simulation in a Model of Quantum Neural Network Based on Quantum Dots

Directory of Open Access Journals (Sweden)

Altaisky Mikhail V.

2016-01-01

Full Text Available We present the results of the simulation of a quantum neural network based on quantum dots using numerical method of path integral calculation. In the proposed implementation of the quantum neural network using an array of single-electron quantum dots with dipole-dipole interaction, the coherence is shown to survive up to 0.1 nanosecond in time and up to the liquid nitrogen temperature of 77K.We study the quantum correlations between the quantum dots by means of calculation of the entanglement of formation in a pair of quantum dots on the GaAs based substrate with dot size of 100 ÷ 101 nanometer and interdot distance of 101 ÷ 102 nanometers order.

Accurate pKa Calculation of the Conjugate Acids of Alkanolamines, Alkaloids and Nucleotide Bases by Quantum Chemical Methods

NARCIS (Netherlands)

Gangarapu, S.; Marcelis, A.T.M.; Zuilhof, H.

2013-01-01

The pKa of the conjugate acids of alkanolamines, neurotransmitters, alkaloid drugs and nucleotide bases are calculated with density functional methods (B3LYP, M08-HX and M11-L) and ab initio methods (SCS-MP2, G3). Implicit solvent effects are included with a conductor-like polarizable continuum

Quantum chemical calculations in the structural analysis of phloretin

Science.gov (United States)

Gómez-Zavaglia, Andrea

2009-07-01

In this work, a conformational search on the molecule of phloretin [2',4',6'-Trihydroxy-3-(4-hydroxyphenyl)-propiophenone] has been performed. The molecule of phloretin has eight dihedral angles, four of them taking part in the carbon backbone and the other four, related with the orientation of the hydroxyl groups. A systematic search involving a random variation of the dihedral angles has been used to generate input structures for the quantum chemical calculations. Calculations at the DFT(B3LYP)/6-311++G(d,p) level of theory permitted the identification of 58 local minima belonging to the C 1 symmetry point group. The molecular structures of the conformers have been analyzed using hierarchical cluster analysis. This method allowed us to group conformers according to their similarities, and thus, to correlate the conformers' stability with structural parameters. The dendrogram obtained from the hierarchical cluster analysis depicted two main clusters. Cluster I included all the conformers with relative energies lower than 25 kJ mol -1 and cluster II, the remaining conformers. The possibility of forming intramolecular hydrogen bonds resulted the main factor contributing for the stability. Accordingly, all conformers depicting intramolecular H-bonds belong to cluster I. These conformations are clearly favored when the carbon backbone is as planar as possible. The values of the νC dbnd O and νOH vibrational modes were compared among all the conformers of phloretin. The redshifts associated with intramolecular H-bonds were correlated with the H-bonds distances and energies.

The quantum Hall effect in quantum dot systems

International Nuclear Information System (INIS)

Beltukov, Y M; Greshnov, A A

2014-01-01

It is proposed to use quantum dots in order to increase the temperatures suitable for observation of the integer quantum Hall effect. A simple estimation using Fock-Darwin spectrum of a quantum dot shows that good part of carriers localized in quantum dots generate the intervals of plateaus robust against elevated temperatures. Numerical calculations employing local trigonometric basis and highly efficient kernel polynomial method adopted for computing the Hall conductivity reveal that quantum dots may enhance peak temperature for the effect by an order of magnitude, possibly above 77 K. Requirements to potentials, quality and arrangement of the quantum dots essential for practical realization of such enhancement are indicated. Comparison of our theoretical results with the quantum Hall measurements in InAs quantum dot systems from two experimental groups is also given

Non-perturbative background field calculations

International Nuclear Information System (INIS)

Stephens, C.R.; Department of Physics, University of Utah, Salt Lake City, Utah 84112)

1988-01-01

New methods are developed for calculating one loop functional determinants in quantum field theory. Instead of relying on a calculation of all the eigenvalues of the small fluctuation equation, these techniques exploit the ability of the proper time formalism to reformulate an infinite dimensional field theoretic problem into a finite dimensional covariant quantum mechanical analog, thereby allowing powerful tools such as the method of Jacobi fields to be used advantageously in a field theory setting. More generally the methods developed herein should be extremely valuable when calculating quantum processes in non-constant background fields, offering a utilitarian alternative to the two standard methods of calculation: perturbation theory in the background field or taking the background field into account exactly. The formalism developed also allows for the approximate calculation of covariances of partial differential equations from a knowledge of the solutions of a homogeneous ordinary differential equation. copyright 1988 Academic Press, Inc

Constructing quantum dynamics from mixed quantum-classical descriptions

International Nuclear Information System (INIS)

Barsegov, V.; Rossky, P.J.

2004-01-01

The influence of quantum bath effects on the dynamics of a quantum two-level system linearly coupled to a harmonic bath is studied when the coupling is both diagonal and off-diagonal. It is shown that the pure dephasing kernel and the non-adiabatic quantum transition rate between Born-Oppenheimer states of the subsystem can be decomposed into a contribution from thermally excited bath modes plus a zero point energy contribution. This quantum rate can be modewise factorized exactly into a product of a mixed quantum subsystem-classical bath transition rate and a quantum correction factor. This factor determines dynamics of quantum bath correlations. Quantum bath corrections to both the transition rate and the pure dephasing kernel are shown to be readily evaluated via a mixed quantum-classical simulation. Hence, quantum dynamics can be recovered from a mixed quantum-classical counterpart by incorporating the missing quantum bath corrections. Within a mixed quantum-classical framework, a simple approach for evaluating quantum bath corrections in calculation of the non-adiabatic transition rate is presented

Spectroscopic and Quantum Mechanical Calculation Study of the Effect of Isotopic Substitution on NIR Spectra of Methanol.

Science.gov (United States)

Grabska, Justyna; Czarnecki, Mirosław A; Beć, Krzysztof B; Ozaki, Yukihiro

2017-10-19

In this work, we studied methanol and its deuterated derivatives (CH 3 OH, CH 3 OD, CD 3 OH, CD 3 OD) by NIR spectroscopy and anharmonic quantum chemical calculations. Vibrational bands corresponding to up to three quanta transitions (first and second overtones, binary and ternary combination modes) were predicted by the use of the VPT2 route. The accuracy of prediction of NIR modes was evaluated through density functional theory (DFT) with selected density functionals and basis sets. On the basis of the theoretical NIR spectra, detailed band assignments for all studied molecules were proposed. It was found that the pattern of bands in NIR spectra of deuterated methanols can be used for identification of isotopically equalized forms. Calculations of NIR spectra of all possible forms of CXXXOX (X = H, D) molecules demonstrated that the isotopic contamination can be identified due to a coexistence of bands specific to OH and OD groups. Also, bands from partially deuterated methyl groups can be distinguished in NIR spectra. Since the VPT2 framework is known to be sensitive to inaccuracy in the case of highly anharmonic modes, we obtained an independent insight by numerical solving of the time-independent Schrödinger equation corresponding to the O-X stretching mode scanned within -0.4 to 2.0 Å over a dense grid of 0.005 Å. This way the energies of vibrational levels of the CX1X2X3OX4 (X = H, D) isotopomers and the corresponding transition frequencies were obtained with high accuracy (<0.1 cm -1 ). The change in normal coordinate influences the reduced mass of the oscillator and thus its frequency. Our results lead to a conclusion that the effect of deuterization of the methyl group introduces a very specific and consistent frequency shift of the first overtone of the O-X stretching mode depending on the substitution of X1, X2, or X3 positions (<2 cm -1 ). However, the pattern of this shift is not reproduced accurately and is also largely overestimated by VPT2

Valley qubit in a gated MoS2 monolayer quantum dot

Science.gov (United States)

Pawłowski, J.; Żebrowski, D.; Bednarek, S.

2018-04-01

The aim of the presented research is to design a nanodevice, based on a MoS2 monolayer, performing operations on a well-defined valley qubit. We show how to confine an electron in a gate-induced quantum dot within the monolayer, and to perform the not operation on its valley degree of freedom. The operations are carried out all electrically via modulation of the confinement potential by oscillating voltages applied to the local gates. Such quantum dot structure is modeled realistically. Through these simulations we investigate the possibility of realization of a valley qubit in analogy with a realization of the spin qubit. We accurately model the potential inside the nanodevice accounting for proper boundary conditions on the gates and space-dependent materials permittivity by solving the generalized Poisson's equation. The time evolution of the system is supported by realistic self-consistent Poisson-Schrödinger tight-binding calculations. The tight-binding calculations are further confirmed by simulations within the effective continuum model.

Auxiliary-field quantum Monte Carlo calculations of molecular systems with a Gaussian basis

International Nuclear Information System (INIS)

Al-Saidi, W.A.; Zhang Shiwei; Krakauer, Henry

2006-01-01

We extend the recently introduced phaseless auxiliary-field quantum Monte Carlo (QMC) approach to any single-particle basis and apply it to molecular systems with Gaussian basis sets. QMC methods in general scale favorably with the system size as a low power. A QMC approach with auxiliary fields, in principle, allows an exact solution of the Schroedinger equation in the chosen basis. However, the well-known sign/phase problem causes the statistical noise to increase exponentially. The phaseless method controls this problem by constraining the paths in the auxiliary-field path integrals with an approximate phase condition that depends on a trial wave function. In the present calculations, the trial wave function is a single Slater determinant from a Hartree-Fock calculation. The calculated all-electron total energies show typical systematic errors of no more than a few millihartrees compared to exact results. At equilibrium geometries in the molecules we studied, this accuracy is roughly comparable to that of coupled cluster with single and double excitations and with noniterative triples [CCSD(T)]. For stretched bonds in H 2 O, our method exhibits a better overall accuracy and a more uniform behavior than CCSD(T)

Quantum close coupling calculation of transport and relaxation properties for Hg-H_2 system

International Nuclear Information System (INIS)

Nemati-Kande, Ebrahim; Maghari, Ali

2016-01-01

Highlights: • Several relaxation cross sections are calculated for Hg-H_2 van der Waals complex. • These cross sections are calculated from exact close-coupling method. • Energy-dependent SBE cross sections are calculated for ortho- and para-H_2 + Hg systems. • Viscosity and diffusion coefficients are calculated using Mason-Monchick approximation. • The results obtained by Mason-Monchick approximation are compared to the exact close-coupling results. - Abstract: Quantum mechanical close coupling calculation of the state-to-state transport and relaxation cross sections have been done for Hg-H_2 molecular system using a high-level ab initio potential energy surface. Rotationally averaged cross sections were also calculated to obtain the energy dependent Senftleben-Beenakker cross sections at the energy range of 0.005–25,000 cm"−"1. Boltzmann averaging of the energy dependent Senftleben-Beenakker cross sections showed the temperature dependency over a wide temperature range of 50–2500 K. Interaction viscosity and diffusion coefficients were also calculated using close coupling cross sections and full classical Mason-Monchick approximation. The results were compared with each other and with the available experimental data. It was found that Mason-Monchick approximation for viscosity is more reliable than diffusion coefficient. Furthermore, from the comparison of the experimental diffusion coefficients with the result of the close coupling and Mason-Monchick approximation, it was found that the Hg-H_2 potential energy surface used in this work can reliably predict diffusion coefficient data.

Quantum key distribution with finite resources: calculating the min-entropy

Energy Technology Data Exchange (ETDEWEB)

Bratzik, Sylvia; Mertz, Markus; Kampermann, Hermann; Abruzzo, Silvestre; Bruss, Dagmar [Heinrich-Heine-Universitaet, Duesseldorf (Germany)

2010-07-01

The min-entropy is an important quantity in quantum key distribution. Recently, a connection between the min- entropy and the minimal-error discrimination problem was found. We use this connection to evaluate the min-entropy for different quantum key distribution setups.

Optical forces, torques, and force densities calculated at a microscopic level using a self-consistent hydrodynamics method

Science.gov (United States)

Ding, Kun; Chan, C. T.

2018-04-01

The calculation of optical force density distribution inside a material is challenging at the nanoscale, where quantum and nonlocal effects emerge and macroscopic parameters such as permittivity become ill-defined. We demonstrate that the microscopic optical force density of nanoplasmonic systems can be defined and calculated using the microscopic fields generated using a self-consistent hydrodynamics model that includes quantum, nonlocal, and retardation effects. We demonstrate this technique by calculating the microscopic optical force density distributions and the optical binding force induced by external light on nanoplasmonic dimers. This approach works even in the limit when the nanoparticles are close enough to each other so that electron tunneling occurs, a regime in which classical electromagnetic approach fails completely. We discover that an uneven distribution of optical force density can lead to a light-induced spinning torque acting on individual particles. The hydrodynamics method offers us an accurate and efficient approach to study optomechanical behavior for plasmonic systems at the nanoscale.

Quantum Monte Carlo calculation of neutral-current ν -12C inclusive quasielastic scattering

Science.gov (United States)

Lovato, A.; Gandolfi, S.; Carlson, J.; Lusk, Ewing; Pieper, Steven C.; Schiavilla, R.

2018-02-01

Quasielastic neutrino scattering is an important aspect of the experimental program to study fundamental neutrino properties including neutrino masses, mixing angles, mass hierarchy, and charge-conjugation parity (CP)- violating phase. Proper interpretation of the experiments requires reliable theoretical calculations of neutrino-nucleus scattering. In this paper we present calculations of response functions and cross sections by neutral-current scattering of neutrinos off 12C. These calculations are based on realistic treatments of nuclear interactions and currents, the latter including the axial, vector, and vector-axial interference terms crucial for determining the difference between neutrino and antineutrino scattering and the CP-violating phase. We find that the strength and energy dependence of two-nucleon processes induced by correlation effects and interaction currents are crucial in providing the most accurate description of neutrino-nucleus scattering in the quasielastic regime.

Nuclear Magnetic Shielding Constants from Quantum Mechanical/Molecular Mechanical Calculations Using Polarizable Embedding: Role of the Embedding Potential

DEFF Research Database (Denmark)

Steinmann, Casper; Olsen, Jógvan Magnus Haugaard; Kongsted, Jacob

2014-01-01

We present NMR shielding constants obtained through quantum mechanical/molecular mechanical (QM/MM) embedding calculations. Contrary to previous reports, we show that a relatively small QM region is sufficient, provided that a high-quality embedding potential is used. The calculated averaged NMR...... shielding constants of both acrolein and acetone solvated in water are based on a number of snapshots extracted from classical molecular dynamics simulations. We focus on the carbonyl chromophore in both molecules, which shows large solvation effects, and we study the convergence of shielding constants...

Quantum and quasi-classical collisional dynamics of O2–Ar at high temperatures

International Nuclear Information System (INIS)

Ulusoy, Inga S.; Andrienko, Daniil A.; Boyd, Iain D.; Hernandez, Rigoberto

2016-01-01

A hypersonic vehicle traveling at a high speed disrupts the distribution of internal states in the ambient flow and introduces a nonequilibrium distribution in the post-shock conditions. We investigate the vibrational relaxation in diatom-atom collisions in the range of temperatures between 1000 and 10 000 K by comparing results of extensive fully quantum-mechanical and quasi-classical simulations with available experimental data. The present paper simulates the interaction of molecular oxygen with argon as the first step in developing the aerothermodynamics models based on first principles. We devise a routine to standardize such calculations also for other scattering systems. Our results demonstrate very good agreement of vibrational relaxation time, derived from quantum-mechanical calculations with the experimental measurements conducted in shock tube facilities. At the same time, the quasi-classical simulations fail to accurately predict rates of vibrationally inelastic transitions at temperatures lower than 3000 K. This observation and the computational cost of adopted methods suggest that the next generation of high fidelity thermochemical models should be a combination of quantum and quasi-classical approaches.

Accurate prediction of retention in hydrophilic interaction chromatography by back calculation of high pressure liquid chromatography gradient profiles.

Science.gov (United States)

Wang, Nu; Boswell, Paul G

2017-10-20

Gradient retention times are difficult to project from the underlying retention factor (k) vs. solvent composition (φ) relationships. A major reason for this difficulty is that gradients produced by HPLC pumps are imperfect - gradient delay, gradient dispersion, and solvent mis-proportioning are all difficult to account for in calculations. However, we recently showed that a gradient "back-calculation" methodology can measure these imperfections and take them into account. In RPLC, when the back-calculation methodology was used, error in projected gradient retention times is as low as could be expected based on repeatability in the k vs. φ relationships. HILIC, however, presents a new challenge: the selectivity of HILIC columns drift strongly over time. Retention is repeatable in short time, but selectivity frequently drifts over the course of weeks. In this study, we set out to understand if the issue of selectivity drift can be avoid by doing our experiments quickly, and if there any other factors that make it difficult to predict gradient retention times from isocratic k vs. φ relationships when gradient imperfections are taken into account with the back-calculation methodology. While in past reports, the accuracy of retention projections was >5%, the back-calculation methodology brought our error down to ∼1%. This result was 6-43 times more accurate than projections made using ideal gradients and 3-5 times more accurate than the same retention projections made using offset gradients (i.e., gradients that only took gradient delay into account). Still, the error remained higher in our HILIC projections than in RPLC. Based on the shape of the back-calculated gradients, we suspect the higher error is a result of prominent gradient distortion caused by strong, preferential water uptake from the mobile phase into the stationary phase during the gradient - a factor our model did not properly take into account. It appears that, at least with the stationary phase

Resonances in A=6 nuclei: use of supersymmetric quantum mechanics

International Nuclear Information System (INIS)

Dutta, S.K.; Das, T.K.; Khan, M.A.; Chakrabarti, B.

2004-01-01

We propose a novel theoretical technique for the calculation of resonances at low excitation energies in weakly bound systems. Starting from an effective potential, supersymmetric quantum mechanics can be successfully used to generate families of isospectral potentials having desirable and adjustable properties. For resonance states, for which there is no bound ground state of the same spin-parity, one can construct an isospectral potential with a bound state in the continuum (BIC). The potential looks quite different but is strictly isospectral with the original one. The quasi-bound state in the original shallow potential will be effectively trapped in the deep well of the isospectral family facilitating an easier and more accurate calculation of the resonance energy. Application to 6 He, 6 Be, and 6 Li systems yields quite accurate results. The beauty of our technique: We get both the bound ground state and the resonances by a single technique and using the same potential. (author)

Exciton scattering approach for optical spectra calculations in branched conjugated macromolecules

International Nuclear Information System (INIS)

Li, Hao; Wu, Chao; Malinin, Sergey V.; Tretiak, Sergei; Chernyak, Vladimir Y.

2016-01-01

The exciton scattering (ES) technique is a multiscale approach based on the concept of a particle in a box and developed for efficient calculations of excited-state electronic structure and optical spectra in low-dimensional conjugated macromolecules. Within the ES method, electronic excitations in molecular structure are attributed to standing waves representing quantum quasi-particles (excitons), which reside on the graph whose edges and nodes stand for the molecular linear segments and vertices, respectively. Exciton propagation on the linear segments is characterized by the exciton dispersion, whereas exciton scattering at the branching centers is determined by the energy-dependent scattering matrices. Using these ES energetic parameters, the excitation energies are then found by solving a set of generalized “particle in a box” problems on the graph that represents the molecule. Similarly, unique energy-dependent ES dipolar parameters permit calculations of the corresponding oscillator strengths, thus, completing optical spectra modeling. Both the energetic and dipolar parameters can be extracted from quantum-chemical computations in small molecular fragments and tabulated in the ES library for further applications. Subsequently, spectroscopic modeling for any macrostructure within a considered molecular family could be performed with negligible numerical effort. We demonstrate the ES method application to molecular families of branched conjugated phenylacetylenes and ladder poly-para-phenylenes, as well as structures with electron donor and acceptor chemical substituents. Time-dependent density functional theory (TD-DFT) is used as a reference model for electronic structure. The ES calculations accurately reproduce the optical spectra compared to the reference quantum chemistry results, and make possible to predict spectra of complex macromolecules, where conventional electronic structure calculations are unfeasible.

Exciton scattering approach for optical spectra calculations in branched conjugated macromolecules

Science.gov (United States)

Li, Hao; Wu, Chao; Malinin, Sergey V.; Tretiak, Sergei; Chernyak, Vladimir Y.

2016-12-01

The exciton scattering (ES) technique is a multiscale approach based on the concept of a particle in a box and developed for efficient calculations of excited-state electronic structure and optical spectra in low-dimensional conjugated macromolecules. Within the ES method, electronic excitations in molecular structure are attributed to standing waves representing quantum quasi-particles (excitons), which reside on the graph whose edges and nodes stand for the molecular linear segments and vertices, respectively. Exciton propagation on the linear segments is characterized by the exciton dispersion, whereas exciton scattering at the branching centers is determined by the energy-dependent scattering matrices. Using these ES energetic parameters, the excitation energies are then found by solving a set of generalized "particle in a box" problems on the graph that represents the molecule. Similarly, unique energy-dependent ES dipolar parameters permit calculations of the corresponding oscillator strengths, thus, completing optical spectra modeling. Both the energetic and dipolar parameters can be extracted from quantum-chemical computations in small molecular fragments and tabulated in the ES library for further applications. Subsequently, spectroscopic modeling for any macrostructure within a considered molecular family could be performed with negligible numerical effort. We demonstrate the ES method application to molecular families of branched conjugated phenylacetylenes and ladder poly-para-phenylenes, as well as structures with electron donor and acceptor chemical substituents. Time-dependent density functional theory (TD-DFT) is used as a reference model for electronic structure. The ES calculations accurately reproduce the optical spectra compared to the reference quantum chemistry results, and make possible to predict spectra of complex macromolecules, where conventional electronic structure calculations are unfeasible.

Exciton scattering approach for optical spectra calculations in branched conjugated macromolecules

Energy Technology Data Exchange (ETDEWEB)

Li, Hao [Department of Chemistry, University of Houston, Houston, TX 77204 (United States); Wu, Chao [Electronic Structure Lab, Center of Microscopic Theory and Simulation, Frontier Institute of Science and Technology, Xian Jiaotong University, Xian 710054 (China); Malinin, Sergey V. [Department of Chemistry, Wayne State University, 5101 Cass Avenue, Detroit, MI 48202 (United States); Tretiak, Sergei, E-mail: serg@lanl.gov [Theoretical Division and Center for Nonlinear Studies, Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Center for Integrated Nanotechnologies, Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Chernyak, Vladimir Y., E-mail: chernyak@chem.wayne.edu [Department of Chemistry, Wayne State University, 5101 Cass Avenue, Detroit, MI 48202 (United States)

2016-12-20

The exciton scattering (ES) technique is a multiscale approach based on the concept of a particle in a box and developed for efficient calculations of excited-state electronic structure and optical spectra in low-dimensional conjugated macromolecules. Within the ES method, electronic excitations in molecular structure are attributed to standing waves representing quantum quasi-particles (excitons), which reside on the graph whose edges and nodes stand for the molecular linear segments and vertices, respectively. Exciton propagation on the linear segments is characterized by the exciton dispersion, whereas exciton scattering at the branching centers is determined by the energy-dependent scattering matrices. Using these ES energetic parameters, the excitation energies are then found by solving a set of generalized “particle in a box” problems on the graph that represents the molecule. Similarly, unique energy-dependent ES dipolar parameters permit calculations of the corresponding oscillator strengths, thus, completing optical spectra modeling. Both the energetic and dipolar parameters can be extracted from quantum-chemical computations in small molecular fragments and tabulated in the ES library for further applications. Subsequently, spectroscopic modeling for any macrostructure within a considered molecular family could be performed with negligible numerical effort. We demonstrate the ES method application to molecular families of branched conjugated phenylacetylenes and ladder poly-para-phenylenes, as well as structures with electron donor and acceptor chemical substituents. Time-dependent density functional theory (TD-DFT) is used as a reference model for electronic structure. The ES calculations accurately reproduce the optical spectra compared to the reference quantum chemistry results, and make possible to predict spectra of complex macromolecules, where conventional electronic structure calculations are unfeasible.

Accurate treatment of material interface dynamics in the calculation of one-dimensional two-phase flows by the integral method of characteristics

International Nuclear Information System (INIS)

Shin, Y.W.; Wiedermann, A.H.

1984-01-01

Accurate numerical methods for treating the junction and boundary conditions needed in the transient two-phase flows of a piping network were published earlier by us; the same methods are used to formulate the treatment of the material interface as a moving boundary. The method formulated is used in a computer program to calculate sample problems designed to test the numerical methods as to their ability and the accuracy limits for calculation of the transient two-phase flows in the piping network downstream of a PWR pressurizer. Independent exact analytical solutions for the sample problems are used as the basis of a critical evaluation of the proposed numerical methods. The evaluation revealed that the proposed boundary scheme indeed generates very accurate numerical results. However, in some extreme flow conditions, numerical difficulties were experienced that eventually led to numerical instability. This paper discusses further a special technique to overcome the difficulty

Quantum features of semiconductor quantum dots

International Nuclear Information System (INIS)

Lozada-Cassou, M.; Dong Shihai; Yu Jiang

2004-01-01

The exact solutions of the two-dimensional Schrodinger equation with the position-dependent mass for the square well potential in the semiconductor quantum dots system are obtained. The eigenvalues, which are closely related to the position-dependent masses μ1 and μ2, the potential well depth V0 and the radius of the quantum dots r0, can be calculated from two boundary conditions. We generalize this quantum system to three-dimensional case. The special cases for the angular momentum quantum number l=0, 1, 2 are studied in some detail. We find that the energy levels are proportional to the parameters μ2, V0 and r0 for l=0. The relations between them for l=1, 2 become very complicated. The scattering states of this quantum system are mentioned briefly

Molecular Structure of Phenytoin: NMR, UV-Vis and Quantum Chemical Calculations

Directory of Open Access Journals (Sweden)

Raluca Luchian

2015-12-01

Full Text Available Due to the presence of the carbonyl and imide groups in the structure of 5,5-diphenylhydantoin (DPH, the possibility for this compound to be involved in hydrogen bonding intermolecular interactions is obvious. Even though such interactions are presumably responsible for the mechanism of action of this drug, however, to the best of our knowledge, the self-hydrogen bonding interactions between the DPH monomers have not been addressed till now. Furthermore, studies reporting on the spectroscopic characteristics of this molecule are scarcely reported in the literature. Here we report on the possible dimers of DPH, investigated by quantum chemical calculations at B3LYP/6-31+G(2d,2p level of theory. Twelve unique DPH dimers were structurally optimized in gas-phase, as well as in ethanol and DMSO and then were used to compute the population-averaged UV-Vis and NMR spectra using Boltzmann statistics. UV-Vis and NMR techniques were employed to assess experimentally the spectroscopical response of this compound. DFT calculations are also used to investigate the structural transformations between the solid and liquid phase, as well as for describing the electronic transitions and for the assignment of NMR spectra of DPH.

Practical Quantum Realization of the Ampere from the Elementary Charge

Directory of Open Access Journals (Sweden)

J. Brun-Picard

2016-12-01

Full Text Available One major change of the future revision of the International System of Units is a new definition of the ampere based on the elementary charge e. Replacing the former definition based on Ampère’s force law will allow one to fully benefit from quantum physics to realize the ampere. However, a quantum realization of the ampere from e, accurate to within 10^{-8} in relative value and fulfilling traceability needs, is still missing despite the many efforts made for the development of single-electron tunneling devices. Starting again with Ohm’s law, applied here in a quantum circuit combining the quantum Hall resistance and Josephson voltage standards with a superconducting cryogenic amplifier, we report on a practical and universal programmable quantum current generator. We demonstrate that currents generated in the milliampere range are accurately quantized in terms of ef_{J} (f_{J} is the Josephson frequency with measurement uncertainty of 10^{-8}. This new quantum current source, which is able to deliver such accurate currents down to the microampere range, can greatly improve the current measurement traceability, as demonstrated with the calibrations of digital ammeters. In addition, it opens the way to further developments in metrology and in fundamental physics, such as a quantum multimeter or new accurate comparisons to single-electron pumps.

Systematic study of imidazoles inhibiting IDO1 via the integration of molecular mechanics and quantum mechanics calculations.

Science.gov (United States)

Zou, Yi; Wang, Fang; Wang, Yan; Guo, Wenjie; Zhang, Yihua; Xu, Qiang; Lai, Yisheng

2017-05-05

Indoleamine 2,3-dioxygenase 1 (IDO1) is regarded as an attractive target for cancer immunotherapy. To rationalize the detailed interactions between IDO1 and its inhibitors at the atomic level, an integrated computational approach by combining molecular mechanics and quantum mechanics methods was employed in this report. Specifically, the binding modes of 20 inhibitors was initially investigated using the induced fit docking (IFD) protocol, which outperformed other two docking protocols in terms of correctly predicting ligand conformations. Secondly, molecular dynamics (MD) simulations and MM/PBSA free energy calculations were employed to determine the dynamic binding process and crucial residues were confirmed through close contact analysis, hydrogen-bond analysis and binding free energy decomposition calculations. Subsequent quantum mechanics and nonbonding interaction analysis were carried out to provide in-depth explanations on the critical role of those key residues, and Arg231 and 7-propionate of the heme group were major contributors to ligand binding, which lowed a great amount of interaction energy. We anticipate that these findings will be valuable for enzymatic studies and rational drug design. Copyright © 2017. Published by Elsevier Masson SAS.

Quantum Simulations for Dense Matter

International Nuclear Information System (INIS)

Ceperley, David M.

2010-01-01

High pressure systems are important, for example, to understand the interiors of giant planets (Jupiter and Saturn), for experiments at NIF (the National Ignition Facility at Livermore) related to inertially confined fusion and for other interests of DOE. In this project, we are developing innovative simulation methods (Quantum Monte Carlo methods) to allow more accurate calculation of properties of systems under extreme conditions of pressure and temperature. These methods can use the power of current day supercomputers made of very many processors, starting from the basic equations of physics to model quantum phenomena important at the microscopic scale. During the grant period, we have settled two important questions of the physics of hydrogen and helium under extreme conditions. We have found the pressures and temperatures when hydrogen and helium mix together; this is important to understand the difference of the interiors of the planets Jupiter and Saturn. Secondly, we have shown that there exists a sharp transition as a function of pressure between molecular and atomic liquid hydrogen at temperatures below 2000K. This prediction can be confirmed with high pressure experiments.

Reference quantum chemical calculations on RNA base pairs directly involving the 2'-OH group of ribose

Czech Academy of Sciences Publication Activity Database

Šponer, Jiří; Zgarbová, M.; Jurečka, Petr; Riley, K.E.; Šponer, Judit E.; Hobza, Pavel

2009-01-01

Roč. 5, č. 4 (2009), s. 1166-1179 ISSN 1549-9618 R&D Projects: GA AV ČR(CZ) IAA400040802; GA AV ČR(CZ) IAA400550701; GA MŠk(CZ) LC06030; GA MŠk(CZ) LC512 Institutional research plan: CEZ:AV0Z50040507; CEZ:AV0Z50040702; CEZ:AV0Z40550506 Keywords : RNA * ribose * quantum calculations Subject RIV: BO - Biophysics Impact factor: 4.804, year: 2009

Accurate quantum calculations of translation-rotation eigenstates in electric-dipole-coupled H2O@C60 assemblies

Science.gov (United States)

Felker, Peter M.; Bačić, Zlatko

2017-09-01

We present methodology for variational calculation of the 6 n -dimensional translation-rotation (TR) eigenstates of assemblies of n H2O@C60 moieties coupled by dipole-dipole interactions. We show that the TR Hamiltonian matrix for any n can be constructed from dipole-dipole matrix elements computed for n = 2 . We present results for linear H2O@C60 assemblies. Two classes of eigenstates are revealed. One class comprises excitations of the 111 rotational level of H2O. The lowest-energy 111 -derived eigenstate for each assembly exhibits significant dipole ordering and shifts down in energy with the assembly size.

In Vivo Anti-Leukemia, Quantum Chemical Calculations and ADMET Investigations of Some Quaternary and Isothiouronium Surfactants

Directory of Open Access Journals (Sweden)

Ahmed A. El-Henawy

2013-04-01

Full Text Available Anti-leukemia screening of previously prepared isothiouronium and quaternary salts was performed, and some salts exhibited promising activity as anticancer agents. Quantum chemical calculations were utilized to explore the electronic structure and stability of these compounds. Computational studies have been carried out at the PM3 semiempirical molecular orbitals level, to establish the HOMO-LUMO, IP and ESP mapping of these compounds. The ADMET properties were also studied to gain a clear view of the potential oral bioavailability of these compounds. The surface properties calculated included critical micelle concentration (CMC, maximum surface excess (Γmax, minimum surface area (Amin, free energy of micellization (ΔGomic and adsorption (ΔGoads.

Learn Quantum Mechanics with Haskell

Directory of Open Access Journals (Sweden)

Scott N. Walck

2016-11-01

Full Text Available To learn quantum mechanics, one must become adept in the use of various mathematical structures that make up the theory; one must also become familiar with some basic laboratory experiments that the theory is designed to explain. The laboratory ideas are naturally expressed in one language, and the theoretical ideas in another. We present a method for learning quantum mechanics that begins with a laboratory language for the description and simulation of simple but essential laboratory experiments, so that students can gain some intuition about the phenomena that a theory of quantum mechanics needs to explain. Then, in parallel with the introduction of the mathematical framework on which quantum mechanics is based, we introduce a calculational language for describing important mathematical objects and operations, allowing students to do calculations in quantum mechanics, including calculations that cannot be done by hand. Finally, we ask students to use the calculational language to implement a simplified version of the laboratory language, bringing together the theoretical and laboratory ideas.

A perspective on quantum mechanics calculations in ADMET predictions.

Science.gov (United States)

Bowen, J Phillip; Güner, Osman F

2013-01-01

Understanding the molecular basis of drug action has been an important objective for pharmaceutical scientists. With the increasing speed of computers and the implementation of quantum chemistry methodologies, pharmacodynamic and pharmacokinetic problems have become more computationally tractable. Historically the former has been the focus of drug design, but within the last two decades efforts to understand the latter have increased. It takes about fifteen years and over $1 billion dollars for a drug to go from laboratory hit, through lead optimization, to final approval by the U.S. Food and Drug Administration. While the costs have increased substantially, the overall clinical success rate for a compound to emerge from clinical trials is approximately 10%. Most of the attrition rate can be traced to ADMET (absorption, distribution, metabolism, excretion, and toxicity) problems, which is a powerful impetus to study these issues at an earlier stage in drug discovery. Quantum mechanics offers pharmaceutical scientists the opportunity to investigate pharmacokinetic problems at the molecular level prior to laboratory preparation and testing. This review will provide a perspective on the use of quantum mechanics or a combination of quantum mechanics coupled with other classical methods in the pharmacokinetic phase of drug discovery. A brief overview of the essential features of theory will be discussed, and a few carefully selected examples will be given to highlight the computational methods.

Quantum Theory of Conducting Matter Superconductivity and Quantum Hall Effect

CERN Document Server

Fujita, Shigeji; Godoy, Salvador

2009-01-01

Explains major superconducting properties including zero resistance, Meissner effect, sharp phase change, flux quantization, excitation energy gap, and Josephson effects using quantum statistical mechanical calculations. This book covers the 2D superconductivity and the quantum Hall effects

Efficient calculation of open quantum system dynamics and time-resolved spectroscopy with distributed memory HEOM (DM-HEOM).

Science.gov (United States)

Kramer, Tobias; Noack, Matthias; Reinefeld, Alexander; Rodríguez, Mirta; Zelinskyy, Yaroslav

2018-06-11

Time- and frequency-resolved optical signals provide insights into the properties of light-harvesting molecular complexes, including excitation energies, dipole strengths and orientations, as well as in the exciton energy flow through the complex. The hierarchical equations of motion (HEOM) provide a unifying theory, which allows one to study the combined effects of system-environment dissipation and non-Markovian memory without making restrictive assumptions about weak or strong couplings or separability of vibrational and electronic degrees of freedom. With increasing system size the exact solution of the open quantum system dynamics requires memory and compute resources beyond a single compute node. To overcome this barrier, we developed a scalable variant of HEOM. Our distributed memory HEOM, DM-HEOM, is a universal tool for open quantum system dynamics. It is used to accurately compute all experimentally accessible time- and frequency-resolved processes in light-harvesting molecular complexes with arbitrary system-environment couplings for a wide range of temperatures and complex sizes. © 2018 Wiley Periodicals, Inc. © 2018 Wiley Periodicals, Inc.

Non-perturbative background field calculations

Science.gov (United States)

Stephens, C. R.

1988-01-01

New methods are developed for calculating one loop functional determinants in quantum field theory. Instead of relying on a calculation of all the eigenvalues of the small fluctuation equation, these techniques exploit the ability of the proper time formalism to reformulate an infinite dimensional field theoretic problem into a finite dimensional covariant quantum mechanical analog, thereby allowing powerful tools such as the method of Jacobi fields to be used advantageously in a field theory setting. More generally the methods developed herein should be extremely valuable when calculating quantum processes in non-constant background fields, offering a utilitarian alternative to the two standard methods of calculation—perturbation theory in the background field or taking the background field into account exactly. The formalism developed also allows for the approximate calculation of covariances of partial differential equations from a knowledge of the solutions of a homogeneous ordinary differential equation.

Calculation of the tunneling time using the extended probability of the quantum histories approach

International Nuclear Information System (INIS)

Rewrujirek, Jiravatt; Hutem, Artit; Boonchui, Sutee

2014-01-01

The dwell time of quantum tunneling has been derived by Steinberg (1995) [7] as a function of the relation between transmission and reflection times τ t and τ r , weighted by the transmissivity and the reflectivity. In this paper, we reexamine the dwell time using the extended probability approach. The dwell time is calculated as the weighted average of three mutually exclusive events. We consider also the scattering process due to a resonance potential in the long-time limit. The results show that the dwell time can be expressed as the weighted sum of transmission, reflection and internal probabilities.

Quantum mechanical study of solvent effects in a prototype SN2 reaction in solution: Cl- attack on CH3Cl.

Science.gov (United States)

Kuechler, Erich R; York, Darrin M

2014-02-07

The nucleophilic attack of a chloride ion on methyl chloride is an important prototype SN2 reaction in organic chemistry that is known to be sensitive to the effects of the surrounding solvent. Herein, we develop a highly accurate Specific Reaction Parameter (SRP) model based on the Austin Model 1 Hamiltonian for chlorine to study the effects of solvation into an aqueous environment on the reaction mechanism. To accomplish this task, we apply high-level quantum mechanical calculations to study the reaction in the gas phase and combined quantum mechanical/molecular mechanical simulations with TIP3P and TIP4P-ew water models and the resulting free energy profiles are compared with those determined from simulations using other fast semi-empirical quantum models. Both gas phase and solution results with the SRP model agree very well with experiment and provide insight into the specific role of solvent on the reaction coordinate. Overall, the newly parameterized SRP Hamiltonian is able to reproduce both the gas phase and solution phase barriers, suggesting it is an accurate and robust model for simulations in the aqueous phase at greatly reduced computational cost relative to comparably accurate ab initio and density functional models.

Accurate Determination of the Values of Fundamental Physical Constants: The Basis of the New "Quantum" SI Units

Science.gov (United States)

Karshenboim, S. G.

2018-03-01

The metric system appeared as the system of units designed for macroscopic (laboratory scale) measurements. The progress in accurate determination of the values of quantum constants (such as the Planck constant) in SI units shows that the capabilities in high-precision measurement of microscopic and macroscopic quantities in terms of the same units have increased substantially recently. At the same time, relative microscopic measurements (for example, the comparison of atomic transition frequencies or atomic masses) are often much more accurate than relative measurements of macroscopic quantities. This is the basis for the strategy to define units in microscopic phenomena and then use them on the laboratory scale, which plays a crucial role in practical methodological applications determined by everyday life and technologies. The international CODATA task group on fundamental constants regularly performs an overall analysis of the precision world data (the so-called Adjustment of the Fundamental Constants) and publishes their recommended values. The most recent evaluation was based on the data published by the end of 2014; here, we review the corresponding data and results. The accuracy in determination of the Boltzmann constant has increased, the consistency of the data on determination of the Planck constant has improved; it is these two dimensional constants that will be used in near future as the basis for the new definition of the kelvin and kilogram, respectively. The contradictions in determination of the Rydberg constant and the proton charge radius remain. The accuracy of determination of the fine structure constant and relative atomic weight of the electron has improved. Overall, we give a detailed review of the state of the art in precision determination of the values of fundamental constants. The mathematical procedure of the Adjustment, the new data and results are considered in detail. The limitations due to macroscopic properties of material

Quantum and quasi-classical collisional dynamics of O{sub 2}–Ar at high temperatures

Energy Technology Data Exchange (ETDEWEB)

Ulusoy, Inga S. [IHP, Im Technologiepark 25, 15236 Frankfurt (Oder) (Germany); Center for Computational and Molecular Science and Technology, School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332-0400 (United States); Andrienko, Daniil A.; Boyd, Iain D. [Nonequilibrium Gas and Plasma Dynamics Laboratory, Department of Aerospace Engineering, University of Michigan, Ann Arbor, Michigan 48109-2140 (United States); Hernandez, Rigoberto, E-mail: hernandez@gatech.edu [Center for Computational and Molecular Science and Technology, School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332-0400 (United States)

2016-06-21

A hypersonic vehicle traveling at a high speed disrupts the distribution of internal states in the ambient flow and introduces a nonequilibrium distribution in the post-shock conditions. We investigate the vibrational relaxation in diatom-atom collisions in the range of temperatures between 1000 and 10 000 K by comparing results of extensive fully quantum-mechanical and quasi-classical simulations with available experimental data. The present paper simulates the interaction of molecular oxygen with argon as the first step in developing the aerothermodynamics models based on first principles. We devise a routine to standardize such calculations also for other scattering systems. Our results demonstrate very good agreement of vibrational relaxation time, derived from quantum-mechanical calculations with the experimental measurements conducted in shock tube facilities. At the same time, the quasi-classical simulations fail to accurately predict rates of vibrationally inelastic transitions at temperatures lower than 3000 K. This observation and the computational cost of adopted methods suggest that the next generation of high fidelity thermochemical models should be a combination of quantum and quasi-classical approaches.

Classical Electrodynamics Coupled to Quantum Mechanics for Calculation of Molecular Optical Properties: a RT-TDDFT/FDTD Approach

Energy Technology Data Exchange (ETDEWEB)

Chen, Hanning; McMahon, J. M.; Ratner, Mark A.; Schatz, George C.

2010-09-02

A new multiscale computational methodology was developed to effectively incorporate the scattered electric field of a plasmonic nanoparticle into a quantum mechanical (QM) optical property calculation for a nearby dye molecule. For a given location of the dye molecule with respect to the nanoparticle, a frequency-dependent scattering response function was first determined by the classical electrodynamics (ED) finite-difference time-domain (FDTD) approach. Subsequently, the time-dependent scattered electric field at the dye molecule was calculated using the FDTD scattering response function through a multidimensional Fourier transform to reflect the effect of polarization of the nanoparticle on the local field at the molecule. Finally, a real-time time-dependent density function theory (RT-TDDFT) approach was employed to obtain a desired optical property (such as absorption cross section) of the dye molecule in the presence of the nanoparticle’s scattered electric field. Our hybrid QM/ED methodology was demonstrated by investigating the absorption spectrum of the N3 dye molecule and the Raman spectrum of pyridine, both of which were shown to be significantly enhanced by a 20 nm diameter silver sphere. In contrast to traditional quantum mechanical optical calculations in which the field at the molecule is entirely determined by intensity and polarization direction of the incident light, in this work we show that the light propagation direction as well as polarization and intensity are important to nanoparticle-bound dye molecule response. At no additional computation cost compared to conventional ED and QM calculations, this method provides a reliable way to couple the response of the dye molecule’s individual electrons to the collective dielectric response of the nanoparticle.

Unbiased reduced density matrices and electronic properties from full configuration interaction quantum Monte Carlo

International Nuclear Information System (INIS)

Overy, Catherine; Blunt, N. S.; Shepherd, James J.; Booth, George H.; Cleland, Deidre; Alavi, Ali

2014-01-01

Properties that are necessarily formulated within pure (symmetric) expectation values are difficult to calculate for projector quantum Monte Carlo approaches, but are critical in order to compute many of the important observable properties of electronic systems. Here, we investigate an approach for the sampling of unbiased reduced density matrices within the full configuration interaction quantum Monte Carlo dynamic, which requires only small computational overheads. This is achieved via an independent replica population of walkers in the dynamic, sampled alongside the original population. The resulting reduced density matrices are free from systematic error (beyond those present via constraints on the dynamic itself) and can be used to compute a variety of expectation values and properties, with rapid convergence to an exact limit. A quasi-variational energy estimate derived from these density matrices is proposed as an accurate alternative to the projected estimator for multiconfigurational wavefunctions, while its variational property could potentially lend itself to accurate extrapolation approaches in larger systems

Quantum control in infinite dimensions

International Nuclear Information System (INIS)

Karwowski, Witold; Vilela Mendes, R.

2004-01-01

Accurate control of quantum evolution is an essential requirement for quantum state engineering, laser chemistry, quantum information and quantum computing. Conditions of controllability for systems with a finite number of energy levels have been extensively studied. By contrast, results for controllability in infinite dimensions have been mostly negative, stating that full control cannot be achieved with a finite-dimensional control Lie algebra. Here we show that by adding a discrete operation to a Lie algebra it is possible to obtain full control in infinite dimensions with a small number of control operators

Multicomponent Density Functional Theory: Impact of Nuclear Quantum Effects on Proton Affinities and Geometries.

Science.gov (United States)

Brorsen, Kurt R; Yang, Yang; Hammes-Schiffer, Sharon

2017-08-03

Nuclear quantum effects such as zero point energy play a critical role in computational chemistry and often are included as energetic corrections following geometry optimizations. The nuclear-electronic orbital (NEO) multicomponent density functional theory (DFT) method treats select nuclei, typically protons, quantum mechanically on the same level as the electrons. Electron-proton correlation is highly significant, and inadequate treatments lead to highly overlocalized nuclear densities. A recently developed electron-proton correlation functional, epc17, has been shown to provide accurate nuclear densities for molecular systems. Herein, the NEO-DFT/epc17 method is used to compute the proton affinities for a set of molecules and to examine the role of nuclear quantum effects on the equilibrium geometry of FHF - . The agreement of the computed results with experimental and benchmark values demonstrates the promise of this approach for including nuclear quantum effects in calculations of proton affinities, pK a 's, optimized geometries, and reaction paths.

Calculations on nonlinear optical properties for large systems the elongation method

CERN Document Server

Gu, Feng Long; Springborg, Michael; Kirtman, Bernard

2014-01-01

For design purposes one needs to relate the structure of proposed materials to their NLO (nonlinear optical) and other properties, which is a situation where theoretical approaches can be very helpful in providing suggestions for candidate systems that subsequently can be synthesized and studied experimentally. This brief describes the quantum-mechanical treatment of the response to one or more external oscillating electric fields for molecular and macroscopic, crystalline systems. To calculate NLO properties of large systems, a linear scaling generalized elongation method for the efficient and accurate calculation is introduced. The reader should be aware that this treatment is particularly feasible for complicated three-dimensional and/or delocalized systems that are intractable when applied to conventional or other linear scaling methods.

Cheap but accurate calculation of chemical reaction rate constants from ab initio data, via system-specific, black-box force fields.

Science.gov (United States)

Steffen, Julien; Hartke, Bernd

2017-10-28

Building on the recently published quantum-mechanically derived force field (QMDFF) and its empirical valence bond extension, EVB-QMDFF, it is now possible to generate a reliable potential energy surface for any given elementary reaction step in an essentially black box manner. This requires a limited and pre-defined set of reference data near the reaction path and generates an accurate approximation of the reference potential energy surface, on and off the reaction path. This intermediate representation can be used to generate reaction rate data, with far better accuracy and reliability than with traditional approaches based on transition state theory (TST) or variational extensions thereof (VTST), even if those include sophisticated tunneling corrections. However, the additional expense at the reference level remains very modest. We demonstrate all this for three arbitrarily chosen example reactions.

Accurate calculation of conformational free energy differences in explicit water: the confinement-solvation free energy approach.

Science.gov (United States)

Esque, Jeremy; Cecchini, Marco

2015-04-23

The calculation of the free energy of conformation is key to understanding the function of biomolecules and has attracted significant interest in recent years. Here, we present an improvement of the confinement method that was designed for use in the context of explicit solvent MD simulations. The development involves an additional step in which the solvation free energy of the harmonically restrained conformers is accurately determined by multistage free energy perturbation simulations. As a test-case application, the newly introduced confinement/solvation free energy (CSF) approach was used to compute differences in free energy between conformers of the alanine dipeptide in explicit water. The results are in excellent agreement with reference calculations based on both converged molecular dynamics and umbrella sampling. To illustrate the general applicability of the method, conformational equilibria of met-enkephalin (5 aa) and deca-alanine (10 aa) in solution were also analyzed. In both cases, smoothly converged free-energy results were obtained in agreement with equilibrium sampling or literature calculations. These results demonstrate that the CSF method may provide conformational free-energy differences of biomolecules with small statistical errors (below 0.5 kcal/mol) and at a moderate computational cost even with a full representation of the solvent.

Quantum symmetry in quantum theory

International Nuclear Information System (INIS)

Schomerus, V.

1993-02-01

Symmetry concepts have always been of great importance for physical problems like explicit calculations, classification or model building. More recently, new 'quantum symmetries' ((quasi) quantum groups) attracted much interest in quantum theory. It is shown that all these quantum symmetries permit a conventional formulation as symmetry in quantum mechanics. Symmetry transformations can act on the Hilbert space H of physical states such that the ground state is invariant and field operators transform covariantly. Models show that one must allow for 'truncation' in the tensor product of representations of a quantum symmetry. This means that the dimension of the tensor product of two representations of dimension σ 1 and σ 2 may be strictly smaller than σ 1 σ 2 . Consistency of the transformation law of field operators local braid relations leads us to expect, that (weak) quasi quantum groups are the most general symmetries in local quantum theory. The elements of the R-matrix which appears in these local braid relations turn out to be operators on H in general. It will be explained in detail how examples of field algebras with weak quasi quantum group symmetry can be obtained. Given a set of observable field with a finite number of superselection sectors, a quantum symmetry together with a complete set of covariant field operators which obey local braid relations are constructed. A covariant transformation law for adjoint fields is not automatic but will follow when the existence of an appropriate antipode is assumed. At the example of the chiral critical Ising model, non-uniqueness of the quantum symmetry will be demonstrated. Generalized quantum symmetries yield examples of gauge symmetries in non-commutative geometry. Quasi-quantum planes are introduced as the simplest examples of quasi-associative differential geometry. (Weak) quasi quantum groups can act on them by generalized derivations much as quantum groups do in non-commutative (differential-) geometry

Calculation of electrical transport properties and electron entanglement in inhomogeneous quantum wires

Directory of Open Access Journals (Sweden)

A A Shokri

2013-10-01

Full Text Available In this paper, we have investigated the spin-dependent transport properties and electron entanglement in a mesoscopic system, which consists of two semi-infinite leads (as source and drain separated by a typical quantum wire with a given potential. The properties studied include current-voltage characteristic, electrical conductivity, Fano factor and shot noise, and concurrence. The calculations are based on the transfer matrix method within the effective mass approximation. Using the Landauer formalism and transmission coefficient, the dependence of the considered quantities on type of potential well, length and width of potential well, energy of transmitted electron, temperature and the voltage have been theoretically studied. Also, the effect of the above-mentioned factors has been investigated in the nanostructure. The application of the present results may be useful in designing spintronice devices.

Quantum Dot Systems: a versatile platform for quantum simulations

International Nuclear Information System (INIS)

Barthelemy, Pierre; Vandersypen, Lieven M.K.

2013-01-01

Quantum mechanics often results in extremely complex phenomena, especially when the quantum system under consideration is composed of many interacting particles. The states of these many-body systems live in a space so large that classical numerical calculations cannot compute them. Quantum simulations can be used to overcome this problem: complex quantum problems can be solved by studying experimentally an artificial quantum system operated to simulate the desired hamiltonian. Quantum dot systems have shown to be widely tunable quantum systems, that can be efficiently controlled electrically. This tunability and the versatility of their design makes them very promising quantum simulators. This paper reviews the progress towards digital quantum simulations with individually controlled quantum dots, as well as the analog quantum simulations that have been performed with these systems. The possibility to use large arrays of quantum dots to simulate the low-temperature Hubbard model is also discussed. The main issues along that path are presented and new ideas to overcome them are proposed. (copyright 2013 by WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

Axion-photon conversion caused by dielectric interfaces: quantum field calculation

Energy Technology Data Exchange (ETDEWEB)

Ioannisian, Ara N. [Yerevan Physics Institute, Alikhanian Br. 2, 375036 Yerevan (Armenia); Kazarian, Narine [Institute for Theoretical Physics and Modeling, 375036 Yerevan (Armenia); Millar, Alexander J.; Raffelt, Georg G., E-mail: ara.ioannisyan@cern.ch, E-mail: narinkaz@gmail.com, E-mail: millar@mpp.mpg.de, E-mail: raffelt@mpp.mpg.de [Max-Planck-Institut für Physik (Werner-Heisenberg-Institut), Föhringer Ring 6, 80805 München (Germany)

2017-09-01

Axion-photon conversion at dielectric interfaces, immersed in a near-homogeneous magnetic field, is the basis for the dielectric haloscope method to search for axion dark matter. In analogy to transition radiation, this process is possible because the photon wave function is modified by the dielectric layers ('Garibian wave function') and is no longer an eigenstate of momentum. A conventional first-order perturbative calculation of the transition probability between a quantized axion state and these distorted photon states provides the microwave production rate. It agrees with previous results based on solving the classical Maxwell equations for the combined system of axions and electromagnetic fields. We argue that in general the average photon production rate is given by our result, independently of the detailed quantum state of the axion field. Moreover, our result provides a new perspective on axion-photon conversion in dielectric haloscopes because the rate is based on an overlap integral between unperturbed axion and photon wave functions, in analogy to the usual treatment of microwave-cavity haloscopes.

Modeling Alkyl p-Methoxy Cinnamate (APMC) as UV absorber based on electronic transition using semiempirical quantum mechanics ZINDO/s calculation

Science.gov (United States)

Salmahaminati; Azis, Muhlas Abdul; Purwiandono, Gani; Arsyik Kurniawan, Muhammad; Rubiyanto, Dwiarso; Darmawan, Arif

2017-11-01

In this research, modeling several alkyl p-methoxy cinnamate (APMC) based on electronic transition by using semiempirical mechanical quantum ZINDO/s calculation is performed. Alkyl cinnamates of C1 (methyl) up to C7 (heptyl) homolog with 1-5 example structures of each homolog are used as materials. Quantum chemistry-package software Hyperchem 8.0 is used to simulate the drawing of the structure, geometry optimization by a semiempirical Austin Model 1 algorithm and single point calculation employing a semiempirical ZINDO/s technique. ZINDO/s calculations use a defined criteria that singly excited -Configuration Interaction (CI) where a gap of HOMO-LUMO energy transition and maximum degeneracy level are 7 and 2, respectively. Moreover, analysis of the theoretical spectra is focused on the UV-B (290-320 nm) and UV-C (200-290 nm) area. The results show that modeling of the compound can be used to predict the type of UV protection activity depends on the electronic transition in the UV area. Modification of the alkyl homolog relatively does not change the value of wavelength absorption to indicate the UV protection activity. Alkyl cinnamate compounds are predicted as UV-B and UV-C sunscreen.

Polylogs, thermodynamics and scaling functions of one-dimensional quantum many-body systems

International Nuclear Information System (INIS)

Guan, X-W; Batchelor, M T

2011-01-01

We demonstrate that the thermodynamics of one-dimensional Lieb-Liniger bosons can be accurately calculated in analytic fashion using the polylog function in the framework of the thermodynamic Bethe ansatz. The approach does away with the need to numerically solve the thermodynamic Bethe ansatz (Yang-Yang) equation. The expression for the equation of state allows the exploration of Tomonaga-Luttinger liquid physics and quantum criticality in an archetypical quantum system. In particular, the low-temperature phase diagram is obtained, along with the scaling functions for the density and compressibility. It has been shown recently by Guan and Ho (arXiv:1010.1301) that such scaling can be used to map out the criticality of ultracold fermionic atoms in experiments. We show here how to map out quantum criticality for Lieb-Liniger bosons. More generally, the polylog function formalism can be applied to a wide range of Bethe ansatz integrable quantum many-body systems which are currently of theoretical and experimental interest, such as strongly interacting multi-component fermions, spinor bosons and mixtures of bosons and fermions. (fast track communication)

Quantum capacity of quantum black holes

Science.gov (United States)

Adami, Chris; Bradler, Kamil

2014-03-01

The fate of quantum entanglement interacting with a black hole has been an enduring mystery, not the least because standard curved space field theory does not address the interaction of black holes with matter. We discuss an effective Hamiltonian of matter interacting with a black hole that has a precise analogue in quantum optics and correctly reproduces both spontaneous and stimulated Hawking radiation with grey-body factors. We calculate the quantum capacity of this channel in the limit of perfect absorption, as well as in the limit of a perfectly reflecting black hole (a white hole). We find that the white hole is an optimal quantum cloner, and is isomorphic to the Unruh channel with positive quantum capacity. The complementary channel (across the horizon) is entanglement-breaking with zero capacity, avoiding a violation of the quantum no-cloning theorem. The black hole channel on the contrary has vanishing capacity, while its complement has positive capacity instead. Thus, quantum states can be reconstructed faithfully behind the black hole horizon, but not outside. This work sheds new light on black hole complementarity because it shows that black holes can both reflect and absorb quantum states without violating the no-cloning theorem, and makes quantum firewalls obsolete.

Comparison Of Quantum Mechanical And Classical Trajectory Calculations Of Cross Sections For Ion-Atom Impact Ionization of Negative - And Positive -Ions For Heavy Ion Fusion Applications

International Nuclear Information System (INIS)

Kaganovich, Igor D.; Startsev, Edward A.; Davidson, Ronald C.

2003-01-01

Stripping cross sections in nitrogen have been calculated using the classical trajectory approximation and the Born approximation of quantum mechanics for the outer shell electrons of 3.2GeV I - and Cs + ions. A large difference in cross section, up to a factor of six, calculated in quantum mechanics and classical mechanics, has been obtained. Because at such high velocities the Born approximation is well validated, the classical trajectory approach fails to correctly predict the stripping cross sections at high energies for electron orbitals with low ionization potential

Quantum kinematics of spacetime. II. A model quantum cosmology with real clocks

International Nuclear Information System (INIS)

Hartle, J.B.

1988-01-01

Nonrelativistic model quantum cosmologies are studied in which the basic time variable is the position of a clock indicator and the time parameter of the Schroedinger equation is an unobservable label. Familiar Schroedinger-Heisenberg quantum mechanics emerges if the clock is ideal: arbitrarily accurate for arbitrarily long times. More realistically, however, the usual formulation emerges only as an approximation appropriate to states of this model universe in which part of the system functions approximately as an ideal clock. It is suggested that the quantum kinematics of spacetime theories such as general relativity may be analogous to those of this model. In particular it is suggested that our familiar notion of time in quantum mechanics is not an inevitable property of a general quantum framework but an approximate feature of specific initial conditions

FragIt: a tool to prepare input files for fragment based quantum chemical calculations.

Directory of Open Access Journals (Sweden)

Casper Steinmann

Full Text Available Near linear scaling fragment based quantum chemical calculations are becoming increasingly popular for treating large systems with high accuracy and is an active field of research. However, it remains difficult to set up these calculations without expert knowledge. To facilitate the use of such methods, software tools need to be available to support these methods and help to set up reasonable input files which will lower the barrier of entry for usage by non-experts. Previous tools relies on specific annotations in structure files for automatic and successful fragmentation such as residues in PDB files. We present a general fragmentation methodology and accompanying tools called FragIt to help setup these calculations. FragIt uses the SMARTS language to locate chemically appropriate fragments in large structures and is applicable to fragmentation of any molecular system given suitable SMARTS patterns. We present SMARTS patterns of fragmentation for proteins, DNA and polysaccharides, specifically for D-galactopyranose for use in cyclodextrins. FragIt is used to prepare input files for the Fragment Molecular Orbital method in the GAMESS program package, but can be extended to other computational methods easily.

Explorations in quantum computing

CERN Document Server

Williams, Colin P

2011-01-01

By the year 2020, the basic memory components of a computer will be the size of individual atoms. At such scales, the current theory of computation will become invalid. ""Quantum computing"" is reinventing the foundations of computer science and information theory in a way that is consistent with quantum physics - the most accurate model of reality currently known. Remarkably, this theory predicts that quantum computers can perform certain tasks breathtakingly faster than classical computers -- and, better yet, can accomplish mind-boggling feats such as teleporting information, breaking suppos

Quantum confined Stark effect in Gaussian quantum wells: A tight-binding study

International Nuclear Information System (INIS)

Ramírez-Morales, A.; Martínez-Orozco, J. C.; Rodríguez-Vargas, I.

2014-01-01

The main characteristics of the quantum confined Stark effect (QCSE) are studied theoretically in quantum wells of Gaussian profile. The semi-empirical tight-binding model and the Green function formalism are applied in the numerical calculations. A comparison of the QCSE in quantum wells with different kinds of confining potential is presented

Quantum confined Stark effect in Gaussian quantum wells: A tight-binding study

Energy Technology Data Exchange (ETDEWEB)

Ramírez-Morales, A.; Martínez-Orozco, J. C.; Rodríguez-Vargas, I. [Unidad Académica de Física, Universidad Autónoma de Zacatecas, Calzada Solidaridad Esquina Con Paseo La Bufa S/N, 98060 Zacatecas, Zac. (Mexico)

2014-05-15

The main characteristics of the quantum confined Stark effect (QCSE) are studied theoretically in quantum wells of Gaussian profile. The semi-empirical tight-binding model and the Green function formalism are applied in the numerical calculations. A comparison of the QCSE in quantum wells with different kinds of confining potential is presented.

Hybrid quantum-classical modeling of quantum dot devices

Science.gov (United States)

Kantner, Markus; Mittnenzweig, Markus; Koprucki, Thomas

2017-11-01

The design of electrically driven quantum dot devices for quantum optical applications asks for modeling approaches combining classical device physics with quantum mechanics. We connect the well-established fields of semiclassical semiconductor transport theory and the theory of open quantum systems to meet this requirement. By coupling the van Roosbroeck system with a quantum master equation in Lindblad form, we introduce a new hybrid quantum-classical modeling approach, which provides a comprehensive description of quantum dot devices on multiple scales: it enables the calculation of quantum optical figures of merit and the spatially resolved simulation of the current flow in realistic semiconductor device geometries in a unified way. We construct the interface between both theories in such a way, that the resulting hybrid system obeys the fundamental axioms of (non)equilibrium thermodynamics. We show that our approach guarantees the conservation of charge, consistency with the thermodynamic equilibrium and the second law of thermodynamics. The feasibility of the approach is demonstrated by numerical simulations of an electrically driven single-photon source based on a single quantum dot in the stationary and transient operation regime.

Quantum-Accurate Molecular Dynamics Potential for Tungsten

Energy Technology Data Exchange (ETDEWEB)

Wood, Mitchell; Thompson, Aidan P.

2017-03-01

The purpose of this short contribution is to report on the development of a Spectral Neighbor Analysis Potential (SNAP) for tungsten. We have focused on the characterization of elastic and defect properties of the pure material in order to support molecular dynamics simulations of plasma-facing materials in fusion reactors. A parallel genetic algorithm approach was used to efficiently search for fitting parameters optimized against a large number of objective functions. In addition, we have shown that this many-body tungsten potential can be used in conjunction with a simple helium pair potential1 to produce accurate defect formation energies for the W-He binary system.

Quantum mechanical electronic structure calculation reveals orientation dependence of hydrogen bond energy in proteins.

Science.gov (United States)

Mondal, Abhisek; Datta, Saumen

2017-06-01

Hydrogen bond plays a unique role in governing macromolecular interactions with exquisite specificity. These interactions govern the fundamental biological processes like protein folding, enzymatic catalysis, molecular recognition. Despite extensive research work, till date there is no proper report available about the hydrogen bond's energy surface with respect to its geometric parameters, directly derived from proteins. Herein, we have deciphered the potential energy landscape of hydrogen bond directly from the macromolecular coordinates obtained from Protein Data Bank using quantum mechanical electronic structure calculations. The findings unravel the hydrogen bonding energies of proteins in parametric space. These data can be used to understand the energies of such directional interactions involved in biological molecules. Quantitative characterization has also been performed using Shannon entropic calculations for atoms participating in hydrogen bond. Collectively, our results constitute an improved way of understanding hydrogen bond energies in case of proteins and complement the knowledge-based potential. Proteins 2017; 85:1046-1055. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.

Quantum Computing in Condensed Matter Systems

National Research Council Canada - National Science Library

Privman, V

1997-01-01

Specific theoretical calculations of Hamiltonians corresponding to several quantum logic gates, including the NOT gate, quantum signal splitting, and quantum copying, were obtained and prepared for publication...

Accurate Calculation of Magnetic Fields in the End Regions of Superconducting Accelerator Magnets using the BEM-FEM Coupling Method

CERN Document Server

Kurz, S

1999-01-01

In this paper a new technique for the accurate calculation of magnetic fields in the end regions of superconducting accelerator magnets is presented. This method couples Boundary Elements (BEM) which discretize the surface of the iron yoke and Finite Elements (FEM) for the modelling of the nonlinear interior of the yoke. The BEM-FEM method is therefore specially suited for the calculation of 3-dimensional effects in the magnets, as the coils and the air regions do not have to be represented in the finite-element mesh and discretization errors only influence the calculation of the magnetization (reduced field) of the yoke. The method has been recently implemented into the CERN-ROXIE program package for the design and optimization of the LHC magnets. The field shape and multipole errors in the two-in-one LHC dipoles with its coil ends sticking out of the common iron yoke is presented.

Accurate structures and energetics of neutral-framework zeotypes from dispersion-corrected DFT calculations

Science.gov (United States)

Fischer, Michael; Angel, Ross J.

2017-05-01

Density-functional theory (DFT) calculations incorporating a pairwise dispersion correction were employed to optimize the structures of various neutral-framework compounds with zeolite topologies. The calculations used the PBE functional for solids (PBEsol) in combination with two different dispersion correction schemes, the D2 correction devised by Grimme and the TS correction of Tkatchenko and Scheffler. In the first part of the study, a benchmarking of the DFT-optimized structures against experimental crystal structure data was carried out, considering a total of 14 structures (8 all-silica zeolites, 4 aluminophosphate zeotypes, and 2 dense phases). Both PBEsol-D2 and PBEsol-TS showed an excellent performance, improving significantly over the best-performing approach identified in a previous study (PBE-TS). The temperature dependence of lattice parameters and bond lengths was assessed for those zeotypes where the available experimental data permitted such an analysis. In most instances, the agreement between DFT and experiment improved when the experimental data were corrected for the effects of thermal motion and when low-temperature structure data rather than room-temperature structure data were used as a reference. In the second part, a benchmarking against experimental enthalpies of transition (with respect to α-quartz) was carried out for 16 all-silica zeolites. Excellent agreement was obtained with the PBEsol-D2 functional, with the overall error being in the same range as the experimental uncertainty. Altogether, PBEsol-D2 can be recommended as a computationally efficient DFT approach that simultaneously delivers accurate structures and energetics of neutral-framework zeotypes.

Accurate Compton scattering measurements for N{sub 2} molecules

Energy Technology Data Exchange (ETDEWEB)

Kobayashi, Kohjiro [Advanced Technology Research Center, Gunma University, 1-5-1 Tenjin-cho, Kiryu, Gunma 376-8515 (Japan); Itou, Masayoshi; Tsuji, Naruki; Sakurai, Yoshiharu [Japan Synchrotron Radiation Research Institute (JASRI), 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198 (Japan); Hosoya, Tetsuo; Sakurai, Hiroshi, E-mail: sakuraih@gunma-u.ac.jp [Department of Production Science and Technology, Gunma University, 29-1 Hon-cho, Ota, Gunma 373-0057 (Japan)

2011-06-14

The accurate Compton profiles of N{sub 2} gas were measured using 121.7 keV synchrotron x-rays. The present accurate measurement proves the better agreement of the CI (configuration interaction) calculation than the Hartree-Fock calculation and suggests the importance of multi-excitation in the CI calculations for the accuracy of wavefunctions in ground states.

Infrared and Raman spectroscopy and quantum chemistry calculation studies of C-H...O hydrogen bondings and thermal behavior of biodegradable polyhydroxyalkanoate

Czech Academy of Sciences Publication Activity Database

Sato, H.; Dybal, Jiří; Murakami, R.; Noda, I.; Ozaki, Y.

744-747, - (2005), s. 35-46 ISSN 0022-2860 R&D Projects: GA AV ČR IAA4050208 Keywords : infrared and Raman spectroscopy * quantum chemical calculation * C-H...O hydrogen bonding Subject RIV: CD - Macromolecular Chemistry Impact factor: 1.440, year: 2005

A group theoretic approach to quantum information

CERN Document Server

Hayashi, Masahito

2017-01-01

This textbook is the first one addressing quantum information from the viewpoint of group symmetry. Quantum systems have a group symmetrical structure. This structure enables to handle systematically quantum information processing. However, there is no other textbook focusing on group symmetry for quantum information although there exist many textbooks for group representation. After the mathematical preparation of quantum information, this book discusses quantum entanglement and its quantification by using group symmetry. Group symmetry drastically simplifies the calculation of several entanglement measures although their calculations are usually very difficult to handle. This book treats optimal information processes including quantum state estimation, quantum state cloning, estimation of group action and quantum channel etc. Usually it is very difficult to derive the optimal quantum information processes without asymptotic setting of these topics. However, group symmetry allows to derive these optimal solu...

LETTER TO THE EDITOR: Quantum manifestations of closed orbits in the photoexcitation scaled spectrum of the hydrogen atom in crossed fields

Science.gov (United States)

Rao, Jianguo; Delande, D.; Taylor, K. T.

2001-06-01

The scaled photoexcitation spectrum of the hydrogen atom in crossed electric and magnetic fields has been obtained by means of accurate quantum mechanical calculation using a new algorithm. Closed orbits in the corresponding classical system have also been obtained, using a new, efficient and practical searching procedure. Two new classes of closed orbit have been identified. Fourier transforming each photoexcitation quantum spectrum to yield a plot against scaled action has allowed direct comparison between peaks in such plots and the scaled action values of closed orbits. Excellent agreement has been found with all peaks assigned.

The rotational spectra of HCNH/+/ and COH/+/ from quantum mechanical calculations

Science.gov (United States)

Defrees, D. J.; Loew, G. H.; Mclean, A. D.

1982-01-01

A description is provided of ab initio molecular orbital calculations designed to provide accurate predictions for the J = 1 to 0 rotational line of the candidate interstellar molecules HCNH(+) and COH(+). The former is believed to be important in the formation of both HCN and HNC in the interstellar medium. The latter, a metastable isomer of HCO(+), was first proposed as an interstellar molecule by Herbst et al. (1976). Attention is given to thermochemical arguments that this molecule can be formed in the same reactions which are proposed to form HCO(+), taking into account theoretical data which establish its stability to intramolecular rearrangement. Rotational constants are derived by applying an empirical correction to the ab initio rotational constants.

Colocalization analysis in fluorescence micrographs: verification of a more accurate calculation of pearson's correlation coefficient.

Science.gov (United States)

Barlow, Andrew L; Macleod, Alasdair; Noppen, Samuel; Sanderson, Jeremy; Guérin, Christopher J

2010-12-01

One of the most routine uses of fluorescence microscopy is colocalization, i.e., the demonstration of a relationship between pairs of biological molecules. Frequently this is presented simplistically by the use of overlays of red and green images, with areas of yellow indicating colocalization of the molecules. Colocalization data are rarely quantified and can be misleading. Our results from both synthetic and biological datasets demonstrate that the generation of Pearson's correlation coefficient between pairs of images can overestimate positive correlation and fail to demonstrate negative correlation. We have demonstrated that the calculation of a thresholded Pearson's correlation coefficient using only intensity values over a determined threshold in both channels produces numerical values that more accurately describe both synthetic datasets and biological examples. Its use will bring clarity and accuracy to colocalization studies using fluorescent microscopy.

Quantum biological information theory

CERN Document Server

Djordjevic, Ivan B

2016-01-01

This book is a self-contained, tutorial-based introduction to quantum information theory and quantum biology. It serves as a single-source reference to the topic for researchers in bioengineering, communications engineering, electrical engineering, applied mathematics, biology, computer science, and physics. The book provides all the essential principles of the quantum biological information theory required to describe the quantum information transfer from DNA to proteins, the sources of genetic noise and genetic errors as well as their effects. Integrates quantum information and quantum biology concepts; Assumes only knowledge of basic concepts of vector algebra at undergraduate level; Provides a thorough introduction to basic concepts of quantum information processing, quantum information theory, and quantum biology; Includes in-depth discussion of the quantum biological channel modelling, quantum biological channel capacity calculation, quantum models of aging, quantum models of evolution, quantum models o...

Quantum Dots: Theory

Energy Technology Data Exchange (ETDEWEB)

Vukmirovic, Nenad; Wang, Lin-Wang

2009-11-10

This review covers the description of the methodologies typically used for the calculation of the electronic structure of self-assembled and colloidal quantum dots. These are illustrated by the results of their application to a selected set of physical effects in quantum dots.

Phase Diagram of Hydrogen and a Hydrogen-Helium Mixture at Planetary Conditions by Quantum Monte Carlo Simulations

Science.gov (United States)

Mazzola, Guglielmo; Helled, Ravit; Sorella, Sandro

2018-01-01

Understanding planetary interiors is directly linked to our ability of simulating exotic quantum mechanical systems such as hydrogen (H) and hydrogen-helium (H-He) mixtures at high pressures and temperatures. Equation of state (EOS) tables based on density functional theory are commonly used by planetary scientists, although this method allows only for a qualitative description of the phase diagram. Here we report quantum Monte Carlo (QMC) molecular dynamics simulations of pure H and H-He mixture. We calculate the first QMC EOS at 6000 K for a H-He mixture of a protosolar composition, and show the crucial influence of He on the H metallization pressure. Our results can be used to calibrate other EOS calculations and are very timely given the accurate determination of Jupiter's gravitational field from the NASA Juno mission and the effort to determine its structure.

Distribution of electron density and internal rotation in phospha-alkenes according to data from quantum-chemical calculations by the MNDO method

International Nuclear Information System (INIS)

Boldeskul, I.E.; Pen'kovskii, V.V.; Povolotskii, M.I.

1988-01-01

A quantum-chemical investigation of the characteristics of the phosphorus-carbon bond and the internal rotation around it in phospha-alkenes has been carried out in the MNDO approximation. The results of the calculation have been compared with experimental dynamic 1 H NMR data

Complex-scaling of screened Coulomb potentials for resonance calculations utilizing the modified Bessel functions

Science.gov (United States)

Jiao, Li-Guang; Ho, Yew Kam

2014-05-01

The screened Coulomb potential (SCP) has been extensively used in atomic physics, nuclear physics, quantum chemistry and plasma physics. However, an accurate calculation for atomic resonances under SCP is still a challenging task for various methods. Within the complex-scaling computational scheme, we have developed a method utilizing the modified Bessel functions to calculate doubly-excited resonances in two-electron atomic systems with configuration interaction-type basis. To test the validity of our method, we have calculated S- and P-wave resonance states of the helium atom with various screening strengths, and have found good agreement with earlier calculations using different methods. Our present method can be applied to calculate high-lying resonances associated with high excitation thresholds of the He+ ion, and with high-angular-momentum states. The derivation and calculation details of our present investigation together with new results of high-angular-momentum states will be presented at the meeting. Supported by NSC of Taiwan.

Quantum close coupling calculation of transport and relaxation properties for Hg-H{sub 2} system

Energy Technology Data Exchange (ETDEWEB)

Nemati-Kande, Ebrahim; Maghari, Ali, E-mail: maghari@ut.ac.ir

2016-11-10

Highlights: • Several relaxation cross sections are calculated for Hg-H{sub 2} van der Waals complex. • These cross sections are calculated from exact close-coupling method. • Energy-dependent SBE cross sections are calculated for ortho- and para-H{sub 2} + Hg systems. • Viscosity and diffusion coefficients are calculated using Mason-Monchick approximation. • The results obtained by Mason-Monchick approximation are compared to the exact close-coupling results. - Abstract: Quantum mechanical close coupling calculation of the state-to-state transport and relaxation cross sections have been done for Hg-H{sub 2} molecular system using a high-level ab initio potential energy surface. Rotationally averaged cross sections were also calculated to obtain the energy dependent Senftleben-Beenakker cross sections at the energy range of 0.005–25,000 cm{sup −1}. Boltzmann averaging of the energy dependent Senftleben-Beenakker cross sections showed the temperature dependency over a wide temperature range of 50–2500 K. Interaction viscosity and diffusion coefficients were also calculated using close coupling cross sections and full classical Mason-Monchick approximation. The results were compared with each other and with the available experimental data. It was found that Mason-Monchick approximation for viscosity is more reliable than diffusion coefficient. Furthermore, from the comparison of the experimental diffusion coefficients with the result of the close coupling and Mason-Monchick approximation, it was found that the Hg-H{sub 2} potential energy surface used in this work can reliably predict diffusion coefficient data.

Solving the scalability issue in quantum-based refinement: Q|R#1.

Science.gov (United States)

Zheng, Min; Moriarty, Nigel W; Xu, Yanting; Reimers, Jeffrey R; Afonine, Pavel V; Waller, Mark P

2017-12-01

Accurately refining biomacromolecules using a quantum-chemical method is challenging because the cost of a quantum-chemical calculation scales approximately as n m , where n is the number of atoms and m (≥3) is based on the quantum method of choice. This fundamental problem means that quantum-chemical calculations become intractable when the size of the system requires more computational resources than are available. In the development of the software package called Q|R, this issue is referred to as Q|R#1. A divide-and-conquer approach has been developed that fragments the atomic model into small manageable pieces in order to solve Q|R#1. Firstly, the atomic model of a crystal structure is analyzed to detect noncovalent interactions between residues, and the results of the analysis are represented as an interaction graph. Secondly, a graph-clustering algorithm is used to partition the interaction graph into a set of clusters in such a way as to minimize disruption to the noncovalent interaction network. Thirdly, the environment surrounding each individual cluster is analyzed and any residue that is interacting with a particular cluster is assigned to the buffer region of that particular cluster. A fragment is defined as a cluster plus its buffer region. The gradients for all atoms from each of the fragments are computed, and only the gradients from each cluster are combined to create the total gradients. A quantum-based refinement is carried out using the total gradients as chemical restraints. In order to validate this interaction graph-based fragmentation approach in Q|R, the entire atomic model of an amyloid cross-β spine crystal structure (PDB entry 2oNA) was refined.

Standard Gibbs energies of formation and equilibrium constants from ab-initio calculations: Covalent dimerization of NO2 and synthesis of NH3

International Nuclear Information System (INIS)

Awasthi, Neha; Ritschel, Thomas; Lipowsky, Reinhard; Knecht, Volker

2013-01-01

Highlights: • ΔG and K eq for NO 2 dimerization and NH 3 synthesis calculated via ab-initio methods. • Vis-á-vis experiments, W1 and CCSD(T) are accurate and G3B3 also does quite well. • CBS-APNO most accurate for NH 3 reaction but shows limitations in modeling NO 2 . • Temperature dependence of ΔG and K eq is calculated for the NH 3 reaction. • Good agreement of calculated K eq with experiments and the van’t Hoff approximation. -- Abstract: Standard quantum chemical methods are used for accurate calculation of thermochemical properties such as enthalpies of formation, entropies and Gibbs energies of formation. Equilibrium reactions are widely investigated and experimental measurements often lead to a range of reaction Gibbs energies and equilibrium constants. It is useful to calculate these equilibrium properties from quantum chemical methods in order to address the experimental differences. Furthermore, most standard calculation methods differ in accuracy and feasibility of the system size. Hence, a systematic comparison of equilibrium properties calculated with different numerical algorithms would provide a useful reference. We select two well-known gas phase equilibrium reactions with small molecules: covalent dimer formation of NO 2 (2NO 2 ⇌ N 2 O 4 ) and the synthesis of NH 3 (N 2 + 3 H 2 ⇌ 2NH 3 ). We test four quantum chemical methods denoted by G3B3, CBS-APNO, W1 and CCSD(T) with aug-cc-pVXZ basis sets (X = 2, 3, and 4), to obtain thermochemical data for NO 2 , N 2 O 4 , and NH 3 . The calculated standard formation Gibbs energies Δ f G° are used to calculate standard reaction Gibbs energies Δ r G° and standard equilibrium constants K eq for the two reactions. Standard formation enthalpies Δ f H° are calculated in a more reliable way using high-level methods such as W1 and CCSD(T). Standard entropies S° for the molecules are calculated well within the range of experiments for all methods, however, the values of standard formation

Channel-coupling theory of covalent bonding in H2: A further application of arrangement-channel quantum mechanics

International Nuclear Information System (INIS)

Levin, F.S.; Krueger, H.

1977-01-01

The dissociation energy D/sub e/ and the equilibrium proton-proton separation R/sub eq/ of H 2 are calculated using the methods of arrangement-channel quantum mechanics. This theory is the channel component version of the channel-coupling array approach to many-body scattering, applied to bound-state problems. In the approximation used herein, the wave function is identical to that of the classic Heitler-London-Sugiura valence-bond calculation, which gave D/sub e/ = 3.14 eV and R/sub eq/ = 1.65a 0 , values accurate to 34% and 17.8%, respectively. The present method yields D/sub e/ = 4.437 eV and R/sub eq/ approx. = 1.42a 0 , accurate to 6.5% and 1%, respectively. Some implications of these results are discussed

Molecular structure of tris(cyclopropylsilyl)amine as determined by gas electron diffraction and quantum-chemical calculations

Science.gov (United States)

Vishnevskiy, Yuri V.; Abaev, Maxim A.; Ivanov, Arkadii A.; Vilkov, Lev V.; Dakkouri, Marwan

2008-10-01

The molecular structure and conformation of tris(cyclopropylsilyl)amine (TCPSA) has been studied by means of gas-phase electron diffraction at 338 K and quantum-chemical calculations. A total of 12 relatively stable conformations of TCPSA molecule were considered. According to the experimental results and the DFT calculations the most stable conformer corresponds to a configuration (according to the Prelog-Klyne notation) of the type (-ac)(-ac)(+ac)-(-ac)(-ac)(+ac), where the first three parentheses describe the three different Si-N-Si-C torsional angles and the latter ones depict the rotation of the three cyclopropyl groups about the C ring-Si axes, respectively. The quantum-mechanical calculations were performed using various density functional (B3LYP, X3LYP and O3LYP) and perturbation MP2 methods in combination with double- and triple- ζ basis sets plus polarization and diffuse functions. The most important experimental geometrical parameters of TCPSA ( ra Å, ∠ h1 degrees) are: (Si-N) av = 1.741(3), (Si-C) av = 1.866(4), (C-C) av = 1.510(3), (C-C(Si)) av = 1.535(3), (N-Si-C) av = 115.1(18)°. For the purpose of comparison and searching for reasons leading to the planarity of the Si 3N moiety in trisilylated amines we carried out NBO analysis and optimized the geometries of numerous silylamines. Among these compounds was tris(allylsilyl)amine (TASA), which is isovalent and isoelectronic to TCPSA. Utilizing the structural results we obtained we could show that Si +⋯Si + electrostatic repulsive interaction is predominantly responsible for the planarity of the Si 3N skeleton in TCPSA and in all other trisilylamines we considered. We also found that regardless the size and partial charges of the substituents the Si-N-Si bond angle in various disilylamines amounts to 130 ± 2°.

MODELING OF ALKYL SALICYLATE COMPOUNDS AS UV ABSORBER BASED ON ELECTRONIC TRANSITION BY USING SEMIEMPIRICAL QUANTUM MECHANICS ZINDO/s CALCULATION

Directory of Open Access Journals (Sweden)

Iqmal Tahir

2010-06-01

Full Text Available Modeling of several alkyl salicylates based on electronic transition by using semiempriical mechanical quantum ZINDO/s calculation has been done. Object of these research were assumed only alkyl salicylates of C4 (butyl until C8 (octyl homologue with 4-7 example structures of each homologue. All of the computation have been performed using quantum chemistry - package software Hyperchem 6.0. The research covered about drawing each of the structure, geometry optimization using semiempirical AM1 algorithm and followed with single point calculation using semiempirical ZINDO/s technique. ZINDO/s calculations used a defined criteria that is singly excited - Configuration Interaction (CI, gap of HOMO-LUMO energy transition was 2 and degeneracy level was 3. Analysis of the theoretical spectra was focused in the UV-B (290-320 nm and UV-C (200-290 nm area. The result showed that modeling of the compound can be used for predicting the type of UV protection activity depending with the electronic transition in the UV area. Modification of the alkyl homologue relatively did not change the value of wavelength absorbtion to indicate the UV protection activity. Alkyl salicylate compounds were predicted as UV-C sunscreen or relatively the compounds have protection effect for UV-C.   Keywords: alkyl salicylate, sunscreen, semiempirical methods

Tuning of few-electron states and optical absorption anisotropy in GaAs quantum rings.

Science.gov (United States)

Wu, Zhenhua; Li, Jian; Li, Jun; Yin, Huaxiang; Liu, Yu

2017-11-15

The electronic and optical properties of a GaAs quantum ring (QR) with few electrons in the presence of the Rashba spin-orbit interaction (RSOI) and the Dresselhaus spin-orbit interaction (DSOI) have been investigated theoretically. The configuration interaction (CI) method is employed to calculate the eigenvalues and eigenstates of the multiple-electron QR accurately. Our numerical results demonstrate that the symmetry breaking induced by the RSOI and DSOI leads to an anisotropic distribution of multi-electron states. The Coulomb interaction offers additional modulation of the electron distribution and thus the optical absorption indices in the quantum rings. By tuning the magnetic/electric fields and/or electron numbers in a quantum ring, one can change its optical properties significantly. Our theory provides a new way to control the multi-electron states and optical properties of a QR by hybrid modulations or by electrical means only.

Repulsive energy and the Grueneisen parameter of alkali halides calculated on the basis of a quantum-statistical ab initio theory

International Nuclear Information System (INIS)

Kucharczyk, M.; Olszewski, S.

1982-01-01

The Grueneisen parameter of alkali halides is calculated by an ab initio quantum-statistical method and then compared with the experimental data. The crystal model applied assumes the crystal ions to be compressible but impenetrable spheres. The ions are described with the aid of a modified Thomas-Fermi theory with exchange. At the next step it is possible to calculate the energy needed to transform the system of the non-interacting ions into the ionic system represented by the crystal lattice. This calculation allows for an ab initio estimate of the parameters entering the Born, or the Born-Mayer, repulsive part of the crystal energy. The parameters are then used in the calculation of the Grueneisen parameter and its dependence on the crystal compression. (author)

Quantum size effect and thermal stability of carbon-nanotube-based quantum dot

International Nuclear Information System (INIS)

Huang, N.Y.; Peng, J.; Liang, S.D.; Li, Z.B.; Xu, N.S.

2004-01-01

Full text: Based on semi-experience quantum chemical calculation, we have investigated the quantum size effect and thermal stability of open-end carbon nanotube (5, 5) quantum dots of 20 to 400 atoms. It was found that there is a gap in the energy band of all carbon nanotube (5, 5) quantum dots although a (5, 5) carbon nanotube is metallic. The energy gap of quantum dots is much dependent of the number of atoms in a dot, as a result of the quantization rules imposed by the finite scales in both radial and axial directions of a carbon nanotube quantum dot. Also, the heat of formation of carbon nanotube quantum dots is dependent of the size of a quantum dot. (author)

Secure multi-party quantum summation based on quantum Fourier transform

Science.gov (United States)

Yang, Hui-Yi; Ye, Tian-Yu

2018-06-01

In this paper, we propose a novel secure multi-party quantum summation protocol based on quantum Fourier transform, where the traveling particles are transmitted in a tree-type mode. The party who prepares the initial quantum states is assumed to be semi-honest, which means that she may misbehave on her own but will not conspire with anyone. The proposed protocol can resist both the outside attacks and the participant attacks. Especially, one party cannot obtain other parties' private integer strings; and it is secure for the colluding attack performed by at most n - 2 parties, where n is the number of parties. In addition, the proposed protocol calculates the addition of modulo d and implements the calculation of addition in a secret-by-secret way rather than a bit-by-bit way.

Quantum computing applied to calculations of molecular energies

Czech Academy of Sciences Publication Activity Database

Pittner, Jiří; Veis, L.

2011-01-01

Roč. 241, - (2011), 151-phys ISSN 0065-7727. [National Meeting and Exposition of the American-Chemical-Society (ACS) /241./. 27.03.2011-31.03.2011, Anaheim] Institutional research plan: CEZ:AV0Z40400503 Keywords : molecular energie * quantum computers Subject RIV: CF - Physical ; Theoretical Chemistry

Dynamics of a quantum phase transition

International Nuclear Information System (INIS)

Zurek, W.H.

2005-01-01

We present two approaches to the non-equilibrium dynamics of a quench-induced phase transition in quantum Ising model. First approach retraces steps of the standard calculation to thermodynamic second order phase transitions in the quantum setting. The second calculation is purely quantum, based on the Landau-Zener formula for transition probabilities in processes that involve avoided level crossings. We show that the two approaches yield compatible results for the scaling of the defect density with the quench rate. We exhibit similarities between them, and comment on the insights they give into dynamics of quantum phase transitions. (author)

Higher order energy transfer. Quantum electrodynamical calculations and graphical representation

International Nuclear Information System (INIS)

Jenkins, R.D.

2000-01-01

In Chapter 1, a novel method of calculating quantum electrodynamic amplitudes is formulated using combinatorial theory. This technique is used throughout instead of conventional time-ordered methods. A variety of hyperspaces are discussed to highlight isomorphism between a number of A generalisation of Pascal's triangle is shown to be beneficial in determining the form of hyperspace graphs. Chapter 2 describes laser assisted resonance energy transfer (LARET), a higher order perturbative contribution to the well-known process resonance energy transfer, accommodating an off resonance auxiliary laser field to stimulate the migration. Interest focuses on energy exchanges between two uncorrelated molecular species, as in a system where molecules are randomly oriented. Both phase-weighted and standard isotropic averaging are required for the calculations. Results are discussed in terms of a laser intensity-dependent mechanism. Identifying the applied field regime where LARET should prove experimentally significant, transfer rate increases of up to 30% are predicted. General results for three-center energy transfer are elucidated in chapter 3. Cooperative and accretive mechanistic pathways are identified with theory formulated to elicit their role in a variety of energy transfer phenomena and their relative dominance. In multichromophoric the interplay of such factors is analysed with regard to molecular architectures. The alignments and magnitudes of donor and acceptor transition moments and polarisabilities prove to have profound effects on achievable pooling efficiency for linear configurations. Also optimum configurations are offered. In ionic lattices, although both mechanisms play significant roles in pooling and cutting processes, only the accretive is responsible for sensitisation. The local, microscopic level results are used to gauge the lattice response, encompassing concentration and structural effects. (author)

A general intermolecular force field based on tight-binding quantum chemical calculations

Science.gov (United States)

Grimme, Stefan; Bannwarth, Christoph; Caldeweyher, Eike; Pisarek, Jana; Hansen, Andreas

2017-10-01

A black-box type procedure is presented for the generation of a molecule-specific, intermolecular potential energy function. The method uses quantum chemical (QC) information from our recently published extended tight-binding semi-empirical scheme (GFN-xTB) and can treat non-covalently bound complexes and aggregates with almost arbitrary chemical structure. The necessary QC information consists of the equilibrium structure, Mulliken atomic charges, charge centers of localized molecular orbitals, and also of frontier orbitals and orbital energies. The molecular pair potential includes model density dependent Pauli repulsion, penetration, as well as point charge electrostatics, the newly developed D4 dispersion energy model, Drude oscillators for polarization, and a charge-transfer term. Only one element-specific and about 20 global empirical parameters are needed to cover systems with nuclear charges up to radon (Z = 86). The method is tested for standard small molecule interaction energy benchmark sets where it provides accurate intermolecular energies and equilibrium distances. Examples for structures with a few hundred atoms including charged systems demonstrate the versatility of the approach. The method is implemented in a stand-alone computer code which enables rigid-body, global minimum energy searches for molecular aggregation or alignment.

Accurate and systematically improvable density functional theory embedding for correlated wavefunctions

International Nuclear Information System (INIS)

Goodpaster, Jason D.; Barnes, Taylor A.; Miller, Thomas F.; Manby, Frederick R.

2014-01-01

We analyze the sources of error in quantum embedding calculations in which an active subsystem is treated using wavefunction methods, and the remainder using density functional theory. We show that the embedding potential felt by the electrons in the active subsystem makes only a small contribution to the error of the method, whereas the error in the nonadditive exchange-correlation energy dominates. We test an MP2 correction for this term and demonstrate that the corrected embedding scheme accurately reproduces wavefunction calculations for a series of chemical reactions. Our projector-based embedding method uses localized occupied orbitals to partition the system; as with other local correlation methods, abrupt changes in the character of the localized orbitals along a reaction coordinate can lead to discontinuities in the embedded energy, but we show that these discontinuities are small and can be systematically reduced by increasing the size of the active region. Convergence of reaction energies with respect to the size of the active subsystem is shown to be rapid for all cases where the density functional treatment is able to capture the polarization of the environment, even in conjugated systems, and even when the partition cuts across a double bond

Analysis of transient electromagnetic interactions on nanodevices using a quantum corrected integral equation approach

KAUST Repository

Uysal, Ismail Enes

2015-10-26

Analysis of electromagnetic interactions on nanodevices can oftentimes be carried out accurately using “traditional” electromagnetic solvers. However, if a gap of sub-nanometer scale exists between any two surfaces of the device, quantum-mechanical effects including tunneling should be taken into account for an accurate characterization of the device\\'s response. Since the first-principle quantum simulators can not be used efficiently to fully characterize a typical-size nanodevice, a quantum corrected electromagnetic model has been proposed as an efficient and accurate alternative (R. Esteban et al., Nat. Commun., 3(825), 2012). The quantum correction is achieved through an effective layered medium introduced into the gap between the surfaces. The dielectric constant of each layer is obtained using a first-principle quantum characterization of the gap with a different dimension.

Quantum Monte Carlo for atoms and molecules

International Nuclear Information System (INIS)

Barnett, R.N.

1989-11-01

The diffusion quantum Monte Carlo with fixed nodes (QMC) approach has been employed in studying energy-eigenstates for 1--4 electron systems. Previous work employing the diffusion QMC technique yielded energies of high quality for H 2 , LiH, Li 2 , and H 2 O. Here, the range of calculations with this new approach has been extended to include additional first-row atoms and molecules. In addition, improvements in the previously computed fixed-node energies of LiH, Li 2 , and H 2 O have been obtained using more accurate trial functions. All computations were performed within, but are not limited to, the Born-Oppenheimer approximation. In our computations, the effects of variation of Monte Carlo parameters on the QMC solution of the Schroedinger equation were studied extensively. These parameters include the time step, renormalization time and nodal structure. These studies have been very useful in determining which choices of such parameters will yield accurate QMC energies most efficiently. Generally, very accurate energies (90--100% of the correlation energy is obtained) have been computed with single-determinant trail functions multiplied by simple correlation functions. Improvements in accuracy should be readily obtained using more complex trial functions

Perturbations in loop quantum cosmology

International Nuclear Information System (INIS)

Nelson, W; Agullo, I; Ashtekar, A

2014-01-01

The era of precision cosmology has allowed us to accurately determine many important cosmological parameters, in particular via the CMB. Confronting Loop Quantum Cosmology with these observations provides us with a powerful test of the theory. For this to be possible, we need a detailed understanding of the generation and evolution of inhomogeneous perturbations during the early, quantum gravity phase of the universe. Here, we have described how Loop Quantum Cosmology provides a completion of the inflationary paradigm, that is consistent with the observed power spectra of the CMB

Coupled-cluster calculations for ground and excited states of closed- and open-shell nuclei using methods of quantum chemistry

International Nuclear Information System (INIS)

Wloch, Marta; Gour, Jeffrey R; Piecuch, Piotr; Dean, David J; Hjorth-Jensen, Morten; Papenbrock, Thomas

2005-01-01

We discuss large-scale ab initio calculations of ground and excited states of 16 O and preliminary calculations for 15 O and 17 O using coupled-cluster methods and algorithms developed in quantum chemistry. By using realistic two-body interactions and the renormalized form of the Hamiltonian obtained with a no-core G-matrix approach, we are able to obtain the virtually converged results for 16 O and promising results for 15 O and 17 O at the level of two-body interactions. The calculated properties other than binding and excitation energies include charge radius and charge form factor. The relatively low costs of coupled-cluster calculations, which are characterized by the low-order polynomial scaling with the system size, enable us to probe large model spaces with up to seven or eight major oscillator shells, for which nontruncated shell-model calculations for nuclei with A = 15-17 active particles are presently not possible

Optimization of digital image processing to determine quantum dots' height and density from atomic force microscopy.

Science.gov (United States)

Ruiz, J E; Paciornik, S; Pinto, L D; Ptak, F; Pires, M P; Souza, P L

2018-01-01

An optimized method of digital image processing to interpret quantum dots' height measurements obtained by atomic force microscopy is presented. The method was developed by combining well-known digital image processing techniques and particle recognition algorithms. The properties of quantum dot structures strongly depend on dots' height, among other features. Determination of their height is sensitive to small variations in their digital image processing parameters, which can generate misleading results. Comparing the results obtained with two image processing techniques - a conventional method and the new method proposed herein - with the data obtained by determining the height of quantum dots one by one within a fixed area, showed that the optimized method leads to more accurate results. Moreover, the log-normal distribution, which is often used to represent natural processes, shows a better fit to the quantum dots' height histogram obtained with the proposed method. Finally, the quantum dots' height obtained were used to calculate the predicted photoluminescence peak energies which were compared with the experimental data. Again, a better match was observed when using the proposed method to evaluate the quantum dots' height. Copyright © 2017 Elsevier B.V. All rights reserved.

Refractory Graft-Versus-Host Disease-Free, Relapse-Free Survival as an Accurate and Easy-to-Calculate Endpoint to Assess the Long-Term Transplant Success.

Science.gov (United States)

Kawamura, Koji; Nakasone, Hideki; Kurosawa, Saiko; Yoshimura, Kazuki; Misaki, Yukiko; Gomyo, Ayumi; Hayakawa, Jin; Tamaki, Masaharu; Akahoshi, Yu; Kusuda, Machiko; Kameda, Kazuaki; Wada, Hidenori; Ishihara, Yuko; Sato, Miki; Terasako-Saito, Kiriko; Kikuchi, Misato; Kimura, Shun-Ichi; Tanihara, Aki; Kako, Shinichi; Kanamori, Heiwa; Mori, Takehiko; Takahashi, Satoshi; Taniguchi, Shuichi; Atsuta, Yoshiko; Kanda, Yoshinobu

2018-02-21

The aim of this study was to develop a new composite endpoint that accurately reflects the long-term success of allogeneic hematopoietic stem cell transplantation (allo-HSCT), as the conventional graft-versus-host disease (GVHD)-free, relapse-free survival (GRFS) overestimates the impact of GVHD. First, we validated current GRFS (cGRFS), which recently was proposed as a more accurate endpoint of long-term transplant success. cGRFS was defined as survival without disease relapse/progression or active chronic GVHD at a given time after allo-HSCT, calculated using 2 distinct methods: a linear combination of a Kaplan-Meier estimates approach and a multistate modelling approach. Next, we developed a new composite endpoint, refractory GRFS (rGRFS). rGRFS was calculated similarly to conventional GRFS treating grade III to IV acute GVHD, chronic GVHD requiring systemic treatment, and disease relapse/progression as events, except that GVHD that resolved and did not require systemic treatment at the last evaluation was excluded as an event in rGRFS. The 2 cGRFS curves obtained using 2 different approaches were superimposed and both were superior to that of conventional GRFS, reflecting the proportion of patients with resolved chronic GVHD. Finally, the curves of cGRFS and rGRFS overlapped after the first 2 years of post-transplant follow-up. These results suggest that cGRFS and rGRFS more accurately reflect transplant success than conventional GRFS. Especially, rGRFS can be more easily calculated than cGRFS and analyzed with widely used statistical approaches, whereas cGRFS more accurately represents the burden of GVHD-related morbidity in the first 2 years after transplantation. Copyright © 2018 The American Society for Blood and Marrow Transplantation. Published by Elsevier Inc. All rights reserved.

Quantum Mechanical Calculations of Monoxides of Silicon Carbide Molecules

National Research Council Canada - National Science Library

Roberts, John

2003-01-01

.... Recent theoretical work has used small quantum mechanical systems embedded in larger molecular mechanics structures to attempt to better understand SiC surfaces and bulk materials and their oxidation...

2D Quantum Mechanical Study of Nanoscale MOSFETs

Science.gov (United States)

Svizhenko, Alexei; Anantram, M. P.; Govindan, T. R.; Biegel, B.; Kwak, Dochan (Technical Monitor)

2000-01-01

With the onset of quantum confinement in the inversion layer in nanoscale MOSFETs, behavior of the resonant level inevitably determines all device characteristics. While most classical device simulators take quantization into account in some simplified manner, the important details of electrostatics are missing. Our work addresses this shortcoming and provides: (a) a framework to quantitatively explore device physics issues such as the source-drain and gate leakage currents, DIBL, and threshold voltage shift due to quantization, and b) a means of benchmarking quantum corrections to semiclassical models (such as density-gradient and quantum-corrected MEDICI). We have developed physical approximations and computer code capable of realistically simulating 2-D nanoscale transistors, using the non-equilibrium Green's function (NEGF) method. This is the most accurate full quantum model yet applied to 2-D device simulation. Open boundary conditions and oxide tunneling are treated on an equal footing. Electrons in the ellipsoids of the conduction band are treated within the anisotropic effective mass approximation. We present the results of our simulations of MIT 25, 50 and 90 nm "well-tempered" MOSFETs and compare them to those of classical and quantum corrected models. The important feature of quantum model is smaller slope of Id-Vg curve and consequently higher threshold voltage. Surprisingly, the self-consistent potential profile shows lower injection barrier in the channel in quantum case. These results are qualitatively consistent with ID Schroedinger-Poisson calculations. The effect of gate length on gate-oxide leakage and subthreshold current has been studied. The shorter gate length device has an order of magnitude smaller current at zero gate bias than the longer gate length device without a significant trade-off in on-current. This should be a device design consideration.

Quantum-electrodynamics corrections in pionic hydrogen

NARCIS (Netherlands)

Schlesser, S.; Le Bigot, E. -O.; Indelicato, P.; Pachucki, K.

2011-01-01

We investigate all pure quantum-electrodynamics corrections to the np --> 1s, n = 2-4 transition energies of pionic hydrogen larger than 1 meV, which requires an accurate evaluation of all relevant contributions up to order alpha 5. These values are needed to extract an accurate strong interaction

Structure-based sampling and self-correcting machine learning for accurate calculations of potential energy surfaces and vibrational levels

Science.gov (United States)

Dral, Pavlo O.; Owens, Alec; Yurchenko, Sergei N.; Thiel, Walter

2017-06-01

We present an efficient approach for generating highly accurate molecular potential energy surfaces (PESs) using self-correcting, kernel ridge regression (KRR) based machine learning (ML). We introduce structure-based sampling to automatically assign nuclear configurations from a pre-defined grid to the training and prediction sets, respectively. Accurate high-level ab initio energies are required only for the points in the training set, while the energies for the remaining points are provided by the ML model with negligible computational cost. The proposed sampling procedure is shown to be superior to random sampling and also eliminates the need for training several ML models. Self-correcting machine learning has been implemented such that each additional layer corrects errors from the previous layer. The performance of our approach is demonstrated in a case study on a published high-level ab initio PES of methyl chloride with 44 819 points. The ML model is trained on sets of different sizes and then used to predict the energies for tens of thousands of nuclear configurations within seconds. The resulting datasets are utilized in variational calculations of the vibrational energy levels of CH3Cl. By using both structure-based sampling and self-correction, the size of the training set can be kept small (e.g., 10% of the points) without any significant loss of accuracy. In ab initio rovibrational spectroscopy, it is thus possible to reduce the number of computationally costly electronic structure calculations through structure-based sampling and self-correcting KRR-based machine learning by up to 90%.

An analytical procedure to evaluate electronic integrals for molecular quantum mechanical calculations

International Nuclear Information System (INIS)

Mundim, Kleber C.

2004-01-01

Full text: We propose an alternative methodology for the calculation of electronic integrals, through an analytical function based on the generalized Gaussian function (q Gaussian), where a single q Gaussian replaces the usual linear combination of Gaussian functions for different basis set. Moreover, the integrals become analytical functions of the interatomic distances. Therefore, when estimating certain quantities such as molecular energy, g Gaussian avoid new calculations of the integrals: they are simply another value of the corresponding function. The procedure proposed here is particularly advantageous, when compared with the usual one, because it reduces drastically the number of two-electronic integrals used in the construction of the Fock matrix, enabling the use of the quantum mechanics in the description of macro-molecular systems. This advantage increases when the size of the molecular systems become larger and more complex. While in the usual approach CPU time increases with n4, in the one proposed here the CPU time scales linearly with n. This catastrophic dependence of the rank the Hamiltonian or Fock matrix with n4 two-electron integrals is a severe bottleneck for petaFLOPS computing time. Its is important to emphasize that this methodology is equally applicable to systems of any sizes, including biomolecules, solid materials and solutions, within the HF, post-HF and DFT theories. (author)

On the Calculation of Quantum Mechanical Ground States from Classical Geodesic Motion on Certain Spaces of Constant Negative Curvature

CERN Document Server

Tomaschitz, R

1989-01-01

We consider geodesic motion on three-dimensional Riemannian manifolds of constant negative curvature, topologically equivalent to S x ]0,1[, S a compact surface of genus two. To those trajectories which are bounded and recurrent in both directions of the time evolution a fractal limit set is associated whose Hausdorff dimension is intimately connected with the quantum mechanical energy ground state, determined by the Schrodinger operator on the manifold. We give a rather detailed and pictorial description of the hyperbolic spaces we have in mind, discuss various aspects of classical and quantum mechanical motion on them as far as they are needed to establish the connection between energy ground state and Hausdorff dimension and give finally some examples of ground state calculations in terms of Hausdorff dimensions of limit sets of classical trajectories.

Calculation of photoionization differential cross sections using complex Gauss-type orbitals.

Science.gov (United States)

Matsuzaki, Rei; Yabushita, Satoshi

2017-09-05

Accurate theoretical calculation of photoelectron angular distributions for general molecules is becoming an important tool to image various chemical reactions in real time. We show in this article that not only photoionization total cross sections but also photoelectron angular distributions can be accurately calculated using complex Gauss-type orbital (cGTO) basis functions. Our method can be easily combined with existing quantum chemistry techniques including electron correlation effects, and applied to various molecules. The so-called two-potential formula is applied to represent the transition dipole moment from an initial bound state to a final continuum state in the molecular coordinate frame. The two required continuum functions, the zeroth-order final continuum state and the first-order wave function induced by the photon field, have been variationally obtained using the complex basis function method with a mixture of appropriate cGTOs and conventional real Gauss-type orbitals (GTOs) to represent the continuum orbitals as well as the remaining bound orbitals. The complex orbital exponents of the cGTOs are optimized by fitting to the outgoing Coulomb functions. The efficiency of the current method is demonstrated through the calculations of the asymmetry parameters and molecular-frame photoelectron angular distributions of H2+ and H2 . In the calculations of H2 , the static exchange and random phase approximations are employed, and the dependence of the results on the basis functions is discussed. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.

Accurate methods for calculating atomic processes in high temperature plasmas

International Nuclear Information System (INIS)

Keady, J.J.; Abdallah, J.A. Jr.; Clark, R.E.H.

1992-01-01

A technique for computing monochromatic X-ray absorption is described and compared to experimental data. Calculations of power loss from carbon plasmas with comprehensive new datasets confirm that the direct inclusion of metastable states can noticeably decrease the calculated power loss

Digital Quantum Simulation of Spin Models with Circuit Quantum Electrodynamics

Directory of Open Access Journals (Sweden)

Y. Salathé

2015-06-01

Full Text Available Systems of interacting quantum spins show a rich spectrum of quantum phases and display interesting many-body dynamics. Computing characteristics of even small systems on conventional computers poses significant challenges. A quantum simulator has the potential to outperform standard computers in calculating the evolution of complex quantum systems. Here, we perform a digital quantum simulation of the paradigmatic Heisenberg and Ising interacting spin models using a two transmon-qubit circuit quantum electrodynamics setup. We make use of the exchange interaction naturally present in the simulator to construct a digital decomposition of the model-specific evolution and extract its full dynamics. This approach is universal and efficient, employing only resources that are polynomial in the number of spins, and indicates a path towards the controlled simulation of general spin dynamics in superconducting qubit platforms.

QUANTUM: A Wolfram Mathematica add-on for Dirac Bra-Ket Notation, Non-Commutative Algebra, and Simulation of Quantum Computing Circuits

International Nuclear Information System (INIS)

Muñoz, J L Gómez; Delgado, F

2016-01-01

This paper introduces QUANTUM, a free library of commands of Wolfram Mathematica that can be used to perform calculations directly in Dirac braket and operator notation. Its development started several years ago, in order to study quantum random walks. Later, many other features were included, like operator and commutator algebra, simulation and graphing of quantum computing circuits, generation and solution of Heisenberg equations of motion, among others. To the best of our knowledge, QUANTUM remains a unique tool in its use of Dirac notation, because it is used both in the input and output of the calculations. This work depicts its usage and features in Quantum Computing and Quantum Hamilton Dynamics. (paper)

Accurate Quantum Wave Packet Study of the Deep Well D+ + HD Reaction: Product Ro-vibrational State-Resolved Integral and Differential Cross Sections.

Science.gov (United States)

He, Haixiang; Zhu, Weimin; Su, Wenli; Dong, Lihui; Li, Bin

2018-03-08

The H + + H 2 reaction and its isotopic variants as the simplest triatomic ion-molecule reactive system have been attracting much interests, however there are few studies on the titled reaction at state-to-state level until recent years. In this work, accurate state-to-state quantum dynamics studies of the titled reaction have been carried out by a reactant Jacobi coordinate-based time-dependent wave packet approach on diabatic potential energy surfaces constructed by Kamisaka et al. Product ro-vibrational state-resolved information has been calculated for collision energies up to 0.2 eV with maximal total angular momentum J = 40. The necessity of including all K-component for accounting the Coriolis coupling for the reaction has been illuminated. Competitions between the two product channels, (D + + HD' → D' + + HD and D + + HD' → H + + DD') were investigated. Total integral cross sections suggest that resonances enhance the reactivity of channel D + + HD'→ H + + DD', however, resonances depress the reactivity of the another channel D + + HD' → D' + + HD. The structures of the differential cross sections are complicated and depend strongly on collision energies of the two channels and also on the product rotational states. All of the product ro-vibrational state-resolved differential cross sections for this reaction do not exhibit rigorous backward-forward symmetry which may indicate that the lifetimes of the intermediate resonance complexes should not be that long. The dynamical observables of this deuterated isotopic reaction are quite different from the reaction of H + + H 2 → H 2 + H + reported previously.

Raman spectrum, quantum mechanical calculations and vibrational assignments of (95% alpha-TeO2/5% Sm2O3) glass.

Science.gov (United States)

Shaltout, I; Mohamed, Tarek A

2007-06-01

Chozen system of tellurite glasses doped with rare earth oxides (95% alpha-TeO(2)+5% Sm2O3) was prepared by melt quenching. Consequently, the Raman spectrum (150-1250 cm(-1)) of the modified tellurite have been recorded. As a continuation to our normal coordinate analysis, force constants and quantum mechanical (QM) calculations for tbp TeO4(4-) (triagonal bipyramid, C(2v)) and TeO(3+1); Te2O7(6-) (bridged tetrahedral), we have carried out ab initio frequency calculations for tpy TeO3(2-) (triagonal pyramidal, C(3v) and C(s)) and tp TeO3(2-) (triagonal planar, D(3h)) ions. The quantum mechanical calculations at the levels of RHF, B3LYP and MP2 allow confident vibrational assignments and structural identification in the binary oxide glass (95% alpha-TeO2 +5% Sm2O3). The dominant three-dimensional network structures in the modified glass are triagonal pyramidal TeO3 with minor features of short range distorted tbp TeO4 and bridged tetrahedral unit of TeO(3+1), leading to a structure of infinite chain. Therefore, alpha-TeO2/Sm2O3 (95/5%) glass experience structural changes from TeO4 (tbp); Te2O7 (TeO(3+1))-->TeO3 (tpy).

Effects of quantum confinement and shape on band gap of core/shell quantum dots and nanowires

Science.gov (United States)

Gao, Faming

2011-05-01

A quantum confinement model for nanocrystals developed is extended to study for the optical gap shifts in core/shell quantum dots and nanowires. The chemical bond properties and gap shifts in the InP/ZnS, CdSe/CdS, CdSe/ZnS, and CdTe/ZnS core/shell quantum dots are calculated in detail. The calculated band gaps are in excellent agreement with experimental values. The effects of structural taping and twinning on quantum confinement of InP and Si nanowires are elucidated. It is found theoretically that a competition between the positive Kubo energy-gap shift and the negative surface energy shift plays the crucial role in the optical gaps of these nanosystems.

Machine learning of accurate energy-conserving molecular force fields

Science.gov (United States)

Chmiela, Stefan; Tkatchenko, Alexandre; Sauceda, Huziel E.; Poltavsky, Igor; Schütt, Kristof T.; Müller, Klaus-Robert

2017-01-01

Using conservation of energy—a fundamental property of closed classical and quantum mechanical systems—we develop an efficient gradient-domain machine learning (GDML) approach to construct accurate molecular force fields using a restricted number of samples from ab initio molecular dynamics (AIMD) trajectories. The GDML implementation is able to reproduce global potential energy surfaces of intermediate-sized molecules with an accuracy of 0.3 kcal mol−1 for energies and 1 kcal mol−1 Å̊−1 for atomic forces using only 1000 conformational geometries for training. We demonstrate this accuracy for AIMD trajectories of molecules, including benzene, toluene, naphthalene, ethanol, uracil, and aspirin. The challenge of constructing conservative force fields is accomplished in our work by learning in a Hilbert space of vector-valued functions that obey the law of energy conservation. The GDML approach enables quantitative molecular dynamics simulations for molecules at a fraction of cost of explicit AIMD calculations, thereby allowing the construction of efficient force fields with the accuracy and transferability of high-level ab initio methods. PMID:28508076

Linear entropy in quantum phase space

International Nuclear Information System (INIS)

Rosales-Zarate, Laura E. C.; Drummond, P. D.

2011-01-01

We calculate the quantum Renyi entropy in a phase-space representation for either fermions or bosons. This can also be used to calculate purity and fidelity, or the entanglement between two systems. We show that it is possible to calculate the entropy from sampled phase-space distributions in normally ordered representations, although this is not possible for all quantum states. We give an example of the use of this method in an exactly soluble thermal case. The quantum entropy cannot be calculated at all using sampling methods in classical symmetric (Wigner) or antinormally ordered (Husimi) phase spaces, due to inner-product divergences. The preferred method is to use generalized Gaussian phase-space methods, which utilize a distribution over stochastic Green's functions. We illustrate this approach by calculating the reduced entropy and entanglement of bosonic or fermionic modes coupled to a time-evolving, non-Markovian reservoir.

Linear entropy in quantum phase space

Energy Technology Data Exchange (ETDEWEB)

Rosales-Zarate, Laura E. C.; Drummond, P. D. [Centre for Atom Optics and Ultrafast Spectroscopy, Swinburne University of Technology, Melbourne 3122 (Australia)

2011-10-15

We calculate the quantum Renyi entropy in a phase-space representation for either fermions or bosons. This can also be used to calculate purity and fidelity, or the entanglement between two systems. We show that it is possible to calculate the entropy from sampled phase-space distributions in normally ordered representations, although this is not possible for all quantum states. We give an example of the use of this method in an exactly soluble thermal case. The quantum entropy cannot be calculated at all using sampling methods in classical symmetric (Wigner) or antinormally ordered (Husimi) phase spaces, due to inner-product divergences. The preferred method is to use generalized Gaussian phase-space methods, which utilize a distribution over stochastic Green's functions. We illustrate this approach by calculating the reduced entropy and entanglement of bosonic or fermionic modes coupled to a time-evolving, non-Markovian reservoir.

Computing pKa Values with a Mixing Hamiltonian Quantum Mechanical/Molecular Mechanical Approach.

Science.gov (United States)

Liu, Yang; Fan, Xiaoli; Jin, Yingdi; Hu, Xiangqian; Hu, Hao

2013-09-10

Accurate computation of the pKa value of a compound in solution is important but challenging. Here, a new mixing quantum mechanical/molecular mechanical (QM/MM) Hamiltonian method is developed to simulate the free-energy change associated with the protonation/deprotonation processes in solution. The mixing Hamiltonian method is designed for efficient quantum mechanical free-energy simulations by alchemically varying the nuclear potential, i.e., the nuclear charge of the transforming nucleus. In pKa calculation, the charge on the proton is varied in fraction between 0 and 1, corresponding to the fully deprotonated and protonated states, respectively. Inspired by the mixing potential QM/MM free energy simulation method developed previously [H. Hu and W. T. Yang, J. Chem. Phys. 2005, 123, 041102], this method succeeds many advantages of a large class of λ-coupled free-energy simulation methods and the linear combination of atomic potential approach. Theory and technique details of this method, along with the calculation results of the pKa of methanol and methanethiol molecules in aqueous solution, are reported. The results show satisfactory agreement with the experimental data.

arXiv Axion-photon conversion caused by dielectric interfaces: quantum field calculation

CERN Document Server

Ioannisian, Ara N.; Millar, Alexander J.; Raffelt, Georg G.

2017-09-05

Axion-photon conversion at dielectric interfaces, immersed in a near-homogeneous magnetic field, is the basis for the dielectric haloscope method to search for axion dark matter. In analogy to transition radiation, this process is possible because the photon wave function is modified by the dielectric layers ("Garibian wave function") and is no longer an eigenstate of momentum. A conventional first-order perturbative calculation of the transition probability between a quantized axion state and these distorted photon states provides the microwave production rate. It agrees with previous results based on solving the classical Maxwell equations for the combined system of axions and electromagnetic fields. We argue that in general the average photon production rate is given by our result, independently of the detailed quantum state of the axion field. Moreover, our result provides a new perspective on axion-photon conversion in dielectric haloscopes because the rate is based on an overlap integral between unpertu...

Accurate calculation of superdeformed bands in Hg and Pb

International Nuclear Information System (INIS)

Lei Yian; Zeng Jinyan

1993-01-01

The superdeformed (SD) rotational bands in Hg and Pb are analyzed by means of the abc expression for rotational bands, which was derived from the Bohr Hamiltonian. The agreement between calculated and observed transition energies is incredibly well. The deviation of the calculated E' γ s from the observed results turns out to be absolute value δ ≤0.5 keV (except for a few cases, 0.5 kev ≤ absolute value δ ≤ 0.7 keV). Some transitions which have not been observed yet in these SD bands are also predicted, which may be useful for experimental investigation

First-principles engineering of charged defects for two-dimensional quantum technologies

Science.gov (United States)

Wu, Feng; Galatas, Andrew; Sundararaman, Ravishankar; Rocca, Dario; Ping, Yuan

2017-12-01

Charged defects in two-dimensional (2D) materials have emerging applications in quantum technologies such as quantum emitters and quantum computation. The advancement of these technologies requires a rational design of ideal defect centers, demanding reliable computation methods for the quantitatively accurate prediction of defect properties. We present an accurate, parameter-free, and efficient procedure to evaluate the quasiparticle defect states and thermodynamic charge transition levels of defects in 2D materials. Importantly, we solve critical issues that stem from the strongly anisotropic screening in 2D materials, that have so far precluded the accurate prediction of charge transition levels in these materials. Using this procedure, we investigate various defects in monolayer hexagonal boron nitride (h -BN ) for their charge transition levels, stable spin states, and optical excitations. We identify CBVN (nitrogen vacancy adjacent to carbon substitution of boron) to be the most promising defect candidate for scalable quantum bit and emitter applications.

Quantum correlator outside a Schwarzschild black hole

Directory of Open Access Journals (Sweden)

Claudia Buss

2018-01-01

Full Text Available We calculate the quantum correlator in Schwarzschild black hole space–time. We perform the calculation for a scalar field in three different quantum states: Boulware, Unruh and Hartle–Hawking, and for points along a timelike circular geodesic. The results show that the correlator presents a global fourfold singularity structure, which is state-independent. Our results also show the different correlations in the three different quantum states arising in-between the singularities.

Photodissociation of ultracold diatomic strontium molecules with quantum state control.

Science.gov (United States)

McDonald, M; McGuyer, B H; Apfelbeck, F; Lee, C-H; Majewska, I; Moszynski, R; Zelevinsky, T

2016-07-07

Chemical reactions at ultracold temperatures are expected to be dominated by quantum mechanical effects. Although progress towards ultracold chemistry has been made through atomic photoassociation, Feshbach resonances and bimolecular collisions, these approaches have been limited by imperfect quantum state selectivity. In particular, attaining complete control of the ground or excited continuum quantum states has remained a challenge. Here we achieve this control using photodissociation, an approach that encodes a wealth of information in the angular distribution of outgoing fragments. By photodissociating ultracold (88)Sr2 molecules with full control of the low-energy continuum, we access the quantum regime of ultracold chemistry, observing resonant and nonresonant barrier tunnelling, matter-wave interference of reaction products and forbidden reaction pathways. Our results illustrate the failure of the traditional quasiclassical model of photodissociation and instead are accurately described by a quantum mechanical model. The experimental ability to produce well-defined quantum continuum states at low energies will enable high-precision studies of long-range molecular potentials for which accurate quantum chemistry models are unavailable, and may serve as a source of entangled states and coherent matter waves for a wide range of experiments in quantum optics.

Quantum game theory

Science.gov (United States)

Stohler, Michael Lehman

2002-01-01

Non-cooperative quantum games have received much attention recently. This thesis defines and divides current works into two major categories of gaming techniques with close attention paid to Nash equilibria, form and possibilities for the payoff functions, and the benefits of using a quantum strategy. In addition to comparing and contrasting these techniques, new applications and calculations are discussed. Finally, the techniques are expanded into 3 x 3 games which allows the study of non-transitive strategies in quantum games.

Quantum Computing's Classical Problem, Classical Computing's Quantum Problem

OpenAIRE

Van Meter, Rodney

2013-01-01

Tasked with the challenge to build better and better computers, quantum computing and classical computing face the same conundrum: the success of classical computing systems. Small quantum computing systems have been demonstrated, and intermediate-scale systems are on the horizon, capable of calculating numeric results or simulating physical systems far beyond what humans can do by hand. However, to be commercially viable, they must surpass what our wildly successful, highly advanced classica...

Energy Dissipation in Quantum Computers

OpenAIRE

Granik, A.; Chapline, G.

2003-01-01

A method is described for calculating the heat generated in a quantum computer due to loss of quantum phase information. Amazingly enough, this heat generation can take place at zero temperature. and may explain why it is impossible to extract energy from vacuum fluctuations. Implications for optical computers and quantum cosmology are also briefly discussed.

Large-scale calculations of solid oxide fuel cell cermet anode by tight-binding quantum chemistry method

International Nuclear Information System (INIS)

Koyama, Michihisa; Kubo, Momoji; Miyamoto, Akira

2005-01-01

Improvement of anode characteristics of solid oxide fuel cells is important for the better cell performance and especially the direct use of hydrocarbons. A mixture of ceramics and metal is generally used as anode, and different combinations of ceramics and metals lead to different electrode characteristics. We performed large-scale calculations to investigate the characteristics of Ni/CeO 2 and Cu/CeO 2 anodes at the electronic level using our tight-binding quantum chemical molecular dynamics program. Charge distribution analysis clarified the electron transfer from metal to oxide in both anodes. The calculations of density of states clarified different contributions of Ni and Cu orbitals to the energy levels at around Fermi level in each cermet. Based on the obtained results, we made considerations to explain different characteristics of both cermet anodes. The effectiveness of our approach for the investigation of complex cermet system was proved

Universal fault-tolerant adiabatic quantum computing with quantum dots or donors

Science.gov (United States)

Landahl, Andrew

I will present a conceptual design for an adiabatic quantum computer that can achieve arbitrarily accurate universal fault-tolerant quantum computations with a constant energy gap and nearest-neighbor interactions. This machine can run any quantum algorithm known today or discovered in the future, in principle. The key theoretical idea is adiabatic deformation of degenerate ground spaces formed by topological quantum error-correcting codes. An open problem with the design is making the four-body interactions and measurements it uses more technologically accessible. I will present some partial solutions, including one in which interactions between quantum dots or donors in a two-dimensional array can emulate the desired interactions in second-order perturbation theory. I will conclude with some open problems, including the challenge of reformulating Kitaev's gadget perturbation theory technique so that it preserves fault tolerance. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.

Quantum chemical calculations and spectroscopic measurements of spectroscopic and thermodynamic properties of given uranyl complexes in aqueous solutions with possible environmental and industrial applications

Directory of Open Access Journals (Sweden)

Višňak Jakub

2016-01-01

Full Text Available A brief introduction into computational methodology and preliminary results for spectroscopic (excitation energies, vibrational frequencies in ground and excited electronic states and thermodynamic (stability constants, standard enthalpies and entropies of complexation reactions properties of some 1:1, 1:2 and 1:3 uranyl sulphato- and selenato- complexes in aqueos solutions will be given. The relativistic effects are included via Effective Core Potential (ECP, electron correlation via (TDDFT/B3LYP (dispersion interaction corrected and solvation is described via explicit inclusion of one hydration sphere beyond the coordinated water molecules. We acknowledge limits of this approximate description – more accurate calculations (ranging from semi-phenomenological two-component spin-orbit coupling up to four-component Dirac-Coulomb-Breit hamiltonian and Molecular Dynamics simulations are in preparation. The computational results are compared with the experimental results from Time-resolved Laser-induced Fluorescence Spectroscopy (TRLFS and UV-VIS spectroscopic studies (including our original experimental research on this topic. In case of the TRLFS and UV-VIS speciation studies, the problem of complex solution spectra decomposition into individual components is ill-conditioned and hints from theoretical chemistry could be very important. Qualitative agreement between our quantum chemical calculations of the spectroscopic properties and experimental data was achieved. Possible applications for geochemical modelling (e.g. safety studies of nuclear waste repositories, modelling of a future mining site and analytical chemical studies (including natural samples are discussed.

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

Science.gov (United States)

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.

Quantum mechanical calculation of aqueuous uranium complexes: carbonate, phosphate, organic and biomolecular species

Directory of Open Access Journals (Sweden)

Jha Prashant

2009-08-01

Full Text Available Abstract Background Quantum mechanical calculations were performed on a variety of uranium species representing U(VI, U(V, U(IV, U-carbonates, U-phosphates, U-oxalates, U-catecholates, U-phosphodiesters, U-phosphorylated N-acetyl-glucosamine (NAG, and U-2-Keto-3-doxyoctanoate (KDO with explicit solvation by H2O molecules. These models represent major U species in natural waters and complexes on bacterial surfaces. The model results are compared to observed EXAFS, IR, Raman and NMR spectra. Results Agreement between experiment and theory is acceptable in most cases, and the reasons for discrepancies are discussed. Calculated Gibbs free energies are used to constrain which configurations are most likely to be stable under circumneutral pH conditions. Reduction of U(VI to U(IV is examined for the U-carbonate and U-catechol complexes. Conclusion Results on the potential energy differences between U(V- and U(IV-carbonate complexes suggest that the cause of slower disproportionation in this system is electrostatic repulsion between UO2 [CO3]35- ions that must approach one another to form U(VI and U(IV rather than a change in thermodynamic stability. Calculations on U-catechol species are consistent with the observation that UO22+ can oxidize catechol and form quinone-like species. In addition, outer-sphere complexation is predicted to be the most stable for U-catechol interactions based on calculated energies and comparison to 13C NMR spectra. Outer-sphere complexes (i.e., ion pairs bridged by water molecules are predicted to be comparable in Gibbs free energy to inner-sphere complexes for a model carboxylic acid. Complexation of uranyl to phosphorus-containing groups in extracellular polymeric substances is predicted to favor phosphonate groups, such as that found in phosphorylated NAG, rather than phosphodiesters, such as those in nucleic acids.

Parametrization of Combined Quantum Mechanical and Molecular Mechanical Methods: Bond-Tuned Link Atoms

Directory of Open Access Journals (Sweden)

Xin-Ping Wu

2018-05-01

Full Text Available Combined quantum mechanical and molecular mechanical (QM/MM methods are the most powerful available methods for high-level treatments of subsystems of very large systems. The treatment of the QM−MM boundary strongly affects the accuracy of QM/MM calculations. For QM/MM calculations having covalent bonds cut by the QM−MM boundary, it has been proposed previously to use a scheme with system-specific tuned fluorine link atoms. Here, we propose a broadly parametrized scheme where the parameters of the tuned F link atoms depend only on the type of bond being cut. In the proposed new scheme, the F link atom is tuned for systems with a certain type of cut bond at the QM−MM boundary instead of for a specific target system, and the resulting link atoms are call bond-tuned link atoms. In principle, the bond-tuned link atoms can be as convenient as the popular H link atoms, and they are especially well adapted for high-throughput and accurate QM/MM calculations. Here, we present the parameters for several kinds of cut bonds along with a set of validation calculations that confirm that the proposed bond-tuned link-atom scheme can be as accurate as the system-specific tuned F link-atom scheme.

Parametrization of Combined Quantum Mechanical and Molecular Mechanical Methods: Bond-Tuned Link Atoms.

Science.gov (United States)

Wu, Xin-Ping; Gagliardi, Laura; Truhlar, Donald G

2018-05-30

Combined quantum mechanical and molecular mechanical (QM/MM) methods are the most powerful available methods for high-level treatments of subsystems of very large systems. The treatment of the QM-MM boundary strongly affects the accuracy of QM/MM calculations. For QM/MM calculations having covalent bonds cut by the QM-MM boundary, it has been proposed previously to use a scheme with system-specific tuned fluorine link atoms. Here, we propose a broadly parametrized scheme where the parameters of the tuned F link atoms depend only on the type of bond being cut. In the proposed new scheme, the F link atom is tuned for systems with a certain type of cut bond at the QM-MM boundary instead of for a specific target system, and the resulting link atoms are call bond-tuned link atoms. In principle, the bond-tuned link atoms can be as convenient as the popular H link atoms, and they are especially well adapted for high-throughput and accurate QM/MM calculations. Here, we present the parameters for several kinds of cut bonds along with a set of validation calculations that confirm that the proposed bond-tuned link-atom scheme can be as accurate as the system-specific tuned F link-atom scheme.

Short-time quantum propagator and Bohmian trajectories

Science.gov (United States)

de Gosson, Maurice; Hiley, Basil

2013-12-01

We begin by giving correct expressions for the short-time action following the work Makri-Miller. We use these estimates to derive an accurate expression modulo Δt2 for the quantum propagator and we show that the quantum potential is negligible modulo Δt2 for a point source, thus justifying an unfortunately largely ignored observation of Holland made twenty years ago. We finally prove that this implies that the quantum motion is classical for very short times.

Short-time quantum propagator and Bohmian trajectories

International Nuclear Information System (INIS)

Gosson, Maurice de; Hiley, Basil

2013-01-01

We begin by giving correct expressions for the short-time action following the work Makri–Miller. We use these estimates to derive an accurate expression modulo Δt 2 for the quantum propagator and we show that the quantum potential is negligible modulo Δt 2 for a point source, thus justifying an unfortunately largely ignored observation of Holland made twenty years ago. We finally prove that this implies that the quantum motion is classical for very short times.

Universality of quantum gravity corrections.

Science.gov (United States)

Das, Saurya; Vagenas, Elias C

2008-11-28

We show that the existence of a minimum measurable length and the related generalized uncertainty principle (GUP), predicted by theories of quantum gravity, influence all quantum Hamiltonians. Thus, they predict quantum gravity corrections to various quantum phenomena. We compute such corrections to the Lamb shift, the Landau levels, and the tunneling current in a scanning tunneling microscope. We show that these corrections can be interpreted in two ways: (a) either that they are exceedingly small, beyond the reach of current experiments, or (b) that they predict upper bounds on the quantum gravity parameter in the GUP, compatible with experiments at the electroweak scale. Thus, more accurate measurements in the future should either be able to test these predictions, or further tighten the above bounds and predict an intermediate length scale between the electroweak and the Planck scale.

Digital Quantum Estimation

Science.gov (United States)

Hassani, Majid; Macchiavello, Chiara; Maccone, Lorenzo

2017-11-01

Quantum metrology calculates the ultimate precision of all estimation strategies, measuring what is their root-mean-square error (RMSE) and their Fisher information. Here, instead, we ask how many bits of the parameter we can recover; namely, we derive an information-theoretic quantum metrology. In this setting, we redefine "Heisenberg bound" and "standard quantum limit" (the usual benchmarks in the quantum estimation theory) and show that the former can be attained only by sequential strategies or parallel strategies that employ entanglement among probes, whereas parallel-separable strategies are limited by the latter. We highlight the differences between this setting and the RMSE-based one.

Specific heat in diluted magnetic semiconductor quantum ring

Science.gov (United States)

Babanlı, A. M.; Ibragimov, B. G.

2017-11-01

In the present paper, we have calculated the specific heat and magnetization of a quantum ring of a diluted magnetic semiconductor (DMS) material in the presence of magnetic field. We take into account the effect of Rashba spin-orbital interaction, the exchange interaction and the Zeeman term on the specific heat. We have calculated the energy spectrum of the electrons in diluted magnetic semiconductor quantum ring. Moreover we have calculated the specific heat dependency on the magnetic field and Mn concentration at finite temperature of a diluted magnetic semiconductor quantum ring.

The CPA Equation of State and an Activity Coefficient Model for Accurate Molar Enthalpy Calculations of Mixtures with Carbon Dioxide and Water/Brine

Energy Technology Data Exchange (ETDEWEB)

Myint, P. C. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Hao, Y. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Firoozabadi, A. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

2015-03-27

Thermodynamic property calculations of mixtures containing carbon dioxide (CO₂) and water, including brines, are essential in theoretical models of many natural and industrial processes. The properties of greatest practical interest are density, solubility, and enthalpy. Many models for density and solubility calculations have been presented in the literature, but there exists only one study, by Spycher and Pruess, that has compared theoretical molar enthalpy predictions with experimental data [1]. In this report, we recommend two different models for enthalpy calculations: the CPA equation of state by Li and Firoozabadi [2], and the CO₂ activity coefficient model by Duan and Sun [3]. We show that the CPA equation of state, which has been demonstrated to provide good agreement with density and solubility data, also accurately calculates molar enthalpies of pure CO₂, pure water, and both CO₂-rich and aqueous (H₂O-rich) mixtures of the two species. It is applicable to a wider range of conditions than the Spycher and Pruess model. In aqueous sodium chloride (NaCl) mixtures, we show that Duan and Sun’s model yields accurate results for the partial molar enthalpy of CO₂. It can be combined with another model for the brine enthalpy to calculate the molar enthalpy of H₂O-CO₂-NaCl mixtures. We conclude by explaining how the CPA equation of state may be modified to further improve agreement with experiments. This generalized CPA is the basis of our future work on this topic.

Studies of quantum dots in the quantum Hall regime

Science.gov (United States)

Goldmann, Eyal

We present two studies of quantum dots in the quantum Hall regime. In the first study, presented in Chapter 3, we investigate the edge reconstruction phenomenon believed to occur when the quantum dot filling fraction is n≲1 . Our approach involves the examination of large dots (≤40 electrons) using a partial diagonalization technique in which the occupancies of the deep interior orbitals are frozen. To interpret the results of this calculation, we evaluate the overlap between the diagonalized ground state and a set of trial wavefunctions which we call projected necklace (PN) states. A PN state is simply the angular momentum projection of a maximum density droplet surrounded by a ring of localized electrons. Our calculations reveal that PN states have up to 99% overlap with the diagonalized ground states, and are lower in energy than the states identified in Chamon and Wen's study of the edge reconstruction. In the second study, presented in Chapter 4, we investigate quantum dots in the fractional quantum Hall regime using a Hartree formulation of composite fermion theory. We find that under appropriate conditions, the chemical potential of the dots oscillates periodically with B due to the transfer of composite fermions between quasi-Landau bands. This effect is analogous the addition spectrum oscillations which occur in quantum dots in the integer quantum Hall regime. Period f0 oscillations are found in sharply confined dots with filling factors nu = 2/5 and nu = 2/3. Period 3 f0 oscillations are found in a parabolically confined nu = 2/5 dot. More generally, we argue that the oscillation period of dots with band pinning should vary continuously with B, whereas the period of dots without band pinning is f0 .

Rotational Spectrum, Conformational Composition, and Quantum Chemical Calculations of Cyanomethyl Formate (HC(O)OCH2C≡N), a Compound of Potential Astrochemical Interest.

Science.gov (United States)

Samdal, Svein; Møllendal, Harald; Carles, Sophie

2015-08-27

The rotational spectrum of cyanomethyl formate (HC(O)OCH2C≡N) has been recorded in the 12–123 GHz spectral range. The spectra of two conformers were assigned. The rotamer denoted I has a symmetry plane and two out-of plane hydrogen atoms belonging to the cyanomethyl (CH2CN) moiety. In the conformer called II, the cyanomethyl group is rotated 80.3° out of this plane. Conformer I has an energy that is 1.4(6) kJ/mol lower than the energy of II according to relative intensity measurements. A large number of rotational transitions have been assigned for the ground and vibrationally excited states of the two conformers and accurate spectroscopic constants have been obtained. These constants should predict frequencies of transitions outside the investigated spectral range with a very high degree of precision. It is suggested that cyanomethyl formate is a potential interstellar compound. This suggestion is based on the fact that its congener methyl formate (HC(O)OCH3) exists across a large variety of interstellar environments and the fact that cyanides are very prevalent in the Universe. The experimental work has been augmented by high-level quantum chemical calculations. The CCSD/cc-pVQZ calculations are found to predict structures of the two forms that are very close to the Born–Oppenheimer equilibrium structures. MP2/cc-pVTZ predictions of several vibration–rotation interaction constants were generally found to be rather inaccurate. A gas-phase reaction between methyl formate and the cyanomethyl radical CH2CN to produce a hydrogen atom and cyanomethyl formate was mimicked using MP2/cc-pVTZ calculations. It was found that this reaction is not favored thermodynamically. It is also conjectured that the possible formation of cyanomethyl formate might be catalyzed and take place on interstellar particles.

Lectures on Quantum Mechanics

CERN Document Server

Dirac, Paul Adrien Maurice

1964-01-01

The author of this concise, brilliant series of lectures on mathematical methods in quantum mechanics was one of the shining intellects in the field, winning a Nobel prize in 1933 for his pioneering work in the quantum mechanics of the atom. Beyond that, he developed the transformation theory of quantum mechanics (which made it possible to calculate the statistical distribution of certain variables), was one of the major authors of the quantum theory of radiation, codiscovered the Fermi-Dirac statistics, and predicted the existence of the positron.The four lectures in this book were delivered

Chern-Simons expectation values and quantum horizons from loop quantum gravity and the Duflo map.

Science.gov (United States)

Sahlmann, Hanno; Thiemann, Thomas

2012-03-16

We report on a new approach to the calculation of Chern-Simons theory expectation values, using the mathematical underpinnings of loop quantum gravity, as well as the Duflo map, a quantization map for functions on Lie algebras. These new developments can be used in the quantum theory for certain types of black hole horizons, and they may offer new insights for loop quantum gravity, Chern-Simons theory and the theory of quantum groups.

On the calculation of quantum mechanical ground states from classical geodesic motion on certain spaces of constant negative curvature

International Nuclear Information System (INIS)

Tomaschitz, R.

1989-01-01

We consider geodesic motion on three-dimensional Riemannian manifolds of constant negative curvature, topologically equivalent to S x ]0,1[, S a compact surface of genus two. To those trajectories which are recurrent in both directions of the time evolution t → +∞, t → -∞ a fractal limit set is associated whose Hausdorff dimension is intimately connected with the quantum mechanical energy ground state, determined by the Schroedinger operator on the manifold. We give a rather detailed and pictorial description of the hyperbolic spaces we have in mind, discuss various aspects of classical and quantum mechanical motion on them as far as they are needed to establish the connection between energy ground state and Hausdorff dimension and give finally some examples of ground state calculations in terms of Hausdorff dimensions of limit sets of classical trajectories. (orig.)

Dynamical coupling of plasmons and molecular excitations by hybrid quantum/classical calculations: time-domain approach

International Nuclear Information System (INIS)

Sakko, Arto; Rossi, Tuomas P; Nieminen, Risto M

2014-01-01

The presence of plasmonic material influences the optical properties of nearby molecules in untrivial ways due to the dynamical plasmon-molecule coupling. We combine quantum and classical calculation schemes to study this phenomenon in a hybrid system that consists of a Na 2 molecule located in the gap between two Au/Ag nanoparticles. The molecule is treated quantum-mechanically with time-dependent density-functional theory, and the nanoparticles with quasistatic classical electrodynamics. The nanoparticle dimer has a plasmon resonance in the visible part of the electromagnetic spectrum, and the Na 2 molecule has an electron-hole excitation in the same energy range. Due to the dynamical interaction of the two subsystems the plasmon and the molecular excitations couple, creating a hybridized molecular-plasmon excited state. This state has unique properties that yield e.g. enhanced photoabsorption compared to the freestanding Na 2 molecule. The computational approach used enables decoupling of the mutual plasmon-molecule interaction, and our analysis verifies that it is not legitimate to neglect the backcoupling effect when describing the dynamical interaction between plasmonic material and nearby molecules. Time-resolved analysis shows nearly instantaneous formation of the coupled state, and provides an intuitive picture of the underlying physics. (paper)

Towards a feasible implementation of quantum neural networks using quantum dots

International Nuclear Information System (INIS)

Altaisky, Mikhail V.; Zolnikova, Nadezhda N.; Kaputkina, Natalia E.; Krylov, Victor A.; Lozovik, Yurii E.; Dattani, Nikesh S.

2016-01-01

We propose an implementation of quantum neural networks using an array of quantum dots with dipole-dipole interactions. We demonstrate that this implementation is both feasible and versatile by studying it within the framework of GaAs based quantum dot qubits coupled to a reservoir of acoustic phonons. Using numerically exact Feynman integral calculations, we have found that the quantum coherence in our neural networks survive for over a hundred ps even at liquid nitrogen temperatures (77 K), which is three orders of magnitude higher than current implementations, which are based on SQUID-based systems operating at temperatures in the mK range.

Analytical scheme calculations of angular momentum coupling and recoupling coefficients

Science.gov (United States)

Deveikis, A.; Kuznecovas, A.

2007-03-01

We investigate the Scheme programming language opportunities to analytically calculate the Clebsch-Gordan coefficients, Wigner 6j and 9j symbols, and general recoupling coefficients that are used in the quantum theory of angular momentum. The considered coefficients are calculated by a direct evaluation of the sum formulas. The calculation results for large values of quantum angular momenta were compared with analogous calculations with FORTRAN and Java programming languages.

Analytical scheme calculations of angular momentum coupling and recoupling coefficients

International Nuclear Information System (INIS)

Deveikis, A.; Kuznecovas, A.

2007-01-01

We investigate the Scheme programming language opportunities to analytically calculate the Clebsch-Gordan coefficients, Wigner 6j and 9j symbols, and general recoupling coefficients that are used in the quantum theory of angular momentum. The considered coefficients are calculated by a direct evaluation of the sum formulas. The calculation results for large values of quantum angular momenta were compared with analogous calculations with FORTRAN and Java programming languages

Quantum information with Gaussian states

International Nuclear Information System (INIS)

Wang Xiangbin; Hiroshima, Tohya; Tomita, Akihisa; Hayashi, Masahito

2007-01-01

Quantum optical Gaussian states are a type of important robust quantum states which are manipulatable by the existing technologies. So far, most of the important quantum information experiments are done with such states, including bright Gaussian light and weak Gaussian light. Extending the existing results of quantum information with discrete quantum states to the case of continuous variable quantum states is an interesting theoretical job. The quantum Gaussian states play a central role in such a case. We review the properties and applications of Gaussian states in quantum information with emphasis on the fundamental concepts, the calculation techniques and the effects of imperfections of the real-life experimental setups. Topics here include the elementary properties of Gaussian states and relevant quantum information device, entanglement-based quantum tasks such as quantum teleportation, quantum cryptography with weak and strong Gaussian states and the quantum channel capacity, mathematical theory of quantum entanglement and state estimation for Gaussian states

Measurement-Device Independency Analysis of Continuous-Variable Quantum Digital Signature

Directory of Open Access Journals (Sweden)

Tao Shang

2018-04-01

Full Text Available With the practical implementation of continuous-variable quantum cryptographic protocols, security problems resulting from measurement-device loopholes are being given increasing attention. At present, research on measurement-device independency analysis is limited in quantum key distribution protocols, while there exist different security problems for different protocols. Considering the importance of quantum digital signature in quantum cryptography, in this paper, we attempt to analyze the measurement-device independency of continuous-variable quantum digital signature, especially continuous-variable quantum homomorphic signature. Firstly, we calculate the upper bound of the error rate of a protocol. If it is negligible on condition that all measurement devices are untrusted, the protocol is deemed to be measurement-device-independent. Then, we simplify the calculation by using the characteristics of continuous variables and prove the measurement-device independency of the protocol according to the calculation result. In addition, the proposed analysis method can be extended to other quantum cryptographic protocols besides continuous-variable quantum homomorphic signature.

Controlling the Shannon Entropy of Quantum Systems

Science.gov (United States)

Xing, Yifan; Wu, Jun

2013-01-01

This paper proposes a new quantum control method which controls the Shannon entropy of quantum systems. For both discrete and continuous entropies, controller design methods are proposed based on probability density function control, which can drive the quantum state to any target state. To drive the entropy to any target at any prespecified time, another discretization method is proposed for the discrete entropy case, and the conditions under which the entropy can be increased or decreased are discussed. Simulations are done on both two- and three-dimensional quantum systems, where division and prediction are used to achieve more accurate tracking. PMID:23818819

Controlling the Shannon Entropy of Quantum Systems

Directory of Open Access Journals (Sweden)

Yifan Xing

2013-01-01

Full Text Available This paper proposes a new quantum control method which controls the Shannon entropy of quantum systems. For both discrete and continuous entropies, controller design methods are proposed based on probability density function control, which can drive the quantum state to any target state. To drive the entropy to any target at any prespecified time, another discretization method is proposed for the discrete entropy case, and the conditions under which the entropy can be increased or decreased are discussed. Simulations are done on both two- and three-dimensional quantum systems, where division and prediction are used to achieve more accurate tracking.

Phase stability of TiO2 polymorphs from diffusion Quantum Monte Carlo

International Nuclear Information System (INIS)

Luo, Ye; Benali, Anouar; Shulenburger, Luke; Krogel, Jaron T; Heinonen, Olle; Kent, Paul R C

2016-01-01

Titanium dioxide, TiO 2 , has multiple applications in catalysis, energy conversion and memristive devices because of its electronic structure. Most of these applications utilize the naturally existing phases: rutile, anatase and brookite. Despite the simple form of TiO 2 and its wide uses, there is long-standing disagreement between theory and experiment on the energetic ordering of these phases that has never been resolved. We present the first analysis of phase stability at zero temperature using the highly accurate many-body fixed node diffusion Quantum Monte Carlo (QMC) method. We also include the effects of temperature by calculating the Helmholtz free energy including both internal energy and vibrational contributions from density functional perturbation theory based quasi harmonic phonon calculations. Our QMC calculations find that anatase is the most stable phase at zero temperature, consistent with many previous mean-field calculations. However, at elevated temperatures, rutile becomes the most stable phase. For all finite temperatures, brookite is always the least stable phase. (paper)

Reaction Mechanism of Mycobacterium Tuberculosis Glutamine Synthetase Using Quantum Mechanics/Molecular Mechanics Calculations.

Science.gov (United States)

Moreira, Cátia; Ramos, Maria J; Fernandes, Pedro Alexandrino

2016-06-27

This paper is devoted to the understanding of the reaction mechanism of mycobacterium tuberculosis glutamine synthetase (mtGS) with atomic detail, using computational quantum mechanics/molecular mechanics (QM/MM) methods at the ONIOM M06-D3/6-311++G(2d,2p):ff99SB//B3LYP/6-31G(d):ff99SB level of theory. The complete reaction undergoes a three-step mechanism: the spontaneous transfer of phosphate from ATP to glutamate upon ammonium binding (ammonium quickly loses a proton to Asp54), the attack of ammonia on phosphorylated glutamate (yielding protonated glutamine), and the deprotonation of glutamine by the leaving phosphate. This exothermic reaction has an activation free energy of 21.5 kcal mol(-1) , which is consistent with that described for Escherichia coli glutamine synthetase (15-17 kcal mol(-1) ). The participating active site residues have been identified and their role and energy contributions clarified. This study provides an insightful atomic description of the biosynthetic reaction that takes place in this enzyme, opening doors for more accurate studies for developing new anti-tuberculosis therapies. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Quantum mechanics and precision measurements

International Nuclear Information System (INIS)

Ramsey, N.F.

1995-01-01

The accuracies of measurements of almost all fundamental physical constants have increased by factors of about 10000 during the past 60 years. Although some of the improvements are due to greater care, most are due to new techniques based on quantum mechanics. Although the Heisenberg Uncertainty Principle often limits measurement accuracies, in many cases the validity of quantum mechanics makes possible the vastly improved measurement accuracies. Seven quantum features that have a profound influence on the science of measurements are: 1) Existence of discrete quantum states of energy. 2) Energy conservation in transitions between two states. 3) Electromagnetic radiation of frequency v is quantized with energy hv per quantum. 4) The identity principle. 5) The Heisenberg Uncertainty Principle. 6) Addition of probability amplitudes (not probabilities). 7) Wave and coherent phase phenomena. Of these seven quantum features, only the Heisenberg Uncertainty Principle limits the accuracy of measurements, and its effect is often negligibly small. The other six features make possible much more accurate measurements of quantum systems than with almost all classical systems. These effects are discussed and illustrated