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Sample records for quantum dynamics calculations

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

    SciTech Connect

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

    2008-03-28

    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.

  2. Accelerating calculations of ultrafast time-resolved electronic spectra with efficient quantum dynamics methods.

    PubMed

    Wehrle, Marius; Sulc, Miroslav; Vanícek, Jirí

    2011-01-01

    We explore three specific approaches for speeding up the calculation of quantum time correlation functions needed for time-resolved electronic spectra. The first relies on finding a minimum set of sufficiently accurate electronic surfaces. The second increases the time step required for convergence of exact quantum simulations by using different split-step algorithms to solve the time-dependent Schrödinger equation. The third approach lowers the number of trajectories needed for convergence of approximate semiclassical dynamics methods.

  3. Equation of State of Al Based on Quantum Molecular Dynamics Calculations

    NASA Astrophysics Data System (ADS)

    Minakov, Dmitry V.; Levashov, Pavel R.; Khishchenko, Konstantin V.

    2011-06-01

    In this work, we present quantum molecular dynamics calculations of the shock Hugoniots of solid and porous samples as well as release isentropes and values of isentropic sound velocity behind the shock front for aluminum. We use the VASP code with an ultrasoft pseudopotential and GGA exchange-correlation functional. Up to 108 particles have been used in calculations. For the Hugoniots of Al we solve the Hugoniot equation numerically. To calculate release isentropes, we use Zel'dovich's approach and integrate an ordinary differential equation for the temperature thus restoring all thermodynamic parameters. Isentropic sound velocity is calculated by differentiation along isentropes. The results of our calculations are in good agreement with experimental data. Thus, quantum molecular dynamics results can be effectively used for verification or calibration of semiempirical equations of state under conditions of lack of experimental information at high energy densities. This work is supported by RFBR, grants 09-08-01129 and 11-08-01225.

  4. Phenol-benzene complexation dynamics: quantum chemistry calculation, molecular dynamics simulations, and two dimensional IR spectroscopy.

    PubMed

    Kwac, Kijeong; Lee, Chewook; Jung, Yousung; Han, Jaebeom; Kwak, Kyungwon; Zheng, Junrong; Fayer, M D; Cho, Minhaeng

    2006-12-28

    Molecular dynamics (MD) simulations and quantum mechanical electronic structure calculations are used to investigate the nature and dynamics of the phenol-benzene complex in the mixed solvent, benzene/CCl4. Under thermal equilibrium conditions, the complexes are continuously dissociating and forming. The MD simulations are used to calculate the experimental observables related to the phenol hydroxyl stretching mode, i.e., the two dimensional infrared vibrational echo spectrum as a function of time, which directly displays the formation and dissociation of the complex through the growth of off-diagonal peaks, and the linear absorption spectrum, which displays two hydroxyl stretch peaks, one for the complex and one for the free phenol. The results of the simulations are compared to previously reported experimental data and are found to be in quite reasonable agreement. The electronic structure calculations show that the complex is T shaped. The classical potential used for the phenol-benzene interaction in the MD simulations is in good accord with the highest level of the electronic structure calculations. A variety of other features is extracted from the simulations including the relationship between the structure and the projection of the electric field on the hydroxyl group. The fluctuating electric field is used to determine the hydroxyl stretch frequency-frequency correlation function (FFCF). The simulations are also used to examine the number distribution of benzene and CCl4 molecules in the first solvent shell around the phenol. It is found that the distribution is not that of the solvent mole fraction of benzene. There are substantial probabilities of finding a phenol in either a pure benzene environment or a pure CCl4 environment. A conjecture is made that relates the FFCF to the local number of benzene molecules in phenol's first solvent shell.

  5. Conformational properties of penicillins: quantum chemical calculations and molecular dynamics simulations of benzylpenicillin.

    PubMed

    Díaz, Natalia; Suárez, Dimas; Sordo, Tomás L

    2003-11-30

    Herein, we present theoretical results on the conformational properties of benzylpenicillin, which are characterized by means of quantum chemical calculations (MP2/6-31G* and B3LYP/6-31G*) and classical molecular dynamics simulations (5 ns) both in the gas phase and in aqueous solution. In the gas phase, the benzylpenicillin conformer in which the thiazolidine ring has the carboxylate group oriented axially is the most favored one. Both intramolecular CH. O and dispersion interactions contribute to stabilize the axial conformer with respect to the equatorial one. In aqueous solution, a molecular dynamics simulation predicts a relative population of the axial:equatorial conformers of 0.70:0.30 in consonance with NMR experimental data. Overall, the quantum chemical calculations as well as the simulations give insight into substituent effects, the conformational dynamics of benzylpenicillin, the frequency of ring-puckering motions, and the correlation of side chain and ring-puckering motions.

  6. Shock Hugoniot calculations of polymers using quantum mechanics and molecular dynamics

    NASA Astrophysics Data System (ADS)

    Chantawansri, Tanya L.; Sirk, Timothy W.; Byrd, Edward F. C.; Andzelm, Jan W.; Rice, Betsy M.

    2012-11-01

    Using quantum mechanics (QM) and classical force-field based molecular dynamics (FF), we have calculated the principle shock Hugoniot curves for numerous amorphous polymers including poly[methyl methacrylate] (PMMA), poly[styrene], polycarbonate, as well as both the amorphous and crystalline forms of poly[ethylene]. In the FF calculations, we considered a non-reactive force field (i.e., polymer consistent FF). The QM calculations were performed with density functional theory (DFT) using dispersion corrected atom centered pseudopotentials. Overall, results obtained by DFT show much better agreement with available experimental data than classical force fields. In particular, DFT calculated Hugoniot curves for PMMA up to 74 GPa are in very good agreement with experimental data, where a preliminary study of chain fracture and association was also performed. Structure analysis calculations of the radius of gyration and carbon-carbon radial distribution function were also carried out to elucidate contraction of the polymer chains with increasing pressure.

  7. Diffusion Rates for Hydrogen on Pd(111) from Molecular Quantum Dynamics Calculations.

    PubMed

    Firmino, Thiago; Marquardt, Roberto; Gatti, Fabien; Dong, Wei

    2014-12-18

    The van Hove formula for the dynamical structure factor (DSF) related to particle scattering at mobile adsorbates is extended to include the relaxation of the adsorbates' vibrational states. The total rate obtained from the DSF is assumed to be the sum of a diffusion and a relaxation rate. A simple kinetic model to support this assumption is presented. To illustrate its potential applicability, the formula is evaluated using wave functions, energies, and lifetimes of vibrational states obtained for H/Pd(111) from first-principle calculations. Results show that quantum effects can be expected to be important even at room temperature.

  8. Understanding the Phosphorylation Mechanism by Using Quantum Chemical Calculations and Molecular Dynamics Simulations.

    PubMed

    Han, Weiwei; Zhu, Jingxuan; Wang, Song; Xu, Dong

    2017-04-20

    Phosphorylation is one of the most frequent post-translational modifications on proteins. It regulates many cellular processes by modulation of phosphorylation on protein structure and dynamics. However, the mechanism of phosphorylation-induced conformational changes of proteins is still poorly understood. Here, we report a computational study of three representative groups of tyrosine in ADP-ribosylhydrolase 1, serine in BTG2, and serine in Sp100C by using six molecular dynamics (MD) simulations and quantum chemical calculations. Added phosphorylation was found to disrupt hydrogen bond, and increase new weak interactions (hydrogen bond and hydrophobic interaction) during MD simulations, leading to conformational changes. Quantum chemical calculations further indicate that the phosphorylation on tyrosine, threonine, and serine could decrease the optical band gap energy (Egap), which can trigger electronic transitions to form or disrupt interactions easily. Our results provide an atomic and electronic description of how phosphorylation facilitates conformational and dynamic changes in proteins, which may be useful for studying protein function and protein design.

  9. Toward extending photosynthetic biosignatures: quantum dynamics calculation of light harvesting complexes

    NASA Astrophysics Data System (ADS)

    Komatsu, Yu; Umemura, Masayuki; Shoji, Mitsuo; Kayanuma, Megumi; Yabana, Kazuhiro; Shiraishi, Kenji

    For detecting life from reflectance spectra on extrasolar planets, several indicators called surface biosignatures have been proposed. One of them is the vegetation red edge (VRE) which derives from surface vegetation. VRE is observed in 700-750 nm on the Earth, but there is no guarantee that exovegetation show the red edge in this wavelength. Therefore it is necessary to check the validity of current standards of VRE as the signatures. In facts, M stars (cooler than Sun) will be the main targets in future missions, it is significantly important to know on the fundamental mechanisms in photosynthetic organism such as purple bacteria which absorb longer wavelength radiation. We investigated light absorptions and excitation energy transfers (EETs) in light harvesting complexes in purple bacteria (LH2s) by using quantum dynamics simulations. In LH2, effective EET is accomplished by corporative electronic excitation of the pigments. In our theoretical model, a dipole-dipole approximation was used for the electronic interactions between pigment excitations. Quantum dynamics simulations were performed according to Liouville equation to examine the EET process. The calculated oscillator strength and the transfer time between LH2 were good agreement with the experimental values. As the system size increases, the absorption bands shifted longer and the transfer velocities became larger. When two pigments in a LHC were exchanged to another pigments with lower excitation energy, faster and intensive light collection were observed.

  10. Open Quantum Dynamics Calculations with the Hierarchy Equations of Motion on Parallel Computers.

    PubMed

    Strümpfer, Johan; Schulten, Klaus

    2012-08-14

    Calculating the evolution of an open quantum system, i.e., a system in contact with a thermal environment, has presented a theoretical and computational challenge for many years. With the advent of supercomputers containing large amounts of memory and many processors, the computational challenge posed by the previously intractable theoretical models can now be addressed. The hierarchy equations of motion present one such model and offer a powerful method that remained under-utilized so far due to its considerable computational expense. By exploiting concurrent processing on parallel computers the hierarchy equations of motion can be applied to biological-scale systems. Herein we introduce the quantum dynamics software PHI, that solves the hierarchical equations of motion. We describe the integrator employed by PHI and demonstrate PHI's scaling and efficiency running on large parallel computers by applying the software to the calculation of inter-complex excitation transfer between the light harvesting complexes 1 and 2 of purple photosynthetic bacteria, a 50 pigment system.

  11. A rigorous full-dimensional quantum dynamics calculation of the vibrational energies of H3O2-

    NASA Astrophysics Data System (ADS)

    Yu, Hua-Gen

    2006-11-01

    The vibrational energy levels of the H3O2- anion have been calculated using a rigorous quantum dynamics method based on an accurate ab initio potential energy surface. The eigenvalue problem is solved using the two-layer Lanczos iterative diagonalization algorithm in a mixed grid/nondirect product basis set, where the system Hamiltonian is expressed in a set of orthogonal polyspherical coordinates. The lowest 312 vibrational energy levels in each inversion symmetry, together with a comparison of fundamental frequencies with previous quantum dynamics calculations, are reported. Finally, a statistical analysis of nearest level spacing distribution is carried out, revealing a strongly chaotic nature.

  12. Photodissociation dynamics of the pyridinyl radical: Time-dependent quantum wave-packet calculations

    NASA Astrophysics Data System (ADS)

    Ehrmaier, Johannes; Picconi, David; Karsili, Tolga N. V.; Domcke, Wolfgang

    2017-03-01

    The H-atom photodissociation reaction from the pyridinyl radical (C5H5NH ) via the low-lying π σ* excited electronic state is investigated by nonadiabatic time-dependent quantum wave-packet dynamics calculations. A model comprising three electronic states and three nuclear coordinates has been constructed using ab initio multi-configurational self-consistent-field and multi-reference perturbation theory methods. Two conical intersections among the three lowest electronic states have been characterized in the framework of the linear vibronic-coupling model. Time-dependent wave-packet simulations have been performed using the multi-configuration time-dependent Hartree method. The population dynamics of the diabatic and adiabatic electronic states and the time-dependent dissociation behavior are analyzed for various vibrational initial conditions. The results provide detailed mechanistic insight into the photoinduced H-atom dissociation process from a hypervalent aromatic radical and show that an efficient dissociation reaction through two conical intersections is possible.

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

    SciTech Connect

    Halverson, Thomas; Poirier, Bill

    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).

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

    PubMed

    Halverson, Thomas; Poirier, Bill

    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).

  15. Acceleration of Semiempirical Quantum Mechanical Calculations by Extended Lagrangian Molecular Dynamics Approach.

    PubMed

    Nam, Kwangho

    2013-08-13

    The implementation and performance of the atom-centered density matrix propagation (ADMP) [J. Chem. Phys. 2001, 114, 9758] and the curvy-steps (CURV) methods [J. Chem. Phys. 2004, 121, 1152] are described. These methods solve the electronic Schrödinger equation approximately by propagating the electronic degrees of freedom using the extended Lagrangian molecular dynamics (ELMD) simulation approach. The ADMP and CURV methods are implemented and parallelized to accelerate semiempirical quantum mechanical (QM) methods (such as the MNDO, AM1, PM3, MNDO/d, and AM1/d methods). Test calculations show that both the ADMP and the CURV methods are 2∼4 times faster than the Born-Oppenheimer molecular dynamics (BOMD) method and conserve the total energy well. The accuracy of the ADMP and CURV simulations is comparable to the BOMD simulations. The parallel implementation accelerates the MD simulation by up to 28 fold for the ADMP method and 25 fold for the CURV method, respectively, relative to the speed of the single core BOMD. In addition, a multiple time scale (MTS) approach is introduced to further speed up the semiempirical QM and QM/MM ELMD simulations. Since a larger integration time step is used for the propagation of the nuclear coordinates than that for the electronic degrees of freedom, the MTS approach allows the ELMD simulation to be carried out with a time step that is larger than the time step accessible by the original ADMP and CURV methods. It renders MD simulation to be carried out about 20 times faster than the BOMD simulation, and yields results that are comparable to the single time scale simulation results. The use of the methods introduced in the present work provides an efficient way to extend the length of the QM and QM/MM molecular dynamics simulations beyond the length accessible by BOMD simulation.

  16. A general rigorous quantum dynamics algorithm to calculate vibrational energy levels of pentaatomic molecules

    NASA Astrophysics Data System (ADS)

    Yu, Hua-Gen

    2009-08-01

    An exact variational algorithm is presented for calculating vibrational energy levels of pentaatomic molecules without any dynamical approximation. The quantum mechanical Hamiltonian of the system is expressed in a set of orthogonal coordinates defined by four scattering vectors in the body-fixed frame. The eigenvalue problem is solved using a two-layer Lanczos iterative diagonalization method in a mixed grid/basis set. A direct product potential-optimized discrete variable representation (PO-DVR) basis is used for the radial coordinates while a non-direct product finite basis representation (FBR) is employed for the angular variables. The two-layer Lanczos method requires only the actions of the Hamiltonian operator on the Lanczos vectors, where the potential-vector products are accomplished via a pseudo-spectral transform technique. By using Jacobi, Radau and orthogonal satellite vectors, we have proposed 21 types of orthogonal coordinate systems so that the algorithm is capable of describing most five-atom systems with small and/or large amplitude vibrational motions. Finally, an universal program ( PetroVib) has been developed. Its applications to the molecules CH and HO2-, and the van der Waals cluster HeCl are also discussed.

  17. Quantum Chemical Calculations

    NASA Technical Reports Server (NTRS)

    Bauschlicher, Charles W.; Arnold, James O. (Technical Monitor)

    1997-01-01

    The current methods of quantum chemical calculations will be reviewed. The accent will be on the accuracy that can be achieved with these methods. The basis set requirements and computer resources for the various methods will be discussed. The utility of the methods will be illustrated with some examples, which include the calculation of accurate bond energies for SiF$_n$ and SiF$_n^+$ and the modeling of chemical data storage.

  18. Quantum Chemical Calculations

    NASA Technical Reports Server (NTRS)

    Bauschlicher, Charles W.; Arnold, James O. (Technical Monitor)

    1997-01-01

    The current methods of quantum chemical calculations will be reviewed. The accent will be on the accuracy that can be achieved with these methods. The basis set requirements and computer resources for the various methods will be discussed. The utility of the methods will be illustrated with some examples, which include the calculation of accurate bond energies for SiF$_n$ and SiF$_n^+$ and the modeling of chemical data storage.

  19. Molecular dynamics simulation and quantum mechanical calculations on α-D-N-acetylneuraminic acid.

    PubMed

    Priyadarzini, Thanu R K; Subashini, Balakrishnan; Selvin, Jeyasigamani F A; Veluraja, Kasinadar

    2012-04-01

    N-Acetylneuraminic acid is a sugar molecule of biological significance due to its pivotal role in molecular recognition processes. The three dimensional structure and conformation of α-Neu5Ac in biological environments can be clearly observed by molecular dynamics (MD) simulation and quantum mechanical (QM) calculations. A 10ns MD simulation on α-Neu5Ac yields two conformational models which are stabilized by water mediated hydrogen bond between O-8/O-9 hydroxyl oxygen and carbonyl of carboxylate group. The average life time of the conformers and the residual time of water which mediates the hydrogen bonding interactions are computed. Based on the amphiprotic nature of water, water mediation of each conformer is divided into two different modes, one donor-one acceptor mode and two donor modes. According to the analysis of simulation trajectories, the preferred mode of water mediation for conformers is the one donor-one acceptor mode. The energy and geometry of the MD derived conformational models of α-Neu5Ac are optimized using HF/6-31G(∗) basis set of Gaussian03. QM calculations also resulted that α-Neu5Ac is preferentially stabilized by water mediated hydrogen bonding between O-8 hydroxyl and the carboxylate group where the mediation is one donor-one acceptor type. The optimized geometry of α-Neu5Ac which is in good agreement with the crystal structure of α-D-N-acetyl-1-O-methylneuraminic acid methyl ester is deposited in the public domain database 3DSDSCAR (http://3dsdscar.org). This optimized structure can be used by biotechnologists, biophysicists and glycobiologists for modelling the sialylglycans and also to design drugs using sialic acid analog inhibitors. Copyright © 2012 Elsevier Ltd. All rights reserved.

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

    NASA Technical Reports Server (NTRS)

    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.

  1. FeynDyn: A MATLAB program for fast numerical Feynman integral calculations for open quantum system dynamics on GPUs

    NASA Astrophysics Data System (ADS)

    Dattani, Nikesh S.

    2013-12-01

    This MATLAB program calculates the dynamics of the reduced density matrix of an open quantum system modeled either by the Feynman-Vernon model or the Caldeira-Leggett model. The user gives the program a Hamiltonian matrix that describes the open quantum system as if it were in isolation, a matrix of the same size that describes how that system couples to its environment, and a spectral distribution function and temperature describing the environment’s influence on it, in addition to the open quantum system’s initial density matrix and a grid of times. With this, the program returns the reduced density matrix of the open quantum system at all moments specified by that grid of times (or just the last moment specified by the grid of times if the user makes this choice). This overall calculation can be divided into two stages: the setup of the Feynman integral, and the actual calculation of the Feynman integral for time propagation of the density matrix. When this program calculates this propagation on a multi-core CPU, it is this propagation that is usually the rate-limiting step of the calculation, but when it is calculated on a GPU, the propagation is calculated so quickly that the setup of the Feynman integral can actually become the rate-limiting step. The overhead of transferring information from the CPU to the GPU and back seems to have a negligible effect on the overall runtime of the program. When the required information cannot fit on the GPU, the user can choose to run the entire program on a CPU. Catalogue identifier: AEPX_v1_0. Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEPX_v1_0.html. Program obtainable from: CPC Program Library, Queen’s University, Belfast, N. Ireland. Licensing provisions: Standard CPC licence, http://cpc.cs.qub.ac.uk/licence/licence.html. No. of lines in distributed program, including test data, etc.: 703. No. of bytes in distributed program, including test data, etc.: 11026. Distribution format: tar.gz. Programming

  2. Accurate quantum chemical calculations

    NASA Technical Reports Server (NTRS)

    Bauschlicher, Charles W., Jr.; Langhoff, Stephen R.; Taylor, Peter R.

    1989-01-01

    An important goal of quantum chemical calculations is to provide an understanding of chemical bonding and molecular electronic structure. A second goal, the prediction of energy differences to chemical accuracy, has been much harder to attain. First, the computational resources required to achieve such accuracy are very large, and second, it is not straightforward to demonstrate that an apparently accurate result, in terms of agreement with experiment, does not result from a cancellation of errors. Recent advances in electronic structure methodology, coupled with the power of vector supercomputers, have made it possible to solve a number of electronic structure problems exactly using the full configuration interaction (FCI) method within a subspace of the complete Hilbert space. These exact results can be used to benchmark approximate techniques that are applicable to a wider range of chemical and physical problems. The methodology of many-electron quantum chemistry is reviewed. Methods are considered in detail for performing FCI calculations. The application of FCI methods to several three-electron problems in molecular physics are discussed. A number of benchmark applications of FCI wave functions are described. Atomic basis sets and the development of improved methods for handling very large basis sets are discussed: these are then applied to a number of chemical and spectroscopic problems; to transition metals; and to problems involving potential energy surfaces. Although the experiences described give considerable grounds for optimism about the general ability to perform accurate calculations, there are several problems that have proved less tractable, at least with current computer resources, and these and possible solutions are discussed.

  3. Attosecond-resolution quantum dynamics calculations for atoms and molecules in strong laser fields.

    PubMed

    Lu, Rui-Feng; Zhang, Pei-Yu; Han, Ke-Li

    2008-06-01

    A parallel quantum electron and nuclei wave packet computer code, LZH-DICP, has been developed to study laser-atom-molecule interaction in the nonperturbative regime with attosecond resolution. The nonlinear phenomena occurring in that regime can be studied with the code in a rigorous way by numerically solving the time-dependent Schrödinger equation of electrons and nuclei. Time propagation of the wave functions is performed using a split-operator approach, and based on a sine discrete variable representation. Photoelectron spectra for hydrogen and kinetic-energy spectra for molecular hydrogen ion in linearly polarized laser fields are calculated using a flux operator scheme, which testifies to the validity and the high efficiency of LZH-DICP.

  4. Quantum Mechanics and physical calculations

    NASA Astrophysics Data System (ADS)

    Karayan, H. S.

    2014-03-01

    We suggest to realize the computer simulation and calculation by the algebraic structure built on the basis of the logic inherent to processes in physical systems (called physical computing). We suggest a principle for the construction of quantum algorithms of neuroinformatics of quantum neural networks. The role of academician Sahakyan is emphasized in the development of quantum physics in Armenia.

  5. Dynamical coupling of plasmons and molecular excitations by hybrid quantum/classical calculations: time-domain approach

    NASA Astrophysics Data System (ADS)

    Sakko, Arto; Rossi, Tuomas P.; Nieminen, Risto M.

    2014-08-01

    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 Na2 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 Na2 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 Na2 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.

  6. Quantum dynamics studies of gas-surface reactions and use of complex absorbing potentials in wave-packet calculations

    NASA Astrophysics Data System (ADS)

    Ge, Jiuyuan

    1999-11-01

    In this thesis, quantum dynamics studies are conducted on gas-surface reactions and complex absorbing potentials. Through a three-dimensional model, dissociation probabilities for O2 on both (110) and (100) surfaces of copper are calculated for ground state as well as rovibrationally excited oxygen molecules. Specifically, the reason for the difference in calculated dissociation probabilities of oxygen on two surfaces is explained. Then the thermal effect of the surface on the dissociation probability is studied by a one dimensional fluctuating barrier. It is observed that the quantum mechanical tunneling probability exhibits a maximum as a function of the oscillating frequency between the low and the high frequency limits. The physical origin and process underlying this resonantlike phenomenon are proposed. In the second part of this thesis, the complex absorbing potential (CAP) is introduced and studied. Exact numerical calculation shows that use of optimized CAP significantly improves the efficiency of wavefunction absorption over that of negative imaginary potential (NIP) in scattering applications. The CAP is optimized by an efficient time-dependent propagation approach. Application to the prototype inelastic scattering of He + H2 demonstrates the accuracy and efficiency of the channel-dependent CAP for extracting state-to-state scattering information.

  7. Quantum Molecular Dynamical Calculations of PEDOT 12-Oligomer and its Selenium and Tellurium Derivatives

    NASA Astrophysics Data System (ADS)

    Mirsakiyeva, Amina; Hugosson, Håkan W.; Crispin, Xavier; Delin, Anna

    2016-12-01

    We present simulation results, computed with the Car-Parrinello molecular dynamics method, at zero and ambient temperature (300 K) for poly(3,4-ethylenedioxythiophene) [PEDOT] and its selenium and tellurium derivatives PEDOS and PEDOTe, represented as 12-oligomer chains. In particular, we focus on structural parameters such as the dihedral rotation angle distribution, as well as how the charge distribution is affected by temperature. We find that for PEDOT, the dihedral angle distribution shows two distinct local maxima whereas for PEDOS and PEDOTe, the distributions only have one clear maximum. The twisting stiffness at ambient temperature appears to be larger the lighter the heteroatom (S, Se, Te) is, in contrast to the case at 0 K. As regards point charge distributions, they suggest that aromaticity increases with temperature, and also that aromaticity becomes more pronounced the lighter the heteroatom is, both at 0 K and ambient temperature. Our results agree well with previous results, where available. The bond lengths are consistent with substantial aromatic character both at 0 K and at ambient temperature. Our calculations also reproduce the expected trend of diminishing gap between the highest occupied molecular orbital and the lowest unoccupied molecular orbital with increasing atomic number of the heteroatom.

  8. Quantum Molecular Dynamical Calculations of PEDOT 12-Oligomer and its Selenium and Tellurium Derivatives

    NASA Astrophysics Data System (ADS)

    Mirsakiyeva, Amina; Hugosson, Håkan W.; Crispin, Xavier; Delin, Anna

    2017-05-01

    We present simulation results, computed with the Car-Parrinello molecular dynamics method, at zero and ambient temperature (300 K) for poly(3,4-ethylenedioxythiophene) [PEDOT] and its selenium and tellurium derivatives PEDOS and PEDOTe, represented as 12-oligomer chains. In particular, we focus on structural parameters such as the dihedral rotation angle distribution, as well as how the charge distribution is affected by temperature. We find that for PEDOT, the dihedral angle distribution shows two distinct local maxima whereas for PEDOS and PEDOTe, the distributions only have one clear maximum. The twisting stiffness at ambient temperature appears to be larger the lighter the heteroatom (S, Se, Te) is, in contrast to the case at 0 K. As regards point charge distributions, they suggest that aromaticity increases with temperature, and also that aromaticity becomes more pronounced the lighter the heteroatom is, both at 0 K and ambient temperature. Our results agree well with previous results, where available. The bond lengths are consistent with substantial aromatic character both at 0 K and at ambient temperature. Our calculations also reproduce the expected trend of diminishing gap between the highest occupied molecular orbital and the lowest unoccupied molecular orbital with increasing atomic number of the heteroatom.

  9. Quantum dynamics calculations using symmetrized, orthogonal Weyl-Heisenberg wavelets with a phase space truncation scheme. III. Representations and calculations.

    PubMed

    Poirier, Bill; Salam, A

    2004-07-22

    In a previous paper [J. Theo. Comput. Chem. 2, 65 (2003)], one of the authors (B.P.) presented a method for solving the multidimensional Schrodinger equation, using modified Wilson-Daubechies wavelets, and a simple phase space truncation scheme. Unprecedented numerical efficiency was achieved, enabling a ten-dimensional calculation of nearly 600 eigenvalues to be performed using direct matrix diagonalization techniques. In a second paper [J. Chem. Phys. 121, 1690 (2004)], and in this paper, we extend and elaborate upon the previous work in several important ways. The second paper focuses on construction and optimization of the wavelength functions, from theoretical and numerical viewpoints, and also examines their localization. This paper deals with their use in representations and eigenproblem calculations, which are extended to 15-dimensional systems. Even higher dimensionalities are possible using more sophisticated linear algebra techniques. This approach is ideally suited to rovibrational spectroscopy applications, but can be used in any context where differential equations are involved.

  10. Quantum dynamical calculation of bound rovibrational states of HO2 up to largest possible total angular momentum, J ≤ 130.

    PubMed

    Petty, Corey; Chen, Wenwu; Poirier, Bill

    2013-08-15

    In a previous article [J. Theor. Comput. Chem. 2010, 9, 435], all rovibrational bound states of HO2 were systematically computed, for all total angular momentum values J = 0-10. In this article, the high-J rovibrational states are computed for every multiple-of-ten J value up to J = 130, which is the point where the centrifugal barrier obliterates the potential well, and bound states no longer exist. The results are used to assess the importance of Coriolis coupling in this floppy system and to evaluate two different J-shifting schemes. Though not effective for multiply vibrationally excited bound states, vibrational-state-dependent J-shifting obtains modestly accurate predictions for the lowest-lying energies [J. Phys. Chem. A 2006, 110, 3246]. However, much better performance is obtained-especially for large J values, and despite substantial Coriolis coupling-using a second, rotational-state-dependent J-shifting scheme [J. Chem. Phys. 1998, 108, 5216], for which the rotational constants themselves depend on J and K. The latter formalism also yields important dynamical insight into the structure of the strongly Coriolis-coupled eigenstate wave functions. The calculations were performed using ScalIT, a suite of codes enabling quantum dynamics calculations on massively parallel computing architectures.

  11. Quantum spectra and dynamics

    NASA Astrophysics Data System (ADS)

    Arce, Julio Cesar

    This work focuses on time-dependent quantum theory and methods for the study of the spectra and dynamics of atomic and molecular systems. Specifically, we have addressed the following two problems: (1) Development of a time-dependent spectral method for the construction of spectra of simple quantum systems. This includes the calculation of eigenenergies, the construction of bound and continuum eigenfunctions, and the calculation of photo cross-sections. Computational applications include the quadrupole photoabsorption spectra and dissociation cross-sections of molecular hydrogen from various vibrational states in its ground electronic potential-energy curve. This method is seen to provide an advantageous alternative, both from the computational and conceptual point of view, to existing standard methods. (2) Explicit time-dependent formulation of photoabsorption processes -- Analytical solutions of the time-dependent Schrodinger equation are constructed and employed for the calculation of probability densities, momentum distributions, fluxes, transition rates, expectation values and correlation functions. These quantities are seen to establish the link between the dynamics and the calculated, or measured, spectra and cross-sections, and to clarify the dynamical nature of the excitation, transition and ejection processes. Numerical calculations on atomic and molecular hydrogen corroborate and complement the previous results, allowing the identification of different regimes during the photoabsorption process.

  12. Quantum Spectra and Dynamics

    NASA Astrophysics Data System (ADS)

    Arce, Julio Cesar

    1992-01-01

    This work focuses on time-dependent quantum theory and methods for the study of the spectra and dynamics of atomic and molecular systems. Specifically, we have addressed the following two problems: (i) Development of a time-dependent spectral method for the construction of spectra of simple quantum systems--This includes the calculation of eigenenergies, the construction of bound and continuum eigenfunctions, and the calculation of photo cross-sections. Computational applications include the quadrupole photoabsorption spectra and dissociation cross-sections of molecular hydrogen from various vibrational states in its ground electronic potential -energy curve. This method is seen to provide an advantageous alternative, both from the computational and conceptual point of view, to existing standard methods. (ii) Explicit time-dependent formulation of photoabsorption processes --Analytical solutions of the time-dependent Schrodinger equation are constructed and employed for the calculation of probability densities, momentum distributions, fluxes, transition rates, expectation values and correlation functions. These quantities are seen to establish the link between the dynamics and the calculated, or measured, spectra and cross-sections, and to clarify the dynamical nature of the excitation, transition and ejection processes. Numerical calculations on atomic and molecular hydrogen corroborate and complement the previous results, allowing the identification of different regimes during the photoabsorption process.

  13. Conformational determinants of tandem GU mismatches in RNA: insights from molecular dynamics simulations and quantum mechanical calculations.

    PubMed

    Pan, Yongping; Priyakumar, U Deva; MacKerell, Alexander D

    2005-02-08

    Structure and energetic properties of base pair mismatches in duplex RNA have been the focus of numerous investigations due to their role in many important biological functions. Such efforts have contributed to the development of models for secondary structure prediction of RNA, including the nearest-neighbor model. In RNA duplexes containing GU mismatches, 5'-GU-3' tandem mismatches have a different thermodynamic stability than 5'-UG-3' mismatches. In addition, 5'-GU-3' mismatches in some sequence contexts do not follow the nearest-neighbor model for stability. To characterize the underlying atomic forces that determine the structural and thermodynamic properties of GU tandem mismatches, molecular dynamics (MD) simulations were performed on a series of 5'-GU-3' and 5'-UG-3' duplexes in different sequence contexts. Overall, the MD-derived structural models agree well with experimental data, including local deviations in base step helicoidal parameters in the region of the GU mismatches and the model where duplex stability is associated with the pattern of GU hydrogen bonding. Further analysis of the simulations, validated by data from quantum mechanical calculations, suggests that the experimentally observed differences in thermodynamic stability are dominated by GG interstrand followed by GU intrastrand base stacking interactions that dictate the one versus two hydrogen bonding scenarios for the GU pairs. In addition, the inability of 5'-GU-3' mismatches in different sequence contexts to all fit into the nearest-neighbor model is indicated to be associated with interactions of the central four base pairs with the surrounding base pairs. The results emphasize the role of GG and GU stacking interactions on the structure and thermodynamics of GU mismatches in RNA.

  14. Communication: Ro-vibrational control of chemical reactivity in H+CH₄→ H₂+CH₃: full-dimensional quantum dynamics calculations and a sudden model.

    PubMed

    Welsch, Ralph; Manthe, Uwe

    2014-08-07

    The mode-selective chemistry of the title reaction is studied by full-dimensional quantum dynamics simulation on an accurate ab initio potential energy surface for vanishing total angular momentum. Using a rigorous transition state based approach and multi-configurational time-dependent Hartree wave packet propagation, initial state-selected reaction probabilities for many ro-vibrational states of methane are calculated. The theoretical results are compared with experimental trends seen in reactions of methane. An intuitive interpretation of the ro-vibrational control of the chemical reactivity provided by a sudden model based on the quantum transition state concept is discussed.

  15. Ab initio molecular orbital calculation considering the quantum mechanical effect of nuclei by path integral molecular dynamics

    NASA Astrophysics Data System (ADS)

    Shiga, Motoyuki; Tachikawa, Masanori; Miura, Shinichi

    2000-12-01

    We present an accurate calculational scheme for many-body systems composed of electrons and nuclei, by path integral molecular dynamics technique combined with the ab initio molecular orbital theory. Based upon the scheme, the simulation of a water molecule at room temperature is demonstrated, applying all-electron calculation at the Hartree-Fock level of theory.

  16. Polyatomic Quantum Dynamics

    NASA Astrophysics Data System (ADS)

    Zhang, Dong Hui

    This thesis presents extensive studies on the quantum dynamics of diatom-diatom systems using primarily the time-dependent(TD) wave packet approach. The theoretical investigations include the photofragmentation of tetraatomic molecules and bimolecular diatom-diatom chemical reaction. Specifically, the quantum mechanical study on direct photodissociation of H_20 _2 is carried out using a time-dependent golden rule wave packet method on an empirical potential energy surface. The calculation shows that the rotation distributions are Gaussian-like and two OH radicals are highly correlated in rotation. Both the time-dependent and time-independent golden rule methods are employed to compute the vibrational predissociation decay widths for weakly bound clusters including D_2HF, H_2HF, HD-HF, and HF-HF. These quantum mechanical calculations reveal that the vibrational predissociation processes are very stereospecific and state specific, that the lifetimes depend critically on the type of mode being excited and the nature of the vibrational coupling, and the theoretical results are very sensitive to details of the interaction potential energy surface including the repulse of the PES. The full-dimensional (6D) dynamics study for diatom -diatom chemical reactions is presented with the first initial state-selected total reaction probabilities, cross sections and thermal rate constants reported for H_2 + OH to H_2 O + H reaction. The effects of reagents rotation and vibration on reaction are examined in detail in this study. Our calculations reveal surprisingly sharp resonance -like features at low collision energies on the Schatz-Elgersma potential surface, and also demonstrate that the potential -averaged 5D (PA5D) treatment can produce reaction probabilities essentially indistinguishable from the full-dimensional (6D) treatment.

  17. Ab Initio Molecular Dynamics Calculations versus Quantum-State-Resolved Experiments on CHD3 + Pt(111): New Insights into a Prototypical Gas-Surface Reaction.

    PubMed

    Nattino, Francesco; Ueta, Hirokazu; Chadwick, Helen; van Reijzen, Maarten E; Beck, Rainer D; Jackson, Bret; van Hemert, Marc C; Kroes, Geert-Jan

    2014-04-17

    The dissociative chemisorption of methane on metal surfaces is of fundamental and practical interest, being a rate-limiting step in the steam reforming process. The reaction is best modeled with quantum dynamics calculations, but these are currently not guaranteed to produce accurate results because they rely on potential energy surfaces based on untested density functionals and on untested dynamical approximations. To help overcome these limitations, here we present for the first time statistically accurate reaction probabilities obtained with ab initio molecular dynamics (AIMD) for a polyatomic gas-phase molecule reacting with a metal surface. Using a general purpose density functional, the AIMD reaction probabilities are in semiquantitative agreement with new quantum-state-resolved experiments on CHD3 + Pt(111). The comparison suggests the use of the sudden approximation for treating the rotations even though CHD3 has large rotational constants and yields an estimated reaction barrier of 0.9 eV for CH4 + Pt(111).

  18. Development of calculation and analysis methods for the dynamic first hyperpolarizability based on the ab initio molecular orbital-quantum master equation method.

    PubMed

    Kishi, Ryohei; Fujii, Hiroaki; Kishimoto, Shingo; Murata, Yusuke; Ito, Soichi; Okuno, Katsuki; Shigeta, Yasuteru; Nakano, Masayoshi

    2012-05-03

    We develop novel calculation and analysis methods for the dynamic first hyperpolarizabilities β [the second-order nonlinear optical (NLO) properties at the molecular level] in the second-harmonic generation based on the quantum master equation method combined with the ab initio molecular orbital (MO) configuration interaction method. As examples, we have evaluated off-resonant dynamic β values of donor (NH(2))- and/or acceptor (NO(2))-substituted benzenes using these methods, which are shown to reproduce those by the conventional summation-over-states method well. The spatial contributions of electrons to the dynamic β of these systems are also analyzed using the dynamic β density and its partition into the MO contributions. The present results demonstrate the advantage of these methods in unraveling the mechanism of dynamic NLO properties and in building the structure-dynamic NLO property relationships of real molecules.

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

    PubMed

    Luo, Ye; Zen, Andrea; Sorella, Sandro

    2014-11-21

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

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

    SciTech Connect

    Luo, Ye Sorella, Sandro; Zen, Andrea

    2014-11-21

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

  1. Apparent randomness in quantum dynamics

    NASA Astrophysics Data System (ADS)

    Cerdeira, Hilda A.; Huberman, B. A.

    1987-08-01

    We show how bounded quantum systems in the presence of time-periodic fields can mimic random behavior in spite of their almost periodic character. We calculate the distribution of values taken by observables in the course of time, and demonstrate how they become asymptotically Gaussian in the large-N limit but with constant variance and a posteriori, δ-correlated noise. Thus, unlike a priori processes, the quantum dynamics of bounded systems remains nondiffusive while appearing to be random.

  2. Quantum path-integral molecular dynamics calculations of the dipole-bound state of the water dimer anion

    NASA Astrophysics Data System (ADS)

    Shiga, Motoyuki; Takayanagi, Toshiyuki

    2003-09-01

    The equilibrium structure of the negatively charged water dimer (H 2O) 2- has been studied using the path-integral molecular dynamics simulation. All the atomic motions as well as the excess electron were treated quantum mechanically, employing a semi-empirical model combining a water-water interatomic potential with an electron-water pseudopotential. It is demonstrated that the molecular structure of (H 2O) 2- is more flexible than that of (H 2O) 2; both the donor switching and donor-acceptor interchange can more effectively occur in (H 2O) 2- than in (H 2O) 2. We conclude that this floppy character is a result of the breakdown of the adiabatic Born-Oppenheimer picture.

  3. Quantum transport calculations using periodic boundaryconditions

    SciTech Connect

    Wang, Lin-Wang

    2004-06-15

    An efficient new method is presented to calculate the quantum transports using periodic boundary conditions. This method allows the use of conventional ground state ab initio programs without big changes. The computational effort is only a few times of a normal groundstate calculations, thus is makes accurate quantum transport calculations for large systems possible.

  4. Quantification of the interaction forces between metals and graphene by quantum chemical calculations and dynamic force measurements under ambient conditions.

    PubMed

    Lazar, Petr; Zhang, Shuai; Safářová, Klára; Li, Qiang; Froning, Jens Peter; Granatier, Jaroslav; Hobza, Pavel; Zbořil, Radek; Besenbacher, Flemming; Dong, Mingdong; Otyepka, Michal

    2013-02-26

    The two-dimensional material graphene has numerous potential applications in nano(opto)electronics, which inevitably involve metal graphene interfaces.Theoretical approaches have been employed to examine metal graphene interfaces, but experimental evidence is currently lacking. Here, we combine atomic force microscopy (AFM) based dynamic force measurements and density functional theory calculations to quantify the interaction between metal-coated AFM tips and graphene under ambient conditions. The results show that copper has the strongest affinity to graphene among the studied metals (Cu, Ag, Au, Pt, Si), which has important implications for the construction of a new generation of electronic devices. Observed differences in the nature of the metal-graphene bonding are well reproduced by the calculations, which included nonlocal Hartree-Fock exchange and van der Waals effects.

  5. Dynamics of quantum entanglement in quantum channels

    NASA Astrophysics Data System (ADS)

    Liang, Shi-Dong

    2017-08-01

    Based on the von Neumann entropy, we give a computational formalism of the quantum entanglement dynamics in quantum channels, which can be applied to a general finite systems coupled with their environments in quantum channels. The quantum entanglement is invariant in the decoupled local unitary quantum channel, but it is variant in the non-local coupled unitary quantum channel. The numerical investigation for two examples, two-qubit and two-qutrit models, indicates that the quantum entanglement evolution in the quantum non-local coupling channel oscillates with the coupling strength and time, and depends on the quantum entanglement of the initial state. It implies that quantum information loses or gains when the state of systems evolves in the quantum non-local coupling channel.

  6. Excited state structures and decay dynamics of 1,3-dimethyluracils in solutions: resonance Raman and quantum mechanical calculation study.

    PubMed

    Li, Ming-Juan; Liu, Ming-Xia; Zhao, Yan-Ying; Pei, Ke-Mei; Wang, Hui-Gang; Zheng, Xuming; Fang, Wei Hai

    2013-10-03

    The resonance Raman spectroscopic study of the excited state structural dynamics of 1,3-dimethyluracil (DMU), 5-bromo-1,3-dimethyluracil (5BrDMU), uracil, and thymine in water and acetonitrile were reported. Density functional theory calculations were carried out to help elucidate the ultraviolet electronic transitions associated with the A-, and B-band absorptions and the vibrational assignments of the resonance Raman spectra. The effect of the methylation at N1, N3 and C5 sites of pyrimidine ring on the structural dynamics of uracils in different solvents were explored on the basis of the resonance Raman intensity patterns. The relative resonance Raman intensities of DMU and 5BrDMU are computed at the B3LYP-TD level. Huge discrepancies between the experimental resonance Raman intensities and the B3LYP-TD predicted ones were observed. The underlying mechanism was briefly discussed. The decay channel through the S1((1)nπ*)/S2((1)ππ*) conical intersection and the S1((1)nπ*)/T1((3)ππ*) intersystem crossing were revealed by using the CASSCF(8,7)/6-31G(d) level of theory calculations.

  7. Quantum causal graph dynamics

    NASA Astrophysics Data System (ADS)

    Arrighi, Pablo; Martiel, Simon

    2017-07-01

    Consider a graph having quantum systems lying at each node. Suppose that the whole thing evolves in discrete time steps, according to a global, unitary causal operator. By causal we mean that information can only propagate at a bounded speed, with respect to the distance given by the graph. Suppose, moreover, that the graph itself is subject to the evolution, and may be driven to be in a quantum superposition of graphs—in accordance to the superposition principle. We show that these unitary causal operators must decompose as a finite-depth circuit of local unitary gates. This unifies a result on quantum cellular automata with another on reversible causal graph dynamics. Along the way we formalize a notion of causality which is valid in the context of quantum superpositions of time-varying graphs, and has a number of good properties. We discuss some of the implications for quantum gravity.

  8. Molecular Dynamics Calculations

    NASA Technical Reports Server (NTRS)

    1996-01-01

    The development of thermodynamics and statistical mechanics is very important in the history of physics, and it underlines the difficulty in dealing with systems involving many bodies, even if those bodies are identical. Macroscopic systems of atoms typically contain so many particles that it would be virtually impossible to follow the behavior of all of the particles involved. Therefore, the behavior of a complete system can only be described or predicted in statistical ways. Under a grant to the NASA Lewis Research Center, scientists at the Case Western Reserve University have been examining the use of modern computing techniques that may be able to investigate and find the behavior of complete systems that have a large number of particles by tracking each particle individually. This is the study of molecular dynamics. In contrast to Monte Carlo techniques, which incorporate uncertainty from the outset, molecular dynamics calculations are fully deterministic. Although it is still impossible to track, even on high-speed computers, each particle in a system of a trillion trillion particles, it has been found that such systems can be well simulated by calculating the trajectories of a few thousand particles. Modern computers and efficient computing strategies have been used to calculate the behavior of a few physical systems and are now being employed to study important problems such as supersonic flows in the laboratory and in space. In particular, an animated video (available in mpeg format--4.4 MB) was produced by Dr. M.J. Woo, now a National Research Council fellow at Lewis, and the G-VIS laboratory at Lewis. This video shows the behavior of supersonic shocks produced by pistons in enclosed cylinders by following exactly the behavior of thousands of particles. The major assumptions made were that the particles involved were hard spheres and that all collisions with the walls and with other particles were fully elastic. The animated video was voted one of two

  9. Quantum Tunneling in Testosterone 6β-Hydroxylation by Cytochrome P450: Reaction Dynamics Calculations Employing Multiconfiguration Molecular-Mechanical Potential Energy Surfaces

    NASA Astrophysics Data System (ADS)

    Zhang, Yan; Lin, Hai

    2009-05-01

    Testosterone hydroxylation is a prototypical reaction of human cytochrome P450 3A4, which metabolizes about 50% of oral drugs on the market. Reaction dynamics calculations were carried out for the testosterone 6β-hydrogen abstraction and the 6β-d1-testosterone 6β-duterium abstraction employing a model that consists of the substrate and the active oxidant compound I. The calculations were performed at the level of canonical variational transition state theory with multidimensional tunneling and were based on a semiglobal full-dimensional potential energy surface generated by the multiconfiguration molecular mechanics technique. The tunneling coefficients were found to be around 3, indicating substantial contributions by quantum tunneling. However, the tunneling made only modest contributions to the kinetic isotope effects. The kinetic isotope effects were computed to be about 2 in the doublet spin state and about 5 in the quartet spin state.

  10. Dynamics of the O(3P)+H2 reaction at low temperatures: Comparison of quasiclassical trajectory with quantum scattering calculations

    NASA Astrophysics Data System (ADS)

    Weck, P. F.; Balakrishnan, N.; Brandão, J.; Rosa, C.; Wang, W.

    2006-02-01

    Quasiclassical trajectory and quantum-mechanical scattering calculations are reported for the O (P3)+H2(XΣg+1;υ=1-3,j=0)→OH(XΠ2)+H(S2) reaction at energies close to the reaction threshold. The dynamics of the reaction have been investigated for zero total angular momentum using the lowest A″3 potential-energy surface developed by Rogers et al. [J. Phys. Chem. A 104, 2308 (2000)] and its recent extensions by Brandão et al. [J. Chem. Phys. 121, 8861 (2004)] which provide an improved description of the van der Waals interaction. Good agreement is observed for this system between quasiclassical and quantal results for incident kinetic energies above the tunneling regime. Quantum-mechanical calculations also confirm recent theoretical predictions of a strong collision-energy dependence of the OH (v'=0)/OH(v'=1) product branching ratio in the O (P3)+H2(v=1) reaction, which explains the differences observed in OH vibrational populations between experiments using different O (P3) sources.

  11. Mechanism of the Glycosidic Bond Cleavage of Mismatched Thymine in Human Thymine DNA Glycosylase Revealed by Classical Molecular Dynamics and Quantum Mechanical/Molecular Mechanical Calculations.

    PubMed

    Kanaan, Natalia; Crehuet, Ramon; Imhof, Petra

    2015-09-24

    Base excision of mismatched or damaged nucleotides catalyzed by glycosylase enzymes is the first step of the base excision repair system, a machinery preserving the integrity of DNA. Thymine DNA glycosylase recognizes and removes mismatched thymine by cleaving the C1'-N1 bond between the base and the sugar ring. Our quantum mechanical/molecular mechanical calculations of this reaction in human thymine DNA glycosylase reveal a requirement for a positive charge in the active site to facilitate C1'-N1 bond scission: protonation of His151 significantly lowers the free energy barrier for C1'-N1 bond dissociation compared to the situation with neutral His151. Shuttling a proton from His151 to the thymine base further reduces the activation free energy for glycosidic bond cleavage. Classical molecular dynamics simulations of the H151A mutant suggest that the mutation to the smaller, neutral, residue increases the water accessibility of the thymine base, rendering direct proton transfer from the bulk feasible. Quantum mechanical/molecular mechanical calculations of the glycosidic bond cleavage reaction in the H151A mutant show that the activation free energy is slightly lower than in the wild-type enzyme, explaining the experimentally observed higher reaction rates in this mutant.

  12. Cold and ultracold dynamics of the barrierless D(+) + H2 reaction: Quantum reactive calculations for ∼R(-4) long range interaction potentials.

    PubMed

    Lara, Manuel; Jambrina, P G; Aoiz, F J; Launay, J-M

    2015-11-28

    Quantum reactive and elastic cross sections and rate coefficients have been calculated for D(+) + H2 (v = 0, j = 0) collisions in the energy range from 10(-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(-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(5) a0 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.

  13. Understanding the structure and dynamic of odorants in the gas phase using a combination of microwave spectroscopy and quantum chemical calculations

    NASA Astrophysics Data System (ADS)

    Mouhib, Halima

    2014-07-01

    This tutorial is an introduction for PhD students and researchers who intend to start their future work in the field of microwave spectroscopy to investigate structural and dynamical aspects of isolated molecular systems in the gas phase. Although the presented case studies are related to odorants, i.e., volatile molecules that possess a noticeable scent, the background and applications of the method can be transferred to any other resembling molecular system. In the early days, microwave spectroscopy was mainly related to the structure determination of very small systems such as OCS or ammonia, where the bond lengths could be determined with high accuracy by measuring the different isotopic species of the molecules. Nowadays, the method is far more advanced and is also used to tackle various fundamental molecular problems in different fields such as physical chemistry and molecular physics. Interesting questions that can be investigated concern, e.g., the molecular structure, i.e., the different conformations, not only of the isolated molecule but also of van der Waals complexes with water, noble gases or other molecules. The dynamical and intra- or intermolecular effects can be straightforwardly observed without the influence of the environment as in the condensed phase. This evolution was only achieved by using quantum chemical methods as a complementary tool to elude the necessity of isotopologues for structure determination, which cannot be realized for large systems (>5 atoms). The combination of microwave spectroscopy and quantum chemical calculations is the method of choice when it comes to sampling the conformational space of molecules. This is particularly the case when small energy differences make it difficult to determine the conformers of the lowest energy using computational methods alone. Although quantum chemical calculations are important for the validation of microwave spectra, the focus of the tutorial is set on the experimental part of the

  14. Quantum biological channel modeling and capacity calculation.

    PubMed

    Djordjevic, Ivan B

    2012-12-10

    Quantum mechanics has an important role in photosynthesis, magnetoreception, and evolution. There were many attempts in an effort to explain the structure of genetic code and transfer of information from DNA to protein by using the concepts of quantum mechanics. The existing biological quantum channel models are not sufficiently general to incorporate all relevant contributions responsible for imperfect protein synthesis. Moreover, the problem of determination of quantum biological channel capacity is still an open problem. To solve these problems, we construct the operator-sum representation of biological channel based on codon basekets (basis vectors), and determine the quantum channel model suitable for study of the quantum biological channel capacity and beyond. The transcription process, DNA point mutations, insertions, deletions, and translation are interpreted as the quantum noise processes. The various types of quantum errors are classified into several broad categories: (i) storage errors that occur in DNA itself as it represents an imperfect storage of genetic information, (ii) replication errors introduced during DNA replication process, (iii) transcription errors introduced during DNA to mRNA transcription, and (iv) translation errors introduced during the translation process. By using this model, we determine the biological quantum channel capacity and compare it against corresponding classical biological channel capacity. We demonstrate that the quantum biological channel capacity is higher than the classical one, for a coherent quantum channel model, suggesting that quantum effects have an important role in biological systems. The proposed model is of crucial importance towards future study of quantum DNA error correction, developing quantum mechanical model of aging, developing the quantum mechanical models for tumors/cancer, and study of intracellular dynamics in general.

  15. Quantum Biological Channel Modeling and Capacity Calculation

    PubMed Central

    Djordjevic, Ivan B.

    2012-01-01

    Quantum mechanics has an important role in photosynthesis, magnetoreception, and evolution. There were many attempts in an effort to explain the structure of genetic code and transfer of information from DNA to protein by using the concepts of quantum mechanics. The existing biological quantum channel models are not sufficiently general to incorporate all relevant contributions responsible for imperfect protein synthesis. Moreover, the problem of determination of quantum biological channel capacity is still an open problem. To solve these problems, we construct the operator-sum representation of biological channel based on codon basekets (basis vectors), and determine the quantum channel model suitable for study of the quantum biological channel capacity and beyond. The transcription process, DNA point mutations, insertions, deletions, and translation are interpreted as the quantum noise processes. The various types of quantum errors are classified into several broad categories: (i) storage errors that occur in DNA itself as it represents an imperfect storage of genetic information, (ii) replication errors introduced during DNA replication process, (iii) transcription errors introduced during DNA to mRNA transcription, and (iv) translation errors introduced during the translation process. By using this model, we determine the biological quantum channel capacity and compare it against corresponding classical biological channel capacity. We demonstrate that the quantum biological channel capacity is higher than the classical one, for a coherent quantum channel model, suggesting that quantum effects have an important role in biological systems. The proposed model is of crucial importance towards future study of quantum DNA error correction, developing quantum mechanical model of aging, developing the quantum mechanical models for tumors/cancer, and study of intracellular dynamics in general. PMID:25371271

  16. Structure, dynamical stability, and electronic properties of phases in TaS2 from a high-level quantum mechanical calculation

    NASA Astrophysics Data System (ADS)

    Lazar, Petr; Martincová, Jana; Otyepka, Michal

    2015-12-01

    TaS2 is a transition-metal dichalcogenide having an exceptionally rich phase diagram, which includes exotic phenomena such as a charge density wave. We analyzed the structure, bonding, ground state, and dynamical stability of 1 T , 2 H , and 3 R phases of TaS2, and a commensurate charge density wave phase from the first principles. Van der Waals interaction among layers and strong electron-electron interactions were included by using the exact exchange plus random phase approximation, a high-level quantum mechanical approach. The calculated structural parameters agree well with the available experimental data. The individual sheets of TaS2 are bound by dispersive forces, which are stronger than dispersive forces in graphite and fluorographite. 1 T -TaS2 is dynamically unstable at low temperature, which leads to the formation of charge density wave and opening of the in-plane band gap. Anharmonic phonon-phonon interactions stabilize the 1 T structure at elevated temperatures. The calculated phase diagram of TaS2 reveals that the 1 T phase is the ground state at temperatures above 1300 K, 2 H below this point, and the charge density wave phase becomes more stable than the perfect 1 T structure below 480 K.

  17. Quantum dynamics and nonintegrability

    NASA Astrophysics Data System (ADS)

    Hogg, T.; Huberman, B. A.

    1983-07-01

    Results of a nonperturbative investigation of the global behavior of quantum systems with time-periodic Hamiltonians are presented. These include the proof of a theorem stating that such systems, if bounded and nonresonant, will reassemble themselves infinitely often in the course of time. In order to illustrate the applicability of this result, an analytic study of a driven harmonic oscillator is presented, together with computer simulations of quantum maps describing the dynamics of a pulsed electron in a well and a periodically kicked rotor. A quantitative study of resonance excitation also shows that in practical situations recurrence is pervasive. Several unique quantum effects are analyzed, and their relevance to the classical limit is discussed. A formula is derived for recurrence times, and computer experiments are performed to test its validity.

  18. First principle thousand atom quantum dot calculations

    SciTech Connect

    Wang, Lin-Wang; Li, Jingbo

    2004-03-30

    A charge patching method and an idealized surface passivation are used to calculate the single electronic states of IV-IV, III-V, II-VI semiconductor quantum dots up to a thousand atoms. This approach scales linearly and has a 1000 fold speed-up compared to direct first principle methods with a cost of eigen energy error of about 20 meV. The calculated quantum dot band gaps are parametrized for future references.

  19. Zeno dynamics in quantum open systems.

    PubMed

    Zhang, Yu-Ran; Fan, Heng

    2015-06-23

    Quantum Zeno effect shows that frequent observations can slow down or even stop the unitary time evolution of an unstable quantum system. This effect can also be regarded as a physical consequence of the statistical indistinguishability of neighboring quantum states. The accessibility of quantum Zeno dynamics under unitary time evolution can be quantitatively estimated by quantum Zeno time in terms of Fisher information. In this work, we investigate the accessibility of quantum Zeno dynamics in quantum open systems by calculating noisy Fisher information when a trace preserving and completely positive map is assumed. We firstly study the consequences of non-Markovian noise on quantum Zeno effect and give the exact forms of the dissipative Fisher information and the quantum Zeno time. Then, for the operator-sum representation, an achievable upper bound of the quantum Zeno time is given with the help of the results in noisy quantum metrology. It is of significance that the noise reducing the accuracy in the entanglement-enhanced parameter estimation can conversely be favorable for the accessibility of quantum Zeno dynamics of entangled states.

  20. Zeno dynamics in quantum open systems

    PubMed Central

    Zhang, Yu-Ran; Fan, Heng

    2015-01-01

    Quantum Zeno effect shows that frequent observations can slow down or even stop the unitary time evolution of an unstable quantum system. This effect can also be regarded as a physical consequence of the statistical indistinguishability of neighboring quantum states. The accessibility of quantum Zeno dynamics under unitary time evolution can be quantitatively estimated by quantum Zeno time in terms of Fisher information. In this work, we investigate the accessibility of quantum Zeno dynamics in quantum open systems by calculating noisy Fisher information when a trace preserving and completely positive map is assumed. We firstly study the consequences of non-Markovian noise on quantum Zeno effect and give the exact forms of the dissipative Fisher information and the quantum Zeno time. Then, for the operator-sum representation, an achievable upper bound of the quantum Zeno time is given with the help of the results in noisy quantum metrology. It is of significance that the noise reducing the accuracy in the entanglement-enhanced parameter estimation can conversely be favorable for the accessibility of quantum Zeno dynamics of entangled states. PMID:26099840

  1. Exploring the sloped-to-peaked S2/S1 seam of intersection of thymine with electronic structure and direct quantum dynamics calculations.

    PubMed

    Asturiol, David; Lasorne, Benjamin; Worth, Graham A; Robb, Michael A; Blancafort, Lluís

    2010-05-21

    The role of the seam of intersection between the lowest (pi,pi*) and (n,pi*) excited states in the decay of electronically excited singlet thymine has been investigated with ab initio complete active space self-consistent field (CASSCF) calculations and direct dynamics variational multiconfiguration Gaussian (DD-vMCG) quantum dynamics on the full-dimensional CASSCF surface, with 39 degrees of freedom. The seam has a sloped-to-peaked topography, and the dynamics at the different segments of the seam have been studied by varying the initial conditions of the propagation. When the wave packet is directed to the peaked segments, part of it traverses the seam, stays on the (pi,pi*) state and heads towards decay to the ground state. In contrast to this, when the wave packet is driven to sloped seam segments it bounces back to the minimum of the (pi,pi*) state. Significant population transfer to the (n,pi*) state is observed in both cases. The results suggest that a sloped-to-peaked topography can be used to control photochemical reactivity, by driving the wave packet to different regions of the seam where a different outcome of the propagation can be expected.

  2. Quantum Noise from Reduced Dynamics

    NASA Astrophysics Data System (ADS)

    Vacchini, Bassano

    2016-07-01

    We consider the description of quantum noise within the framework of the standard Copenhagen interpretation of quantum mechanics applied to a composite system environment setting. Averaging over the environmental degrees of freedom leads to a stochastic quantum dynamics, described by equations complying with the constraints arising from the statistical structure of quantum mechanics. Simple examples are considered in the framework of open system dynamics described within a master equation approach, pointing in particular to the appearance of the phenomenon of decoherence and to the relevance of quantum correlation functions of the environment in the determination of the action of quantum noise.

  3. Chiral recognition of Propranolol enantiomers by β-Cyclodextrin: Quantum chemical calculation and molecular dynamics simulation studies

    NASA Astrophysics Data System (ADS)

    Ghatee, Mohammad Hadi; Sedghamiz, Tahereh

    2014-12-01

    Enantiomeric recognition of Propranolol by complexation with β-Cyclodextrin was studied by PM3 method and molecular dynamics (MD) simulation. Gas phase results show that the R-enantiomer complex is more stable than the S-enantiomer complex by 8.54 kJ/mol (Hartree-Fock energy). Using polarized continuum model, solution phase of R-enantiomer complex was found to be more stable than S-enantiomer complex by 25.95 kJ/mol. Both complexes hardly occur at room temperature free-energy-wise, though, complexation with R-enantiomer is more favorable than with S-enantiomer enthalpy-wise. Also, complexes were studied by molecular dynamics simulation in gas and solution phases. More stability of R-enantiomer complex in gas phase is confirmed by MD van der Waals energy (5.04 kJ/mol) and closely by the counterpart PM3 binding energy (8.54 kJ/mol). Simulation in solution phase indicates more stability of R-enantiomer complex. Finally, simulated transport property provides insight into the high anisotropic atoms motion according to which S-Propranolol found possessing significantly higher dynamics.

  4. Accurate quantum dynamics calculations of vibrational spectrum of dideuteromethane CH{sub 2}D{sub 2}

    SciTech Connect

    Yu, Hua-Gen

    2015-05-21

    We report a rigorous variational study of the infrared (IR) vibrational spectra of both CH{sub 2}D{sub 2} and {sup 13}CH{sub 2}D{sub 2} isotopomers using an exact molecular Hamiltonian. Calculations are carried out using a recently developed multi-layer Lanczos algorithm based on the accurate refined Wang and Carrington potential energy surface of methane and the low-order truncated ab initio dipole moment surface of Yurchenko et al. [J. Mol. Spectrosc. 291, 69 (2013)]. All well converged 357 vibrational energy levels up to 6100 cm{sup −1} of CH{sub 2}D{sub 2} are obtained, together with a comparison to previous calculations and 91 experimental bands available. The calculated frequencies are in excellent agreement with the experimental results and give a root-mean-square error of 0.67 cm{sup −1}. In particular, we also compute the transition intensities from the vibrational ground state for both isotopomers. Based on the theoretical results, 20 experimental bands are suggested to be re-assigned. Surprisingly, an anomalous C isotopic effect is discovered in the nν{sub 5} modes of CH{sub 2}D{sub 2}. The predicted IR spectra provide useful information for understanding those unknown bands.

  5. Quantum dynamics in the partial Wigner picture

    NASA Astrophysics Data System (ADS)

    Beck, Geoffrey M.; Sergi, Alessandro

    2013-10-01

    Recently we have shown how the partial Wigner representation of quantum mechanics can be used to study hybrid quantum models where a system with a finite number of energy levels is coupled to linear or nonlinear oscillators (Beck and Sergi 2013 Phys. Lett. A 377 1047). The purpose of this work is to provide a detailed derivation of the partially Wigner-transformed quantum equations of motion for nonlinear oscillator subsystems under the action of general polynomial potentials. Such equations can be written in terms of a propagator, which can then be expanded in a power series. The linear terms of the series describe quantum-classical dynamics while the nonlinear terms provide the corrections needed to restore the fully quantum character of the evolution. In the case of polynomial potentials and position dependent couplings, the number of nonlinear terms is finite and the corrections can be calculated explicitly. In this work we show how to implement numerically the above scheme where, in principle, no assumption about the strength of the coupling must be taken. We illustrate the formalism by studying a two-level system interacting with an asymmetric quartic oscillator. We integrate the quantum dynamics of the total system and provide a comparison with the case of the quantum-classical dynamics of the quartic oscillator. The approach presented here is expected to be effective for studying hybrid quantum circuits in quantum information theory and for witnessing the quantum-to-classical transition in nano-oscillators coupled to pseudo-spins.

  6. Fluorescence of tryptophan in designed hairpin and Trp-cage miniproteins: measurements of fluorescence yields and calculations by quantum mechanical molecular dynamics simulations.

    PubMed

    McMillan, Andrew W; Kier, Brandon L; Shu, Irene; Byrne, Aimee; Andersen, Niels H; Parson, William W

    2013-02-14

    The quantum yield of tryptophan (Trp) fluorescence was measured in 30 designed miniproteins (17 β-hairpins and 13 Trp-cage peptides), each containing a single Trp residue. Measurements were made in D(2)O and H(2)O to distinguish between fluorescence quenching mechanisms involving electron and proton transfer in the hairpin peptides, and at two temperatures to check for effects of partial unfolding of the Trp-cage peptides. The extent of folding of all the peptides also was measured by NMR. The fluorescence yields ranged from 0.01 in some of the Trp-cage peptides to 0.27 in some hairpins. Fluorescence quenching was found to occur by electron transfer from the excited indole ring of the Trp to a backbone amide group or the protonated side chain of a nearby histidine, glutamate, aspartate, tyrosine, or cysteine residue. Ionized tyrosine side chains quenched strongly by resonance energy transfer or electron transfer to the excited indole ring. Hybrid classical/quantum mechanical molecular dynamics simulations were performed by a method that optimized induced electric dipoles separately for the ground and excited states in multiple π-π* and charge-transfer (CT) excitations. Twenty 0.5 ns trajectories in the tryptophan's lowest excited singlet π-π* state were run for each peptide, beginning by projections from trajectories in the ground state. Fluorescence quenching was correlated with the availability of a CT or exciton state that was strongly coupled to the π-π* state and that matched or fell below the π-π* state in energy. The fluorescence yields predicted by summing the calculated rates of charge and energy transfer are in good accord with the measured yields.

  7. Quantum fluid dynamics approach for electronic structure calculation: application to the study of ground-state properties of rare gas atoms

    NASA Astrophysics Data System (ADS)

    Roy, Amlan K.; Chu, Shih-I.

    2002-05-01

    We explore the usefulness of a quantum fluid dynamics (QFD) approach for quantitative electronic structure calculations of many-electron systems. By combining QFD and density functional theory, a single time-dependent nonlinear QFD equation can be derived. The equation is further transformed into a diffusion-type form by an imaginary-time evolution method, whose asymptotic solution reaches a global minimum and the many-body ground-state wavefunction. The time-dependent generalized pseudospectral method is extended to solve the diffusion equation in spherical coordinates, allowing optimal and nonuniform spatial discretization and accurate and efficient solution of the diffusion function in space and time. The procedure is applied to the study of electronic energies, densities and other ground-state properties of noble gas atoms (He, Ne, Ar, Kr, Xe). The results are in good agreement with other best available values. The method offers a conceptually appealing and computationally practical procedure for the treatment of many-electron systems beyond the Hartree-Fock level.

  8. Quantum backreaction on classical dynamics

    NASA Astrophysics Data System (ADS)

    Vachaspati, Tanmay

    2017-06-01

    Motivated by various systems in which quantum effects occur in classical backgrounds, we consider the dynamics of a classical particle as described by a coherent state that is coupled to a quantum bath via biquadratic interactions. We evaluate the resulting quantum dissipation of the motion of the classical particle. We also find classical initial conditions for the bath that effectively lead to the same dissipation as that due to quantum effects, possibly providing a way to approximately account for quantum backreaction within a classical analysis.

  9. Molecular dynamics with quantum fluctuations

    SciTech Connect

    Georgescu, Ionut; Mandelshtam, Vladimir A.

    2010-09-01

    A quantum dynamics approach, called Gaussian molecular dynamics, is introduced. As in the centroid molecular dynamics, the N-body quantum system is mapped to an N-body classical system with an effective Hamiltonian arising within the variational Gaussian wave-packet approximation. The approach is exact for the harmonic oscillator and for the high-temperature limit, accurate in the short-time limit and is computationally very efficient.

  10. Communication: Ro-vibrational control of chemical reactivity in H+CH{sub 4}→ H{sub 2}+CH{sub 3} : Full-dimensional quantum dynamics calculations and a sudden model

    SciTech Connect

    Welsch, Ralph Manthe, Uwe

    2014-08-07

    The mode-selective chemistry of the title reaction is studied by full-dimensional quantum dynamics simulation on an accurate ab initio potential energy surface for vanishing total angular momentum. Using a rigorous transition state based approach and multi-configurational time-dependent Hartree wave packet propagation, initial state-selected reaction probabilities for many ro-vibrational states of methane are calculated. The theoretical results are compared with experimental trends seen in reactions of methane. An intuitive interpretation of the ro-vibrational control of the chemical reactivity provided by a sudden model based on the quantum transition state concept is discussed.

  11. Fractal dynamics in chaotic quantum transport

    NASA Astrophysics Data System (ADS)

    Rasanen, Esa; Kotimaki, Ville; Hennig, Holger; Heller, Eric

    2013-03-01

    Despite several experiments on chaotic quantum transport, corresponding ab initio quantum simulations have been out of reach so far. Here we carry out quantum transport calculations in real space and real time for a two-dimensional stadium cavity that shows chaotic dynamics. Applying a large set of magnetic fields yields a complete picture of the magnetoconductance that indicates fractal scaling on intermediate time scales. Two methods that originate from different fields of physics are used to analyze the scaling exponent and the fractal dimension. They lead to consistent results that, in turn, qualitatively agree with the previous experimental data.

  12. The quantum dynamics of interfacial hydrogen: Path integral maximum entropy calculation of adsorbate vibrational line shapes for the H/Ni(111) system

    NASA Astrophysics Data System (ADS)

    Kim, Dongsup; Doll, J. D.; Gubernatis, J. E.

    1997-01-01

    Vibrational line shapes for a hydrogen atom on an embedded atom model (EAM) of the Ni(111) surface are extracted from path integral Monte Carlo data. Maximum entropy methods are utilized to stabilize this inversion. Our results indicate that anharmonic effects are significant, particularly for vibrational motion parallel to the surface. Unlike their normal mode analogs, calculated quantum line shapes for the EAM potential predict the correct ordering of vibrational features corresponding to parallel and perpendicular adsorbate motion.

  13. Quantum Monte Carlo calculations for light nuclei

    SciTech Connect

    Wiringa, R.B.

    1997-10-01

    Quantum Monte Carlo calculations of ground and low-lying excited states for nuclei with A {le} 8 have been made using a realistic Hamiltonian that fits NN scattering data. Results for more than two dozen different (J{sup {pi}}, T) p-shell states, not counting isobaric analogs, have been obtained. The known excitation spectra of all the nuclei are reproduced reasonably well. Density and momentum distributions and various electromagnetic moments and form factors have also been computed. These are the first microscopic calculations that directly produce nuclear shell structure from realistic NN interactions.

  14. Quantum Monte Carlo calculations for light nuclei.

    SciTech Connect

    Wiringa, R. B.

    1998-10-23

    Quantum Monte Carlo calculations of ground and low-lying excited states for nuclei with A {le} 8 are made using a realistic Hamiltonian that fits NN scattering data. Results for more than 40 different (J{pi}, T) states, plus isobaric analogs, are obtained and the known excitation spectra are reproduced reasonably well. Various density and momentum distributions and electromagnetic form factors and moments have also been computed. These are the first microscopic calculations that directly produce nuclear shell structure from realistic NN interactions.

  15. Quantum Monte Carlo calculations for light nuclei

    SciTech Connect

    Wiringa, R.B.

    1998-08-01

    Quantum Monte Carlo calculations of ground and low-lying excited states for nuclei with A {le} 8 are made using a realistic Hamiltonian that fits NN scattering data. Results for more than 30 different (j{sup {prime}}, T) states, plus isobaric analogs, are obtained and the known excitation spectra are reproduced reasonably well. Various density and momentum distributions and electromagnetic form factors and moments have also been computed. These are the first microscopic calculations that directly produce nuclear shell structure from realistic NN interactions.

  16. Fractal dynamics in chaotic quantum transport.

    PubMed

    Kotimäki, V; Räsänen, E; Hennig, H; Heller, E J

    2013-08-01

    Despite several experiments on chaotic quantum transport in two-dimensional systems such as semiconductor quantum dots, corresponding quantum simulations within a real-space model have been out of reach so far. Here we carry out quantum transport calculations in real space and real time for a two-dimensional stadium cavity that shows chaotic dynamics. By applying a large set of magnetic fields we obtain a complete picture of magnetoconductance that indicates fractal scaling. In the calculations of the fractality we use detrended fluctuation analysis-a widely used method in time-series analysis-and show its usefulness in the interpretation of the conductance curves. Comparison with a standard method to extract the fractal dimension leads to consistent results that in turn qualitatively agree with the previous experimental data.

  17. Fractal dynamics in chaotic quantum transport

    NASA Astrophysics Data System (ADS)

    Kotimäki, V.; Räsänen, E.; Hennig, H.; Heller, E. J.

    2013-08-01

    Despite several experiments on chaotic quantum transport in two-dimensional systems such as semiconductor quantum dots, corresponding quantum simulations within a real-space model have been out of reach so far. Here we carry out quantum transport calculations in real space and real time for a two-dimensional stadium cavity that shows chaotic dynamics. By applying a large set of magnetic fields we obtain a complete picture of magnetoconductance that indicates fractal scaling. In the calculations of the fractality we use detrended fluctuation analysis—a widely used method in time-series analysis—and show its usefulness in the interpretation of the conductance curves. Comparison with a standard method to extract the fractal dimension leads to consistent results that in turn qualitatively agree with the previous experimental data.

  18. On quantum potential dynamics

    NASA Astrophysics Data System (ADS)

    Goldstein, Sheldon; Struyve, Ward

    2015-01-01

    Non-relativistic de Broglie-Bohm theory describes particles moving under the guidance of the wave function. In de Broglie's original formulation, the particle dynamics is given by a first-order differential equation. In Bohm's reformulation, it is given by Newton's law of motion with an extra potential that depends on the wave function—the quantum potential—together with a constraint on the possible velocities. It was recently argued, mainly by numerical simulations, that relaxing this velocity constraint leads to a physically untenable theory. We provide further evidence for this by showing that for various wave functions the particles tend to escape the wave packet. In particular, we show that for a central classical potential and bound energy eigenstates the particle motion is often unbounded. This work seems particularly relevant for ways of simulating wave function evolution based on Bohm's formulation of the de Broglie-Bohm theory. Namely, the simulations may become unstable due to deviations from the velocity constraint.

  19. Dynamics of nonrelativistic quantum mechanics

    NASA Astrophysics Data System (ADS)

    Efthimiades, Spyros

    2017-01-01

    We show that the wavefunction of an electron interacting with an electric potential is accurately represented by the superposition of plane waves that fulfills the total energy relation. As a result, we explicitly derive the Schrödinger, Pauli, Klein-Gordon, and Dirac equations. While the traditional nonrelativistic quantum dynamics is based on postulates, the dynamics we introduce is theoretically justified, in agreement with experimental measurements, and consistent with the fundamental theory of quantum electrodynamics.

  20. Quantum dynamics of the parametric oscillator

    NASA Astrophysics Data System (ADS)

    Kinsler, P.; Drummond, P. D.

    1991-06-01

    We present dynamical calculations for the quantum parametric oscillator using both number-state and coherent-state bases. The coherent-state methods use the positive-P representation, which has a nonclassical phase space-an essential requirement in obtaining an exact stochastic representation of this nonlinear problem. This also provides a way to directly simulate quantum tunneling between the two above-threshold stable states of the oscillator. The coherent-state methods provide both analytic results at large photon numbers, and numerical results for any photon number, while our number-state calculations are restricted to numerical results in the low-photon-number regime. The number-state and coherent-state methods give precise agreement within the accuracy of the numerical calculations. We also compare our results with methods based on a truncated Wigner representation equivalent to stochastic electrodynamics, and find that these are unable to correctly predict the tunneling rate given by the other methods. An interesting feature of the results is the much faster tunneling predicted by the exact quantum-theory methods compared with earlier semiclassical calculations using an approximate potential barrier. This is similar to the faster tunneling found when comparing quantum penetration of a barrier to classical thermal activation. The quantum parametric oscillator, which has an exact steady-state solution, therefore provides a useful and accessible system in which nonlinear quantum effects can be studied far from thermal equilibrium.

  1. Dynamics of Super Quantum Correlations and Quantum Correlations for a System of Three Qubits

    NASA Astrophysics Data System (ADS)

    Siyouri, F.; El Baz, M.; Rfifi, S.; Hassouni, Y.

    2016-04-01

    The dynamics of quantum discord for two qubits independently interacting with dephasing reservoirs have been studied recently. The authors [Phys. Rev. A 88 (2013) 034304] found that for some Bell-diagonal states (BDS) which interact with their environments the calculation of quantum discord could experience a sudden transition in its dynamics, this phenomenon is known as the sudden change. Here in the present paper, we analyze the dynamics of normal quantum discord and super quantum discord for tripartite Bell-diagonal states independently interacting with dephasing reservoirs. Then, we find that basis change does not necessary mean sudden change of quantum correlations.

  2. Quantum wave packet ab initio molecular dynamics: an approach to study quantum dynamics in large systems.

    PubMed

    Iyengar, Srinivasan S; Jakowski, Jacek

    2005-03-15

    A methodology to efficiently conduct simultaneous dynamics of electrons and nuclei is presented. The approach involves quantum wave packet dynamics using an accurate banded, sparse and Toeplitz representation for the discrete free propagator, in conjunction with ab initio molecular dynamics treatment of the electronic and classical nuclear degree of freedom. The latter may be achieved either by using atom-centered density-matrix propagation or by using Born-Oppenheimer dynamics. The two components of the methodology, namely, quantum dynamics and ab initio molecular dynamics, are harnessed together using a time-dependent self-consistent field-like coupling procedure. The quantum wave packet dynamics is made computationally robust by using adaptive grids to achieve optimized sampling. One notable feature of the approach is that important quantum dynamical effects including zero-point effects, tunneling, as well as over-barrier reflections are treated accurately. The electronic degrees of freedom are simultaneously handled at accurate levels of density functional theory, including hybrid or gradient corrected approximations. Benchmark calculations are provided for proton transfer systems and the dynamics results are compared with exact calculations to determine the accuracy of the approach.

  3. Quantum mechanical calculations to chemical accuracy

    NASA Technical Reports Server (NTRS)

    Bauschlicher, Charles W., Jr.; Langhoff, Stephen R.

    1991-01-01

    The accuracy of current molecular-structure calculations is illustrated with examples of quantum mechanical solutions for chemical problems. Two approaches are considered: (1) the coupled-cluster singles and doubles (CCSD) with a perturbational estimate of the contribution of connected triple excitations, or CCDS(T); and (2) the multireference configuration-interaction (MRCI) approach to the correlation problem. The MRCI approach gains greater applicability by means of size-extensive modifications such as the averaged-coupled pair functional approach. The examples of solutions to chemical problems include those for C-H bond energies, the vibrational frequencies of O3, identifying the ground state of Al2 and Si2, and the Lewis-Rayleigh afterglow and the Hermann IR system of N2. Accurate molecular-wave functions can be derived from a combination of basis-set saturation studies and full configuration-interaction calculations.

  4. Trotter-based simulation of quantum-classical dynamics.

    PubMed

    Kernan, Dónal Mac; Ciccotti, Giovanni; Kapral, Raymond

    2008-01-17

    Quantum rate processes in condensed phase systems are often computed by combining quantum and classical descriptions of the dynamics. An algorithm for simulating the quantum-classical Liouville equation, which describes the dynamics of a quantum subsystem coupled to a classical bath, is presented in this paper. The algorithm is based on a Trotter decomposition of the quantum-classical propagator, in conjunction with Monte Carlo sampling of quantum transitions, to yield a surface-hopping representation of the dynamics. An expression for the nonadiabatic propagator that is responsible for quantum transitions and associated bath momentum changes is derived in a form that is convenient for Monte Carlo sampling and exactly conserves the total energy of the system in individual trajectories. The expectation values of operators or quantum correlation functions can be evaluated by initial sampling of quantum states and use of quantum-classical Liouville dynamics for the time evolution. The algorithm is tested by calculations on the spin-boson model, for which exact quantum results are available, and is shown to reproduce the exact results for stronger nonadiabatic coupling and much longer times using fewer trajectories than other schemes for simulating quantum-classical Liouville dynamics.

  5. Dynamical quantum phase transitions (Review Article)

    NASA Astrophysics Data System (ADS)

    Zvyagin, A. A.

    2016-11-01

    During recent years the interest to dynamics of quantum systems has grown considerably. Quantum many body systems out of equilibrium often manifest behavior, different from the one predicted by standard statistical mechanics and thermodynamics in equilibrium. Since the dynamics of a many-body quantum system typically involve many excited eigenstates, with a non-thermal distribution, the time evolution of such a system provides an unique way for investigation of non-equilibrium quantum statistical mechanics. Last decade such new subjects like quantum quenches, thermalization, pre-thermalization, equilibration, generalized Gibbs ensemble, etc. are among the most attractive topics of investigation in modern quantum physics. One of the most interesting themes in the study of dynamics of quantum many-body systems out of equilibrium is connected with the recently proposed important concept of dynamical quantum phase transitions. During the last few years a great progress has been achieved in studying of those singularities in the time dependence of characteristics of quantum mechanical systems, in particular, in understanding how the quantum critical points of equilibrium thermodynamics affect their dynamical properties. Dynamical quantum phase transitions reveal universality, scaling, connection to the topology, and many other interesting features. Here we review the recent achievements of this quickly developing part of low-temperature quantum physics. The study of dynamical quantum phase transitions is especially important in context of their connection to the problem of the modern theory of quantum information, where namely non-equilibrium dynamics of many-body quantum system plays the major role.

  6. Experimental realization of quantum zeno dynamics

    PubMed Central

    Schäfer, F.; Herrera, I.; Cherukattil, S.; Lovecchio, C.; Cataliotti, F.S.; Caruso, F.; Smerzi, A.

    2014-01-01

    It is generally impossible to probe a quantum system without disturbing it. However, it is possible to exploit the back action of quantum measurements and strong couplings to tailor and protect the coherent evolution of a quantum system. This is a profound and counterintuitive phenomenon known as quantum Zeno dynamics. Here we demonstrate quantum Zeno dynamics with a rubidium Bose–Einstein condensate in a five-level Hilbert space. We harness measurements and strong couplings to dynamically disconnect different groups of quantum states and constrain the atoms to coherently evolve inside a two-level subregion. In parallel to the foundational importance due to the realization of a dynamical superselection rule and the theory of quantum measurements, this is an important step forward in protecting and controlling quantum dynamics and, broadly speaking, quantum information processing. PMID:24476716

  7. Fractional-time quantum dynamics.

    PubMed

    Iomin, Alexander

    2009-08-01

    Application of the fractional calculus to quantum processes is presented. In particular, the quantum dynamics is considered in the framework of the fractional time Schrödinger equation (SE), which differs from the standard SE by the fractional time derivative: partial differential/partial differentialt --> partial differential(alpha)/partial differentialt(alpha). It is shown that for alpha=1/2 the fractional SE is isospectral to a comb model. An analytical expression for the Green's functions of the systems are obtained. The semiclassical limit is discussed.

  8. Quantum dynamics in open quantum-classical systems.

    PubMed

    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.

  9. Excited state proton transfer dynamics of thioacetamide in S2(ππ*) state: resonance Raman spectroscopic and quantum mechanical calculations study.

    PubMed

    Chen, Xiao; Zhao, Yanying; Zhang, Haibo; Xue, Jiadan; Zheng, Xuming

    2015-02-05

    The photophysics and photochemistry of thioacetamide (CH3CSNH2) after excitation to the S2 electronic state were investigated by using resonance Raman spectroscopy in conjunction with the complete active space self-consistent field (CASSCF) method and density functional theory (DFT) calculations. The A-band resonance Raman spectra in acetonitrile, methanol, and water were obtained at 299.1, 282.4, 266.0, 252.7, and 245.9 nm excitation wavelengths to probe the structural dynamics of thioacetamide in the S2 state. CASSCF calculations were done to determine the transition energies and structures of the lower-lying excited states, the conical intersection points CI(S2/S1) and CI(S1/S0), and intersystem crossing points. The structural dynamics of thioacetamide in the S2 state was revealed to be along eight Franck-Condon active vibrational modes ν15, ν11, ν14, ν10, ν8, ν12, ν18, and ν19, mostly in the CC/CS/CN stretches and the CNH8,9/CCH5,6,7/CCN/CCS in-plane bends as indicated by the corresponding normal mode descriptions. The S2 → S1 decay process via the S2/S1 conical intersection point as the major channel were excluded. The thione-thiol photoisomerization reaction mechanism of thioacetamide via the S2,FC → S'1,min excited state proton transfer (ESPT) reaction channel was proposed.

  10. The quantum dynamic capacity formula of a quantum channel

    NASA Astrophysics Data System (ADS)

    Wilde, Mark M.; Hsieh, Min-Hsiu

    2012-12-01

    The dynamic capacity theorem characterizes the reliable communication rates of a quantum channel when combined with the noiseless resources of classical communication, quantum communication, and entanglement. In prior work, we proved the converse part of this theorem by making contact with many previous results in the quantum Shannon theory literature. In this work, we prove the theorem with an "ab initio" approach, using only the most basic tools in the quantum information theorist's toolkit: the Alicki-Fannes' inequality, the chain rule for quantum mutual information, elementary properties of quantum entropy, and the quantum data processing inequality. The result is a simplified proof of the theorem that should be more accessible to those unfamiliar with the quantum Shannon theory literature. We also demonstrate that the "quantum dynamic capacity formula" characterizes the Pareto optimal trade-off surface for the full dynamic capacity region. Additivity of this formula reduces the computation of the trade-off surface to a tractable, textbook problem in Pareto trade-off analysis, and we prove that its additivity holds for the quantum Hadamard channels and the quantum erasure channel. We then determine exact expressions for and plot the dynamic capacity region of the quantum dephasing channel, an example from the Hadamard class, and the quantum erasure channel.

  11. Interchain impacts on electronic structures of heterocyclic oligomers and polymers containing group 14, 15, and 16 heteroatoms: quantum chemical calculations in combination with molecular dynamics simulations.

    PubMed

    Zhang, Guiling; Ma, Jing; Wen, Jin

    2007-10-11

    The packing structures and packing effects on excitation energies of oligomers of polyfuran (PFu), polypyrrole (PPy), polycyclopentidene (PCp), polythiophene (PTh), polyphosphole (PPh), and polysilole (PSi) are comparatively studied by employing molecular dynamics (MD) simulations and time-dependent density functional theory (TDDFT) calculations. The dependence of packing structures on the main group of heteroatoms in the five-membered heterocyclic oligomers is exhibited from MD simulations. The planarity of backbones and the population of pi-stacked structures increase with the heteroatoms going from group 14 to group 16; i.e., PCp < PPy < PFu; PSi < PPh < PTh. The polymers with the third row elements, PSi and PPh, tend to have larger chain flexibilities in the packing systems than those with the second row elements, PCp and PPy, respectively. On the basis of the second-order Møller-Plesset perturbation (MP2) and natural bond orbital (NBO) calculations of the pi-stacked pairs, the difference in pi-stack orientations, head-to-tail vs head-to-head, between various packing systems is rationalized by individual interchain bond orbital interactions involved with heteroatoms. The packing systems with higher row elements tend to have narrower band gaps. The band gaps are closely related to the chain torsions driven by interchain interactions. The noticeable chain distortions in the packing systems of PCp, PSi, and PPh lead to the significant increase of band gaps in comparison with those appraised from periodic boundary conditions (PBC) calculations on their planar isolated chains.

  12. Advances in Quantum Trajectory Approaches to Dynamics

    NASA Astrophysics Data System (ADS)

    Askar, Attila

    2001-03-01

    The quantum fluid dynamics (QFD) formulation is based on the separation of the amplitude and phase of the complex wave function in Schrodinger's equation. The approach leads to conservation laws for an equivalent "gas continuum". The Lagrangian [1] representation corresponds to following the particles of the fluid continuum, i. e. calculating "quantum trajectories". The Eulerian [2] representation on the other hand, amounts to observing the dynamics of the gas continuum at the points of a fixed coordinate frame. The combination of several factors leads to a most encouraging computational efficiency. QFD enables the numerical analysis to deal with near monotonic amplitude and phase functions. The Lagrangian description concentrates the computation effort to regions of highest probability as an optimal adaptive grid. The Eulerian representation allows the study of multi-coordinate problems as a set of one-dimensional problems within an alternating direction methodology. An explicit time integrator limits the increase in computational effort with the number of discrete points to linear. Discretization of the space via local finite elements [1,2] and global radial functions [3] will be discussed. Applications include wave packets in four-dimensional quadratic potentials and two coordinate photo-dissociation problems for NOCl and NO2. [1] "Quantum fluid dynamics (QFD) in the Lagrangian representation with applications to photo-dissociation problems", F. Sales, A. Askar and H. A. Rabitz, J. Chem. Phys. 11, 2423 (1999) [2] "Multidimensional wave-packet dynamics within the fluid dynamical formulation of the Schrodinger equation", B. Dey, A. Askar and H. A. Rabitz, J. Chem. Phys. 109, 8770 (1998) [3] "Solution of the quantum fluid dynamics equations with radial basis function interpolation", Xu-Guang Hu, Tak-San Ho, H. A. Rabitz and A. Askar, Phys. Rev. E. 61, 5967 (2000)

  13. Quantum dynamics of two-photon quantum Rabi model

    NASA Astrophysics Data System (ADS)

    Lü, Zhiguo; Zhao, Chunjian; Zheng, Hang

    2017-02-01

    We apply a simple analytical method based on a unitary transformation to calculate the ground state, its excitation spectrum and quantum dynamic evolution of physical quantities for the double-photon quantum Rabi Hamiltonian over the wide coupling-strength range. The concise analytical method possesses the same mathematical simplicity as the approach of the rotating wave approximation (RWA). By quantitative comparison with the numerically exact result obtained by matrix diagonalization, we confirm that our calculated results obtained by transformed rotating-wave method are not only accurate in the weak coupling regime but also correct in intermediate strong-coupling case. In the intermediate ultrastrong-coupling regime, the calculated values of the ground state and lower lying excited states are nearly the same as the exact ones. It turns out that our calculation for the energy spectrum is beyond the ordinary-RWA. Meanwhile, we demonstrate the signatures resulting from the counter-rotating wave terms by monitoring the population, the coherence, the squeezing of the photon under the ultra-strong conditions. In particular, we find that when the frequency of the photon is much larger than the transition frequency of the system, the lineshape of the time evolution becomes complicated with the increase of the coupling strength, which may be verified experimentally.

  14. Quantum effects in unimolecular reaction dynamics

    SciTech Connect

    Gezelter, Joshua Daniel

    1995-12-01

    This work is primarily concerned with the development of models for the quantum dynamics of unimolecular isomerization and photodissociation reactions. We apply the rigorous quantum methodology of a Discrete Variable Representation (DVR) with Absorbing Boundary Conditions (ABC) to these models in an attempt to explain some very surprising results from a series of experiments on vibrationally excited ketene. Within the framework of these models, we are able to identify the experimental signatures of tunneling and dynamical resonances in the energy dependence of the rate of ketene isomerization. Additionally, we investigate the step-like features in the energy dependence of the rate of dissociation of triplet ketene to form 3B1 CH2 + 1σ+ CO that have been observed experimentally. These calculations provide a link between ab initio calculations of the potential energy surfaces and the experimentally observed dynamics on these surfaces. Additionally, we develop an approximate model for the partitioning of energy in the products of photodissociation reactions of large molecules with appreciable barriers to recombination. In simple bond cleavage reactions like CH3COCl → CH3CO + Cl, the model does considerably better than other impulsive and statistical models in predicting the energy distribution in the products. We also investigate ways of correcting classical mechanics to include the important quantum mechanical aspects of zero-point energy. The method we investigate is found to introduce a number of undesirable dynamical artifacts including a reduction in the above-threshold rates for simple reactions, and a strong mixing of the chaotic and regular energy domains for some model problems. We conclude by discussing some of the directions for future research in the field of theoretical chemical dynamics.

  15. New methods for quantum mechanical reaction dynamics

    SciTech Connect

    Thompson, Ward Hugh

    1996-12-01

    Quantum mechanical methods are developed to describe the dynamics of bimolecular chemical reactions. We focus on developing approaches for directly calculating the desired quantity of interest. Methods for the calculation of single matrix elements of the scattering matrix (S-matrix) and initial state-selected reaction probabilities are presented. This is accomplished by the use of absorbing boundary conditions (ABC) to obtain a localized (L2) representation of the outgoing wave scattering Green`s function. This approach enables the efficient calculation of only a single column of the S-matrix with a proportionate savings in effort over the calculation of the entire S-matrix. Applying this method to the calculation of the initial (or final) state-selected reaction probability, a more averaged quantity, requires even less effort than the state-to-state S-matrix elements. It is shown how the same representation of the Green`s function can be effectively applied to the calculation of negative ion photodetachment intensities. Photodetachment spectroscopy of the anion ABC- can be a very useful method for obtaining detailed information about the neutral ABC potential energy surface, particularly if the ABC- geometry is similar to the transition state of the neutral ABC. Total and arrangement-selected photodetachment spectra are calculated for the H3O- system, providing information about the potential energy surface for the OH + H2 reaction when compared with experimental results. Finally, we present methods for the direct calculation of the thermal rate constant from the flux-position and flux-flux correlation functions. The spirit of transition state theory is invoked by concentrating on the short time dynamics in the area around the transition state that determine reactivity. These methods are made efficient by evaluating the required quantum mechanical trace in the basis of eigenstates of the

  16. Cluster dynamical mean-field calculations for TiOCl

    NASA Astrophysics Data System (ADS)

    Saha-Dasgupta, T.; Lichtenstein, A.; Hoinkis, M.; Glawion, S.; Sing, M.; Claessen, R.; Valentí, R.

    2007-10-01

    Based on a combination of cluster dynamical mean field theory (DMFT) and density functional calculations, we calculated the angle-integrated spectral density in the layered s=1/2 quantum magnet TiOCl. The agreement with recent photoemission and oxygen K-edge x-ray absorption spectroscopy experiments is found to be good. The improvement achieved with this calculation with respect to previous single-site DMFT calculations is an indication of the correlated nature and low-dimensionality of TiOCl.

  17. Radiation from quantum weakly dynamical horizons in loop quantum gravity.

    PubMed

    Pranzetti, Daniele

    2012-07-06

    We provide a statistical mechanical analysis of quantum horizons near equilibrium in the grand canonical ensemble. By matching the description of the nonequilibrium phase in terms of weakly dynamical horizons with a local statistical framework, we implement loop quantum gravity dynamics near the boundary. The resulting radiation process provides a quantum gravity description of the horizon evaporation. For large black holes, the spectrum we derive presents a discrete structure which could be potentially observable.

  18. Quantum pattern formation dynamics of photoinduced nucleation

    NASA Astrophysics Data System (ADS)

    Ishida, Kunio; Nasu, Keiichiro

    2008-06-01

    We study the dynamics of quantum pattern formation processes in molecular crystals which is concomitant with photoinduced nucleation. Since the nucleation process in coherent regime is driven by the nonadiabatic transition in each molecule followed by the propagation of phonons, it is necessary to take into account the quantum nature of both electrons and phonons in order to pursue the dynamics of the system. Therefore, we employ a model of localized electrons coupled with a quantized phonon mode and solve the time-dependent Schrödinger equation numerically. We found that there is a minimal size of clusters of excited molecules which triggers the photoinduced nucleation process; i.e., nucleation does not take place unless sufficient photoexcitation energy is concentrated within a narrow area of the system. We show that this result means that the spatial distribution of photoexcited molecules plays an important role in the nonlinearity of the dynamics and also in the optical properties observed in experiments. We calculate the conversion ratio, the rate of cluster formation, and correlation functions to reveal the dynamical properties of the pattern formation process; the initial dynamics of the photoinduced structural change is discussed from the viewpoint of pattern formation.

  19. Ergodicity and mixing in quantum dynamics

    NASA Astrophysics Data System (ADS)

    Zhang, Dongliang; Quan, H. T.; Wu, Biao

    2016-08-01

    After a brief historical review of ergodicity and mixing in dynamics, particularly in quantum dynamics, we introduce definitions of quantum ergodicity and mixing using the structure of the system's energy levels and spacings. Our definitions are consistent with the usual understanding of ergodicity and mixing. Two parameters concerning the degeneracy in energy levels and spacings are introduced. They are computed for right triangular billiards and the results indicate a very close relation between quantum ergodicity (mixing) and quantum chaos. At the end, we argue that, besides ergodicity and mixing, there may exist a third class of quantum dynamics which is characterized by a maximized entropy.

  20. Non-Markovian dynamics of quantum discord

    SciTech Connect

    Fanchini, F. F.; Caldeira, A. O.; Werlang, T.; Brasil, C. A.; Arruda, L. G. E.

    2010-05-15

    We evaluate the quantum discord dynamics of two qubits in independent and common non-Markovian environments. We compare the dynamics of entanglement with that of quantum discord. For independent reservoirs the quantum discord vanishes only at discrete instants whereas the entanglement can disappear during a finite time interval. For a common reservoir, quantum discord and entanglement can behave very differently with sudden birth of the former but not of the latter. Furthermore, in this case the quantum discord dynamics presents sudden changes in the derivative of its time evolution which is evidenced by the presence of kinks in its behavior at discrete instants of time.

  1. Quantum dynamics in dual spaces

    SciTech Connect

    Sudarshan, E.C.G.

    1993-12-31

    Quantum mechanics gives us information about spectra of dynamical variables and transition rates including scattering cross sections. They can be exhibited as spectral information in analytically continued spaces and their duals. Quantum mechanics formulated in these generalized spaces is used to study scattering and time evolution. It is shown that the usual asymptotic condition is inadequate to deal with scattering of composite or unstable particles. Scattering theory needs amendment when the interacting system is not isospectral with the free Hamiltonian, and the amendment is formulated. Perturbation theory in generalized spaces is developed and used to study the deletion and augmentation of the spectrum of the Hamiltonian. A complete set of algebraically independent constants for an interacting system is obtained. The question of the breaking of time symmetry is discussed.

  2. Stochastic description of quantum Brownian dynamics

    NASA Astrophysics Data System (ADS)

    Yan, Yun-An; Shao, Jiushu

    2016-08-01

    Classical Brownian motion has well been investigated since the pioneering work of Einstein, which inspired mathematicians to lay the theoretical foundation of stochastic processes. A stochastic formulation for quantum dynamics of dissipative systems described by the system-plus-bath model has been developed and found many applications in chemical dynamics, spectroscopy, quantum transport, and other fields. This article provides a tutorial review of the stochastic formulation for quantum dissipative dynamics. The key idea is to decouple the interaction between the system and the bath by virtue of the Hubbard-Stratonovich transformation or Itô calculus so that the system and the bath are not directly entangled during evolution, rather they are correlated due to the complex white noises introduced. The influence of the bath on the system is thereby defined by an induced stochastic field, which leads to the stochastic Liouville equation for the system. The exact reduced density matrix can be calculated as the stochastic average in the presence of bath-induced fields. In general, the plain implementation of the stochastic formulation is only useful for short-time dynamics, but not efficient for long-time dynamics as the statistical errors go very fast. For linear and other specific systems, the stochastic Liouville equation is a good starting point to derive the master equation. For general systems with decomposable bath-induced processes, the hierarchical approach in the form of a set of deterministic equations of motion is derived based on the stochastic formulation and provides an effective means for simulating the dissipative dynamics. A combination of the stochastic simulation and the hierarchical approach is suggested to solve the zero-temperature dynamics of the spin-boson model. This scheme correctly describes the coherent-incoherent transition (Toulouse limit) at moderate dissipation and predicts a rate dynamics in the overdamped regime. Challenging problems

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

    SciTech Connect

    Lara, Manuel; Jambrina, P. G.; Aoiz, F. J.; Launay, J.-M.

    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.

  4. Why quantum dynamics is linear

    NASA Astrophysics Data System (ADS)

    Jordan, Thomas F.

    2009-11-01

    A seed George planted 45 years ago is still producing fruit now. In 1961, George set out the fundamental proposition that quantum dynamics is described most generally by linear maps of density matrices. Since the first sprout from George's seed appeared in 1962, we have known that George's fundamental proposition can be used to derive the linear Schrodinger equation in cases where it can be expected to apply. Now we have a proof of George's proposition that density matrices are mapped linearly to density matrices, that there can be no nonlinear generalization of this. That completes the derivation of the linear Schrodinger equation. The proof of George's proposition replaces Wigner's theorem that a symmetry transformation is represented by a linear or antilinear operator. The assumption needed to prove George's proposition is just that the dynamics does not depend on anything outside the system but must allow the system to be described as part of a larger system. This replaces the physically less compelling assumption of Wigner's theorem that absolute values of inner products are preserved. The history of this question is reviewed. Nonlinear generalizations of quantum mechanics have been proposed. They predict small but clear nonlinear effects, which very accurate experiments have not seen. This begs the question. Is there a reason in principle why nonlinearity is not found? Is it impossible? Does quantum dynamics have to be linear? Attempts to prove this have not been decisive, because either their assumptions are not compelling or their arguments are not conclusive. The question has been left unsettled. The simple answer, based on a simple assumption, was found in two steps separated by 44 years.

  5. Quantum coherence in the dynamical Casimir effect

    NASA Astrophysics Data System (ADS)

    Samos-Sáenz de Buruaga, D. N.; Sabín, Carlos

    2017-02-01

    We propose to use quantum coherence as the ultimate proof of the quantum nature of the radiation that appears by means of the dynamical Casimir effect in experiments with superconducting microwave waveguides. We show that, unlike previously considered measurements such as entanglement and discord, quantum coherence does not require a threshold value of the external pump amplitude and is highly robust to thermal noise.

  6. Quantum surface and intertwiner dynamics in loop quantum gravity

    NASA Astrophysics Data System (ADS)

    Feller, Alexandre; Livine, Etera R.

    2017-06-01

    We introduce simple generic models of surface dynamics in loop quantum gravity (LQG). A quantum surface is defined as a set of elementary patches of area glued together. We provide it with an extra structure of locality (nearest neighbors), thought of as induced by the whole spin network state defining the 3d bulk geometry around the quantum surface. Here, we focus on classical surface dynamics, using a spinorial description of surface degrees of freedom. We introduce two classes of dynamics, to be thought as templates for future investigation of LQG dynamics with the dynamics of quantum black holes in mind. The first defines global dynamics of the closure defect of the surface, with two basic toy models, either a dissipative dynamics relaxing towards the closure constraint or a Hamiltonian dynamics precessing the closure defect. The second class of dynamics describes the isolated regime, when both area and closure defect are conserved throughout the evolution. The surface dynamics is implemented through U (N ) transformations and generalizes to a Bose-Hubbard Hamiltonian with a local quadratic potential interaction. We briefly discuss the implications of modeling the quantum black hole dynamics by a surface Bose-Hubbard model.

  7. Model dynamics for quantum computing

    NASA Astrophysics Data System (ADS)

    Tabakin, Frank

    2017-08-01

    A model master equation suitable for quantum computing dynamics is presented. In an ideal quantum computer (QC), a system of qubits evolves in time unitarily and, by virtue of their entanglement, interfere quantum mechanically to solve otherwise intractable problems. In the real situation, a QC is subject to decoherence and attenuation effects due to interaction with an environment and with possible short-term random disturbances and gate deficiencies. The stability of a QC under such attacks is a key issue for the development of realistic devices. We assume that the influence of the environment can be incorporated by a master equation that includes unitary evolution with gates, supplemented by a Lindblad term. Lindblad operators of various types are explored; namely, steady, pulsed, gate friction, and measurement operators. In the master equation, we use the Lindblad term to describe short time intrusions by random Lindblad pulses. The phenomenological master equation is then extended to include a nonlinear Beretta term that describes the evolution of a closed system with increasing entropy. An external Bath environment is stipulated by a fixed temperature in two different ways. Here we explore the case of a simple one-qubit system in preparation for generalization to multi-qubit, qutrit and hybrid qubit-qutrit systems. This model master equation can be used to test the stability of memory and the efficacy of quantum gates. The properties of such hybrid master equations are explored, with emphasis on the role of thermal equilibrium and entropy constraints. Several significant properties of time-dependent qubit evolution are revealed by this simple study.

  8. Quantum scattering calculation for reaction Br + H2 on two potential energy surfaces

    NASA Astrophysics Data System (ADS)

    Quan, Wei-Long; Tang, Ping-Ying; Tang, Bi-Yu

    Three-dimensional time-dependent quantum wave packet calculations have been carried out for Br + H2 on a new global ab initio and a semi-empirical extended London-Eyring-Polanyi-Sato potential energy surface. It is shown that on the ab initio surface, the threshold energy is much lower, and the reaction probabilities, cross sections, and rate constants are much larger. The effects of the initial rovibrational excitation have also been studied. Comparison of rate constants with experimental measurement implies that the ab initio surface is more suitable for quantum dynamic calculation. The possible reasons and mechanism for the dynamical difference on the two PES are analyzed and discussed.

  9. Quantum emitters dynamically coupled to a quantum field

    NASA Astrophysics Data System (ADS)

    Acevedo, O. L.; Quiroga, L.; Rodríguez, F. J.; Johnson, N. F.

    2013-12-01

    We study theoretically the dynamical response of a set of solid-state quantum emitters arbitrarily coupled to a single-mode microcavity system. Ramping the matter-field coupling strength in round trips, we quantify the hysteresis or irreversible quantum dynamics. The matter-field system is modeled as a finite-size Dicke model which has previously been used to describe equilibrium (including quantum phase transition) properties of systems such as quantum dots in a microcavity. Here we extend this model to address non-equilibrium situations. Analyzing the system's quantum fidelity, we find that the near-adiabatic regime exhibits the richest phenomena, with a strong asymmetry in the internal collective dynamics depending on which phase is chosen as the starting point. We also explore signatures of the crossing of the critical points on the radiation subsystem by monitoring its Wigner function; then, the subsystem can exhibit the emergence of non-classicality and complexity.

  10. Quantum emitters dynamically coupled to a quantum field

    SciTech Connect

    Acevedo, O. L.; Quiroga, L.; Rodríguez, F. J.; Johnson, N. F.

    2013-12-04

    We study theoretically the dynamical response of a set of solid-state quantum emitters arbitrarily coupled to a single-mode microcavity system. Ramping the matter-field coupling strength in round trips, we quantify the hysteresis or irreversible quantum dynamics. The matter-field system is modeled as a finite-size Dicke model which has previously been used to describe equilibrium (including quantum phase transition) properties of systems such as quantum dots in a microcavity. Here we extend this model to address non-equilibrium situations. Analyzing the system’s quantum fidelity, we find that the near-adiabatic regime exhibits the richest phenomena, with a strong asymmetry in the internal collective dynamics depending on which phase is chosen as the starting point. We also explore signatures of the crossing of the critical points on the radiation subsystem by monitoring its Wigner function; then, the subsystem can exhibit the emergence of non-classicality and complexity.

  11. Multi-state Approach to Chemical Reactivity in Fragment Based Quantum Chemistry Calculations.

    PubMed

    Lange, Adrian W; Voth, Gregory A

    2013-09-10

    We introduce a multistate framework for Fragment Molecular Orbital (FMO) quantum mechanical calculations and implement it in the context of protonated water clusters. The purpose of the framework is to address issues of nonuniqueness and dynamic fragmentation in FMO as well as other related fragment methods. We demonstrate that our new approach, Fragment Molecular Orbital Multistate Reactive Molecular Dynamics (FMO-MS-RMD), can improve energetic accuracy and yield stable molecular dynamics for small protonated water clusters undergoing proton transfer reactions.

  12. Opinion dynamics model based on quantum formalism

    SciTech Connect

    Artawan, I. Nengah; Trisnawati, N. L. P.

    2016-03-11

    Opinion dynamics model based on quantum formalism is proposed. The core of the quantum formalism is on the half spin dynamics system. In this research the implicit time evolution operators are derived. The analogy between the model with Deffuant dan Sznajd models is discussed.

  13. Quantum nuclear dynamics in the photophysics of diamondoids

    NASA Astrophysics Data System (ADS)

    Patrick, Christopher E.; Giustino, Feliciano

    2013-06-01

    The unusual electronic properties of diamondoids, the nanoscale relatives of diamond, make them attractive for applications ranging from drug delivery to field emission displays. Identifying the fundamental origin of these properties has proven highly challenging, with even the most advanced quantum many-body calculations unable to reproduce measurements of a quantity as ubiquitous as the optical gap. Here, by combining first-principles calculations and Importance Sampling Monte Carlo methods, we show that the quantum dynamics of carbon nuclei is key to understanding the electronic and optical properties of diamondoids. Quantum nuclear effects dramatically modify the absorption lineshapes and renormalize the optical gaps. These findings allow us to formulate a complete theory of optical absorption in diamondoids, and establish the universal role of quantum nuclear dynamics in nanodiamond across the length scales.

  14. Quantum chemical calculations of glycine glutaric acid

    NASA Astrophysics Data System (ADS)

    Arioǧlu, ćaǧla; Tamer, Ömer; Avci, Davut; Atalay, Yusuf

    2017-02-01

    Density functional theory (DFT) calculations of glycine glutaric acid were performed by using B3LYP levels with 6-311++G(d,p) basis set. The theoretical structural parameters such as bond lengths and bond angles are in a good agreement with the experimental values of the title compound. HOMO and LUMO energies were calculated, and the obtained energy gap shows that charge transfer occurs in the title compound. Vibrational frequencies were calculated and compare with experimental ones. 3D molecular surfaces of the title compound were simulated using the same level and basis set. Finally, the 13C and 1H NMR chemical shift values were calculated by the application of the gauge independent atomic orbital (GIAO) method.

  15. Dynamical symmetries in Kondo tunneling through complex quantum dots.

    PubMed

    Kuzmenko, T; Kikoin, K; Avishai, Y

    2002-10-07

    Kondo tunneling reveals hidden SO(n) dynamical symmetries of evenly occupied quantum dots. As is exemplified for an experimentally realizable triple quantum dot in parallel geometry, the possible values n=3,4,5,7 can be easily tuned by gate voltages. Following construction of the corresponding o(n) algebras, scaling equations are derived and Kondo temperatures are calculated. The symmetry group for a magnetic field induced anisotropic Kondo tunneling is SU(2) or SO(4).

  16. Quantum speed limits in open system dynamics.

    PubMed

    del Campo, A; Egusquiza, I L; Plenio, M B; Huelga, S F

    2013-02-01

    Bounds to the speed of evolution of a quantum system are of fundamental interest in quantum metrology, quantum chemical dynamics, and quantum computation. We derive a time-energy uncertainty relation for open quantum systems undergoing a general, completely positive, and trace preserving evolution which provides a bound to the quantum speed limit. When the evolution is of the Lindblad form, the bound is analogous to the Mandelstam-Tamm relation which applies in the unitary case, with the role of the Hamiltonian being played by the adjoint of the generator of the dynamical semigroup. The utility of the new bound is exemplified in different scenarios, ranging from the estimation of the passage time to the determination of precision limits for quantum metrology in the presence of dephasing noise.

  17. Quantum dynamics of fast chemical reactions

    SciTech Connect

    Light, J.C.

    1993-12-01

    The aims of this research are to explore, develop, and apply theoretical methods for the evaluation of the dynamics of gas phase collision processes, primarily chemical reactions. The primary theoretical tools developed for this work have been quantum scattering theory, both in time dependent and time independent forms. Over the past several years, the authors have developed and applied methods for the direct quantum evaluation of thermal rate constants, applying these to the evaluation of the hydrogen isotopic exchange reactions, applied wave packet propagation techniques to the dissociation of Rydberg H{sub 3}, incorporated optical potentials into the evaluation of thermal rate constants, evaluated the use of optical potentials for state-to-state reaction probability evaluations, and, most recently, have developed quantum approaches for electronically non-adiabatic reactions which may be applied to simplify calculations of reactive, but electronically adiabatic systems. Evaluation of the thermal rate constants and the dissociation of H{sub 3} were reported last year, and have now been published.

  18. Dynamics of a Quantum Phase Transition

    SciTech Connect

    Zurek, Wojciech H.; Dorner, Uwe; Zoller, Peter

    2005-09-02

    We present two approaches to the dynamics of a quench-induced phase transition in the quantum Ising model. One follows the standard treatment of thermodynamic second order phase transitions but applies it to the quantum phase transitions. The other approach is quantum, and uses Landau-Zener formula for transition probabilities in avoided level crossings. We show that predictions of the two approaches of how the density of defects scales with the quench rate are compatible, and discuss the ensuing insights into the dynamics of quantum phase transitions.

  19. Fast and accurate calculation of dilute quantum gas using Uehling-Uhlenbeck model equation

    NASA Astrophysics Data System (ADS)

    Yano, Ryosuke

    2017-02-01

    The Uehling-Uhlenbeck (U-U) model equation is studied for the fast and accurate calculation of a dilute quantum gas. In particular, the direct simulation Monte Carlo (DSMC) method is used to solve the U-U model equation. DSMC analysis based on the U-U model equation is expected to enable the thermalization to be accurately obtained using a small number of sample particles and the dilute quantum gas dynamics to be calculated in a practical time. Finally, the applicability of DSMC analysis based on the U-U model equation to the fast and accurate calculation of a dilute quantum gas is confirmed by calculating the viscosity coefficient of a Bose gas on the basis of the Green-Kubo expression and the shock layer of a dilute Bose gas around a cylinder.

  20. Quantum mechanical cluster calculations of critical scintillationprocesses

    SciTech Connect

    Derenzo, Stephen E.; Klintenberg, Mattias K.; Weber, Marvin J.

    2000-02-22

    This paper describes the use of commercial quantum chemistrycodes to simu-late several critical scintillation processes. The crystalis modeled as a cluster of typically 50 atoms embedded in an array oftypically 5,000 point charges designed to reproduce the electrostaticfield of the infinite crystal. The Schrodinger equation is solved for theground, ionized, and excited states of the system to determine the energyand electron wavefunction. Computational methods for the followingcritical processes are described: (1) the formation and diffusion ofrelaxed holes, (2) the formation of excitons, (3) the trapping ofelectrons and holes by activator atoms, (4) the excitation of activatoratoms, and (5) thermal quenching. Examples include hole diffusion in CsI,the exciton in CsI, the excited state of CsI:Tl, the energy barrier forthe diffusion of relaxed holes in CaF2 and PbF2, and prompt hole trappingby activator atoms in CaF2:Eu and CdS:Te leading to an ultra-fast (<50ps) scintillation risetime.

  1. Quantum mechanical calculations and mineral spectroscopy

    NASA Astrophysics Data System (ADS)

    Kubicki, J. D.

    2006-05-01

    Interpretation of spectra in systems of environmental interest is not generally straightforward due to the lack of close analogs and a clear structure of some components of the system. Computational chemistry can be used as an objective method to test interpretations of spectra. This talk will focus on applying ab initio methods to complement vibrational, NMR, and EXAFS spectroscopic information. Examples of systems studied include phosphate/Fe-hydroxides, arsenate/Al- and Fe-hydroxide, fractured silica surfaces. Phosphate interactions with Fe-hydroxides are important in controlling nutrient availability in soils and transport within streams. In addition, organo-phosphate bonding may be a key attachment mechanism for bacteria at Fe-oxide surfaces. Interpretation of IR spectra is enhanced by model predictions of vibrational frequencies for various surface complexes. Ab initio calculations were used to help explain As(V) and As(III) adsorption behavior onto amorphous Al- and Fe-hydroxides in conjunction with EXAFS measurements. Fractured silica surfaces have been implicated in silicosis. These calculations test structures that could give rise to radical formation on silica surfaces. Calculations to simulate the creation of Si and SiO radical species on sufaces and their subsequent production of OH radicals will be discussed.

  2. Quantum versus classical dynamics in the optical centrifuge

    NASA Astrophysics Data System (ADS)

    Armon, Tsafrir; Friedland, Lazar

    2017-09-01

    The interplay between classical and quantum-mechanical evolution in the optical centrifuge (OC) is discussed. The analysis is based on the quantum-mechanical formalism starting from either the ground state or a thermal ensemble. Two resonant mechanisms are identified, i.e., the classical autoresonance and the quantum-mechanical ladder climbing, yielding different dynamics and rotational excitation efficiencies. The rotating-wave approximation is used to analyze the two resonant regimes in the associated dimensionless two-parameter space and calculate the OC excitation efficiency. The results show good agreement between numerical simulations and theory and are relevant to existing experimental setups.

  3. Mapping quantum state dynamics in spontaneous emission

    PubMed Central

    Naghiloo, M.; Foroozani, N.; Tan, D.; Jadbabaie, A.; Murch, K. W.

    2016-01-01

    The evolution of a quantum state undergoing radiative decay depends on how its emission is detected. If the emission is detected in the form of energy quanta, the evolution is characterized by a quantum jump to a lower energy state. In contrast, detection of the wave nature of the emitted radiation leads to different dynamics. Here, we investigate the diffusive dynamics of a superconducting artificial atom under continuous homodyne detection of its spontaneous emission. Using quantum state tomography, we characterize the correlation between the detected homodyne signal and the emitter's state, and map out the conditional back-action of homodyne measurement. By tracking the diffusive quantum trajectories of the state as it decays, we characterize selective stochastic excitation induced by the choice of measurement basis. Our results demonstrate dramatic differences from the quantum jump evolution associated with photodetection and highlight how continuous field detection can be harnessed to control quantum evolution. PMID:27167893

  4. Dynamics of Quenched Ultracold Quantum Gases

    NASA Astrophysics Data System (ADS)

    Corson, John P.

    Recent advances in the tunability of ultracold atomic gases have created opportunities for studying interesting quantum many-body systems. Fano-Feshbach resonances, in particular, allow experimenters to freely adjust the scattering of atoms by controlling an external magnetic field. By rapidly changing this field near a resonance, it is possible to drive systems out of equilibrium towards novel quantum states where correlations between atoms change dynamically. In this thesis, we take a wave-function-based approach to theoretically examine the response of several interesting systems to suddenly-switched, or "quenched", interactions. We first calculate the time evolution of a Bose-Einstein condensate that is quenched to the unitarity regime, where the scattering length a diverges. Working within the time-dependent variational formalism, we find that the condensate does not deplete as quickly as the usual Bogoliubov theory would suggest. We also make a quantitative prediction for the dynamics of short-range pair correlations, encoded in Tan's contact. We then consider the dynamics of these correlations for quenches to small a, and we find that bound states can cause high-contrast oscillations of the contact. These dynamics can be modeled quantitatively at short times by using a properly-chosen two-body model. Finally, we characterize the nonlocal correlation waves that are generated by an interaction quench in arbitrary dimensionality. Our analysis demonstrates that the large-momentum limit of the post-quench momentum distribution can sometimes include contributions from both the short range and the long range, depending on the quench protocol.

  5. Exact geometries from quantum chemical calculations

    NASA Astrophysics Data System (ADS)

    Cremer, Dieter; Kraka, Elfi; He, Yuan

    2001-06-01

    For seventeen molecules, complete basis set (CBS) geometries are obtained for Møller-Plesset perturbation methods at second (MP2), fourth (MP4), and sixth order (MP6) as well as for the Coupled Cluster methods CCD, CCSD, and CCSD( T). The correlation consistent basis sets cc-pVDZ, cc-pVTZ, and cc-pVQZ were systematically applied and calculated geometries extrapolated to the limit of an infinitely large basis set. MP6 equilibrium geometries are more accurate than MP2 or MP4 geometries at the CBS limit and provide AH bond lengths with an accuracy of 0.001 Å. However, AB bonds are always predicted too long because of the lack of sufficient coupling effects between p-electron correlation at MP6. CCSD( T) provides reasonable AB bond lengths although these are in general too short by 0.003 Å. Due to error cancellation very accurate geometries are obtained at the CCSD( T)/cc-pVTZ and CCSD( T)/cc-pVQZ level of theory. With the help of the accurate equilibrium geometries obtained in this work, several experimentally based geometries could be corrected. The effects of HF-optimized basis sets, diffuse functions or the frozen core approximation on geometry optimizations are discussed. It is emphasized that the use of the cc-pVDZ or any other VDZ+P basis set should be avoided in correlation corrected ab initio calculations.

  6. Quantum regression theorem and non-Markovianity of quantum dynamics

    NASA Astrophysics Data System (ADS)

    Guarnieri, Giacomo; Smirne, Andrea; Vacchini, Bassano

    2014-08-01

    We explore the connection between two recently introduced notions of non-Markovian quantum dynamics and the validity of the so-called quantum regression theorem. While non-Markovianity of a quantum dynamics has been defined looking at the behavior in time of the statistical operator, which determines the evolution of mean values, the quantum regression theorem makes statements about the behavior of system correlation functions of order two and higher. The comparison relies on an estimate of the validity of the quantum regression hypothesis, which can be obtained exactly evaluating two-point correlation functions. To this aim we consider a qubit undergoing dephasing due to interaction with a bosonic bath, comparing the exact evaluation of the non-Markovianity measures with the violation of the quantum regression theorem for a class of spectral densities. We further study a photonic dephasing model, recently exploited for the experimental measurement of non-Markovianity. It appears that while a non-Markovian dynamics according to either definition brings with itself violation of the regression hypothesis, even Markovian dynamics can lead to a failure of the regression relation.

  7. Can the ring polymer molecular dynamics method be interpreted as real time quantum dynamics?

    SciTech Connect

    Jang, Seogjoo; Sinitskiy, Anton V.; Voth, Gregory A.

    2014-04-21

    The ring polymer molecular dynamics (RPMD) method has gained popularity in recent years as a simple approximation for calculating real time quantum correlation functions in condensed media. However, the extent to which RPMD captures real dynamical quantum effects and why it fails under certain situations have not been clearly understood. Addressing this issue has been difficult in the absence of a genuine justification for the RPMD algorithm starting from the quantum Liouville equation. To this end, a new and exact path integral formalism for the calculation of real time quantum correlation functions is presented in this work, which can serve as a rigorous foundation for the analysis of the RPMD method as well as providing an alternative derivation of the well established centroid molecular dynamics method. The new formalism utilizes the cyclic symmetry of the imaginary time path integral in the most general sense and enables the expression of Kubo-transformed quantum time correlation functions as that of physical observables pre-averaged over the imaginary time path. Upon filtering with a centroid constraint function, the formulation results in the centroid dynamics formalism. Upon filtering with the position representation of the imaginary time path integral, we obtain an exact quantum dynamics formalism involving the same variables as the RPMD method. The analysis of the RPMD approximation based on this approach clarifies that an explicit quantum dynamical justification does not exist for the use of the ring polymer harmonic potential term (imaginary time kinetic energy) as implemented in the RPMD method. It is analyzed why this can cause substantial errors in nonlinear correlation functions of harmonic oscillators. Such errors can be significant for general correlation functions of anharmonic systems. We also demonstrate that the short time accuracy of the exact path integral limit of RPMD is of lower order than those for finite discretization of path. The

  8. Quantum Molecular Dynamics Simulations of Nanotube Tip Assisted Reactions

    NASA Technical Reports Server (NTRS)

    Menon, Madhu

    1998-01-01

    In this report we detail the development and application of an efficient quantum molecular dynamics computational algorithm and its application to the nanotube-tip assisted reactions on silicon and diamond surfaces. The calculations shed interesting insights into the microscopic picture of tip surface interactions.

  9. Multi-million atom electronic structure calculations for quantum dots

    NASA Astrophysics Data System (ADS)

    Usman, Muhammad

    Quantum dots grown by self-assembly process are typically constructed by 50,000 to 5,000,000 structural atoms which confine a small, countable number of extra electrons or holes in a space that is comparable in size to the electron wavelength. Under such conditions quantum dots can be interpreted as artificial atoms with the potential to be custom tailored to new functionality. In the past decade or so, these nanostructures have attracted significant experimental and theoretical attention in the field of nanoscience. The new and tunable optical and electrical properties of these artificial atoms have been proposed in a variety of different fields, for example in communication and computing systems, medical and quantum computing applications. Predictive and quantitative modeling and simulation of these structures can help to narrow down the vast design space to a range that is experimentally affordable and move this part of nanoscience to nano-Technology. Modeling of such quantum dots pose a formidable challenge to theoretical physicists because: (1) Strain originating from the lattice mismatch of the materials penetrates deep inside the buffer surrounding the quantum dots and require large scale (multi-million atom) simulations to correctly capture its effect on the electronic structure, (2) The interface roughness, the alloy randomness, and the atomistic granularity require the calculation of electronic structure at the atomistic scale. Most of the current or past theoretical calculations are based on continuum approach such as effective mass approximation or k.p modeling capturing either no or one of the above mentioned effects, thus missing some of the essential physics. The Objectives of this thesis are: (1) to model and simulate the experimental quantum dot topologies at the atomistic scale; (2) to theoretically explore the essential physics i.e. long range strain, linear and quadratic piezoelectricity, interband optical transition strengths, quantum confined

  10. Detailed discussions and calculations of quantum Regge calculus of Einstein-Cartan theory

    SciTech Connect

    Xue Shesheng

    2010-09-15

    This article presents detailed discussions and calculations of the recent paper 'Quantum Regge calculus of Einstein-Cartan theory' in [9]. The Euclidean space-time is discretized by a four-dimensional simplicial complex. We adopt basic tetrad and spin-connection fields to describe the simplicial complex. By introducing diffeomorphism and local Lorentz invariant holonomy fields, we construct a regularized Einstein-Cartan theory for studying the quantum dynamics of the simplicial complex and fermion fields. This regularized Einstein-Cartan action is shown to properly approach to its continuum counterpart in the continuum limit. Based on the local Lorentz invariance, we derive the dynamical equations satisfied by invariant holonomy fields. In the mean-field approximation, we show that the averaged size of 4-simplex, the element of the simplicial complex, is larger than the Planck length. This formulation provides a theoretical framework for analytical calculations and numerical simulations to study the quantum Einstein-Cartan theory.

  11. Partial hydrodynamic representation of quantum molecular dynamics

    NASA Astrophysics Data System (ADS)

    Gu, Bing; Franco, Ignacio

    2017-05-01

    A hybrid method is proposed to propagate system-bath quantum dynamics that use both basis functions and coupled quantum trajectories. In it, the bath is represented with an ensemble of Bohmian trajectories while the system degrees of freedom are accounted through reduced density matrices. By retaining the Hilbert space structure for the system, the method is able to capture interference processes that are challenging to describe in Bohmian dynamics due to singularities that these processes introduce in the quantum potential. By adopting quantum trajectories to represent the bath, the method beats the exponential scaling of the computational cost with the bath size. This combination makes the method suitable for large-scale ground and excited state fully quantum molecular dynamics simulations. Equations of motion for the quantum trajectories and reduced density matrices are derived from the Schrödinger equation and a computational algorithm to solve these equations is proposed. Through computations in two-dimensional model systems, the method is shown to offer an accurate description of subsystem observables and of quantum decoherence, which is difficult to obtain when the quantum nature of the bath is ignored. The scaling of the method is demonstrated using a model with 21 degrees of freedom. The limit of independent trajectories is recovered when the mass of bath degrees of freedom is much larger than the one of the system, in agreement with mixed quantum-classical descriptions.

  12. Conditional measurements as probes of quantum dynamics

    SciTech Connect

    Siddiqui, Shabnam; Erenso, Daniel; Vyas, Reeta; Singh, Surendra

    2003-06-01

    We discuss conditional measurements as probes of quantum dynamics and show that they provide different ways to characterize quantum fluctuations. We illustrate this by considering the light from a subthreshold degenerate parametric oscillator. Analytic results and curves are presented to illustrate the behavior.

  13. Quantum Dynamics Simulations for Modeling Experimental Pump-Probe Measurements

    NASA Astrophysics Data System (ADS)

    Pearson, Brett; Nayyar, Sahil; Liss, Kyle; Weinacht, Thomas

    2016-05-01

    Time-resolved studies of quantum dynamics have benefited greatly from developments in ultrafast table-top and free electron lasers. Advances in computer software and hardware have lowered the barrier for performing calculations such that relatively simple simulations allow for direct comparison with experimental results. We describe here a set of quantum dynamics calculations in low-dimensional molecular systems. The calculations incorporate coupled electronic-nuclear dynamics, including two interactions with an applied field and nuclear wave packet propagation. The simulations were written and carried out by undergraduates as part of a senior research project, with the specific goal of allowing for detailed interpretation of experimental pump-probe data (in additional to the pedagogical value).

  14. Nonadiabatic quantum dynamics of C(1D)+H2→CH+H: coupled-channel calculations including Renner-Teller and Coriolis terms.

    PubMed

    Defazio, Paolo; Bussery-Honvault, Béatrice; Honvault, Pascal; Petrongolo, Carlo

    2011-09-21

    The Renner-Teller (RT) coupled-channel dynamics for the C((1)D)+H(2)(X(1)Σ(g) (+))→CH(X(2)Π)+H((2)S) reaction has been investigated for the first time, considering the first two singlet states ã̃(1)A' and b(1)A'' of CH(2) dissociating into the products and RT couplings, evaluated through the ab initio matrix elements of the electronic angular momentum. We have obtained initial-state-resolved probabilities, cross sections and thermal rate constants via the real wavepacket method for both coupled electronic states. In contrast to the N((2)D)+H(2)(X(1)Σ(g)(+)) system, RT effects tend to reduce probabilities, cross sections, and rate constants in the low energy range compared to Born-Oppenheimer (BO) ones, due to the presence of a repulsive RT barrier in the effective potentials and to long-lived resonances. Furthermore, contrary to BO results, the rate constants have a positive temperature dependence in the 100-400 K range. The two-state RT rate constant at 300 K, lower than the BO one, remains inside the error bars of the experimental value.

  15. Efficient free energy calculations of quantum systems through computer simulations

    NASA Astrophysics Data System (ADS)

    Antonelli, Alex; Ramirez, Rafael; Herrero, Carlos; Hernandez, Eduardo

    2009-03-01

    In general, the classical limit is assumed in computer simulation calculations of free energy. This approximation, however, is not justifiable for a class of systems in which quantum contributions for the free energy cannot be neglected. The inclusion of quantum effects is important for the determination of reliable phase diagrams of these systems. In this work, we present a new methodology to compute the free energy of many-body quantum systems [1]. This methodology results from the combination of the path integral formulation of statistical mechanics and efficient non-equilibrium methods to estimate free energy, namely, the adiabatic switching and reversible scaling methods. A quantum Einstein crystal is used as a model to show the accuracy and reliability the methodology. This new method is applied to the calculation of solid-liquid coexistence properties of neon. Our findings indicate that quantum contributions to properties such as, melting point, latent heat of fusion, entropy of fusion, and slope of melting line can be up to 10% of the calculated values using the classical approximation. [1] R. M. Ramirez, C. P. Herrero, A. Antonelli, and E. R. Hernández, Journal of Chemical Physics 129, 064110 (2008)

  16. Robust dynamical decoupling for quantum computing and quantum memory.

    PubMed

    Souza, Alexandre M; Alvarez, Gonzalo A; Suter, Dieter

    2011-06-17

    Dynamical decoupling (DD) is a popular technique for protecting qubits from the environment. However, unless special care is taken, experimental errors in the control pulses used in this technique can destroy the quantum information instead of preserving it. Here, we investigate techniques for making DD sequences robust against different types of experimental errors while retaining good decoupling efficiency in a fluctuating environment. We present experimental data from solid-state nuclear spin qubits and introduce a new DD sequence that is suitable for quantum computing and quantum memory.

  17. Exploring the dynamics of reaction C(3P) + C2H4 with crossed beam/photoionization experiments and quantum chemical calculations.

    PubMed

    Chin, Chih-Hao; Chen, Wei-Kan; Huang, Wen-Jian; Lin, Yi-Cheng; Lee, Shih-Huang

    2012-07-26

    We investigated the title reaction at collision energy 3.5 kcal mol(-1) in a crossed molecular beam apparatus using undulator radiation as an ionization source. Time-of-flight (TOF) spectra of product C(3)H(3) were measured in laboratory angles from 20° to 100° using two photoionization energies 9.5 and 11.6 eV. These two sets of experimental data exhibit almost the same TOF distributions and laboratory angular distributions. From the best simulation, seven angle-specific kinetic-energy distributions and a nearly isotropic angular distribution are derived for product channel C(3)H(3) + H that has an average kinetic-energy release of 15.5 kcal mol(-1), corresponding to an average internal energy of 33.3 kcal mol(-1) in C(3)H(3). Furthermore, TOF spectra of product C(3)H(3) were measured at laboratory angle 52° with ionizing photon energies from 7 to 12 eV. The appearance of TOF spectra remains almost the same, indicating that a species exclusively contributes to product C(3)H(3); the species is identified as H(2)CCCH (propargyl) based on the ionization energy of 8.6 ± 0.2 eV and the maximal kinetic-energy release of 49 kcal mol(-1). Theoretical calculations indicate that the rapid inversion mechanism and rotation in intermediate H(2)CCCH(2) can result in a forward-backward symmetric angular distribution for product C(3)H(3) + H. The present work avoids the interference of reactions of C((1)D) and C(2) radicals with C(2)H(4) and rules out the probability of production of other isomers like c-C(3)H(3) and H(3)CCC proposed in the previous work at least at the investigated collision energy.

  18. Quantum dynamics of the abstraction reaction of H with cyclopropane.

    PubMed

    Shan, Xiao; Clary, David C

    2014-10-30

    The dynamics of the abstraction reaction of H atoms with the cyclopropane molecule is studied using quantum mechanical scattering theory. The quantum scattering calculations are performed in hyperspherical coordinates with a two-dimensional (2D) potential energy surface. The ab initio energy calculations are carried out with CCSD(T)-F12a/cc-pVTZ-F12 level of theory with the geometry and frequency calculations at the MP2/cc-pVTZ level. The contribution to the potential energy surface from the spectator modes is included as the projected zero-point energy correction to the ab initio energy. The 2D surface is fitted with a 29-parameter double Morse potential. An R-matrix propagation scheme is carried out to solve the close-coupled equations. The adiabatic energy barrier and reaction enthalpy are compared with high level computational calculations as well as experimental data. The calculated reaction rate constants shows very good agreement when compared with the experimental data, especially at lower temperature highlighting the importance of quantum tunnelling. The reaction probabilities are also presented and discussed. The special features of performing quantum dynamics calculation on the chemical reaction of a cyclic molecule are discussed.

  19. Looking into DNA breathing dynamics via quantum physics.

    PubMed

    Wu, Lian-Ao; Wu, Stephen S; Segal, Dvira

    2009-06-01

    We study generic aspects of bubble dynamics in DNA under time-dependent perturbations, for example, temperature change, by mapping the associated Fokker-Planck equation to a quantum time-dependent Schrödinger equation with imaginary time. In the static case we show that the eigenequation is exactly the same as that of the beta-deformed nuclear liquid drop model, without the issue of noninteger angular momentum. A universal breathing dynamics is demonstrated by using an approximate method in quantum mechanics. The calculated bubble autocorrelation function qualitatively agrees with experimental data. Under time-dependent modulations, utilizing the adiabatic approximation, bubble properties reveal memory effects.

  20. Efficient hierarchical Liouville space propagator to quantum dissipative dynamics.

    PubMed

    Shi, Qiang; Chen, Liping; Nan, Guangjun; Xu, Rui-Xue; Yan, Yijing

    2009-02-28

    We propose an efficient method to propagate the hierarchical quantum master equations based on a reformulation of the original formalism and the incorporation of a filtering algorithm that automatically truncates the hierarchy with a preselected tolerance. The new method is applied to calculate electron transfer dynamics in a spin-boson model and the absorption spectra of an excitonic dimmer. The proposed method significantly reduces the number of auxiliary density operators used in the hierarchical equation approach and thus provides an efficient way capable of studying real time dynamics of non-Markovian quantum dissipative systems in strong system-bath coupling and low temperature regimes.

  1. Semiclassical description of hyperfine interaction in calculating chemically induced dynamic nuclear polarization in weak magnetic fields

    SciTech Connect

    Purtov, P.A.; Salikhov, K.M.

    1987-09-01

    Semiclassical HFI description is applicable to calculating the integral CIDNP effect in weak fields. The HFI has been calculated for radicals with sufficiently numerous magnetically equivalent nuclei (n greater than or equal to 5) in satisfactory agreement with CIDNP calculations based on quantum-mechanical description of radical-pair spin dynamics.

  2. The quantum Rabi model: solution and dynamics

    NASA Astrophysics Data System (ADS)

    Xie, Qiongtao; Zhong, Honghua; Batchelor, Murray T.; Lee, Chaohong

    2017-03-01

    This article presents a review of recent developments on various aspects of the quantum Rabi model. Particular emphasis is given on the exact analytic solution obtained in terms of confluent Heun functions. The analytic solutions for various generalisations of the quantum Rabi model are also discussed. Results are also reviewed on the level statistics and the dynamics of the quantum Rabi model. The article concludes with an introductory overview of several experimental realisations of the quantum Rabi model. An outlook towards future developments is also given.

  3. Quantum entropies, Schur concavity and dynamical semigroups

    NASA Astrophysics Data System (ADS)

    Aniello, Paolo

    2017-01-01

    Entropy plays a fundamental role in several branches of physics. In the quantum setting, one usually considers the von Neumann entropy, but other useful quantities have been proposed in the literature; e.g., the Rényi and the Tsallis entropies. The evolution of an open quantum system, described by a semigroup of dynamical maps (in short, a dynamical semigroup), may decrease a quantum entropy, for some initial condition. We will discuss various characterizations of those dynamical semigroups that, for every initial condition, do not decrease a general class of quantum entropies, which is defined using the notion of Schur concavity of a function. We will not assume that such a dynamical semigroup be completely positive, the physical justification of this condition being controversial. Therefore, we will consider semigroups of trace-preserving, positive — but not necessarily completely positive — linear maps. We will next focus on a special class of (completely positive) dynamical semigroups, the twirling semigroups, having applications in quantum information science. We will argue that the whole class of dynamical semigroups that do not decrease a quantum entropy can be obtained as a suitable generalization of the twirling semigroups.

  4. What is dynamics in quantum gravity?

    NASA Astrophysics Data System (ADS)

    Małkiewicz, Przemysław

    2017-10-01

    The appearance of the Hamiltonian constraint in the canonical formalism for general relativity reflects the lack of a fixed external time. The dynamics of general relativistic systems can be expressed with respect to an arbitrarily chosen internal degree of freedom, the so-called internal clock. We investigate the way in which the choice of internal clock determines the quantum dynamics and how much different quantum dynamics induced by different clocks are. We develop our method of comparison by extending the Hamilton–Jacobi theory of contact transformations to include a new type of transformation which transforms both the canonical variables and the internal clock. We employ our method to study the quantum dynamics of the Friedmann–Lemaitre model and obtain semiclassical corrections to the classical dynamics, which depend on the choice of internal clock. For a unique quantisation map we find the abundance of inequivalent semiclassical corrections induced by quantum dynamics taking place in different internal clocks. It follows that the concepts like minimal volume, maximal curvature and the number of quantum bounces, often used to describe quantum effects in cosmological models, depend on the choice of internal clock.

  5. Comparison of calculated with measured dynamic aperture

    SciTech Connect

    Zimmermann, F.

    1994-06-01

    The measured dynamic aperture of the HERA proton ring and the value expected from simulation studies agree within a factor of 2. A better agreement is achieved if a realistic tune modulation is included in the simulation. The approximate threshold of tune-modulation induced diffusion can be calculated analytically. Its value is in remarkable agreement with the dynamic aperture measured. The calculation is based on parameters of resonances through order 11 which are computed using differential-algebra methods and normal-form algorithms. Modulational diffusion in conjunction with drifting machine parameters appears to be the most important transverse diffusion process.

  6. Efficient method for the calculation of dissipative quantum transport in quantum cascade lasers.

    PubMed

    Greck, Peter; Birner, Stefan; Huber, Bernhard; Vogl, Peter

    2015-03-09

    We present a novel and very efficient method for calculating quantum transport in quantum cascade lasers (QCLs). It follows the nonequilibrium Green's function (NEGF) framework but sidesteps the calculation of lesser self-energies by replacing them by a quasi-equilibrium expression. This method generalizes the phenomenological Büttiker probe model by taking into account individual scattering mechanisms. It is orders of magnitude more efficient than a fully self-consistent NEGF calculation for realistic devices. We apply this method to a new THz QCL design which works up to 250 K - according to our calculations.

  7. Dynamical typicality of embedded quantum systems

    NASA Astrophysics Data System (ADS)

    Ithier, Grégoire; Benaych-Georges, Florent

    2017-07-01

    We consider the dynamics of an arbitrary quantum system coupled to a large arbitrary and fully quantum-mechanical environment through a random interaction. We establish analytically and check numerically the typicality of this dynamics, in other words, the fact that the reduced density matrix of the system has a self-averaging property. This phenomenon, which lies in a generalized central limit theorem, justifies rigorously averaging procedures over certain classes of random interactions and can explain the absence of sensitivity to microscopic details of irreversible processes, such as thermalization. It provides more generally an ergodic principle for embedded quantum systems.

  8. Carrier Dynamics in Quantum Cascade Lasers

    NASA Astrophysics Data System (ADS)

    Harrison, P.; Indjin, D.; Jovanović, V. D.; Mirčetić, A.; Ikonić, Z.; Kelsall, R. W.; McTavish, J.; Savić, I.; Vukmirović, N.; Milanović, V.

    2005-01-01

    A fully quantum-mechanical model for carrier scattering transport in semiconductor intersubband devices was applied to modelling of carrier dynamics in quantum cascade lasers. The standard model uses the envelope function and effective mass approximations to solve electron band structure under an applied bias. The k·p model has been employed in p-type systems where the more complex band structure requires it. The resulting wave functions are then used to evaluate all relevant carrier-phonon, carrier-carrier and alloy scattering rates from each quantised state to all others within the same and the neighbouring period. This piece of information is then used to construct a rate equation for the equilibrium carrier density in each subband and this set of coupled rate equations are solved self-consistently to obtain the carrier density in each eigenstate. The latter is a fundamental description of the device and can be used to calculate the current density and gain as a function of the applied bias and temperature, which in turn yields the threshold current and expected temperature dependence of the device characteristics. A recent extension which includes a further iteration of an energy balance equation also yields the electron (or hole) temperature over the subbands. This paper will review the method and describe its application to mid-infrared and terahertz, GaAs, GaN, and SiGe cascade laser designs.

  9. Subfemtosecond quantum nuclear dynamics in water isotopomers.

    PubMed

    Rao, B Jayachander; Varandas, A J C

    2015-05-21

    Subfemtosecond quantum dynamics studies of all water isotopomers in the X̃ (2)B1 and à (2)A1 electronic states of the cation formed by Franck-Condon ionization of the neutral ground electronic state are reported. Using the ratio of the autocorrelation functions for the isotopomers as obtained from the solution of the time-dependent Schrödinger equation in a grid representation, high-order harmonic generation signals are calculated as a function of time. The results are found to be in agreement with the available experimental findings and with our earlier study for D2O(+)/H2O(+). Maxima are predicted in the autocorrelation function ratio at various times. Their origin and occurrence is explained by calculating expectation values of the bond lengths and bond angle of the water isotopomers as a function of time. The values so calculated for the (2)B1 and (2)A1 electronic states of the cation show quasiperiodic oscillations that can be associated with the time at which the nuclear wave packet reaches the minima of the potential energy surface, there being responsible for the peaks in the HHG signals.

  10. Quantum mechanical calculation of Rydberg-Rydberg autoionization rates

    NASA Astrophysics Data System (ADS)

    Kiffner, Martin; Ceresoli, Davide; Li, Wenhui; Jaksch, Dieter

    2016-10-01

    We present quantum mechanical calculations of autoionization rates for two rubidium Rydberg atoms with weakly overlapping electron clouds. We neglect exchange effects and consider tensor products of independent atom states forming an approximate basis of the two-electron state space. We consider large sets of two-atom states with randomly chosen quantum numbers and find that the charge overlap between the two Rydberg electrons allows one to characterise the magnitude of the autoionization rates. If the electron clouds overlap by more than one percent, the autoionization rates increase approximately exponentially with the charge overlap. This finding is independent of the energy of the initial state.

  11. Computational approach for calculating bound states in quantum field theory

    NASA Astrophysics Data System (ADS)

    Lv, Q. Z.; Norris, S.; Brennan, R.; Stefanovich, E.; Su, Q.; Grobe, R.

    2016-09-01

    We propose a nonperturbative approach to calculate bound-state energies and wave functions for quantum field theoretical models. It is based on the direct diagonalization of the corresponding quantum field theoretical Hamiltonian in an effectively discretized and truncated Hilbert space. We illustrate this approach for a Yukawa-like interaction between fermions and bosons in one spatial dimension and show where it agrees with the traditional method based on the potential picture and where it deviates due to recoil and radiative corrections. This method permits us also to obtain some insight into the spatial characteristics of the distribution of the fermions in the ground state, such as the bremsstrahlung-induced widening.

  12. Efficient hybrid-symbolic methods for quantum mechanical calculations

    NASA Astrophysics Data System (ADS)

    Scott, T. C.; Zhang, Wenxing

    2015-06-01

    We present hybrid symbolic-numerical tools to generate optimized numerical code for rapid prototyping and fast numerical computation starting from a computer algebra system (CAS) and tailored to any given quantum mechanical problem. Although a major focus concerns the quantum chemistry methods of H. Nakatsuji which has yielded successful and very accurate eigensolutions for small atoms and molecules, the tools are general and may be applied to any basis set calculation with a variational principle applied to its linear and non-linear parameters.

  13. Quantum correlation dynamics in photosynthetic processes assisted by molecular vibrations

    SciTech Connect

    Giorgi, G.L.; Roncaglia, M.; Raffa, F.A.; Genovese, M.

    2015-10-15

    During the long course of evolution, nature has learnt how to exploit quantum effects. In fact, recent experiments reveal the existence of quantum processes whose coherence extends over unexpectedly long time and space ranges. In particular, photosynthetic processes in light-harvesting complexes display a typical oscillatory dynamics ascribed to quantum coherence. Here, we consider the simple model where a dimer made of two chromophores is strongly coupled with a quasi-resonant vibrational mode. We observe the occurrence of wide oscillations of genuine quantum correlations, between electronic excitations and the environment, represented by vibrational bosonic modes. Such a quantum dynamics has been unveiled through the calculation of the negativity of entanglement and the discord, indicators widely used in quantum information for quantifying the resources needed to realize quantum technologies. We also discuss the possibility of approximating additional weakly-coupled off-resonant vibrational modes, simulating the disturbances induced by the rest of the environment, by a single vibrational mode. Within this approximation, one can show that the off-resonant bath behaves like a classical source of noise.

  14. Dynamical Correspondence in a Generalized Quantum Theory

    NASA Astrophysics Data System (ADS)

    Niestegge, Gerd

    2015-05-01

    In order to figure out why quantum physics needs the complex Hilbert space, many attempts have been made to distinguish the C*-algebras and von Neumann algebras in more general classes of abstractly defined Jordan algebras (JB- and JBW-algebras). One particularly important distinguishing property was identified by Alfsen and Shultz and is the existence of a dynamical correspondence. It reproduces the dual role of the selfadjoint operators as observables and generators of dynamical groups in quantum mechanics. In the paper, this concept is extended to another class of nonassociative algebras, arising from recent studies of the quantum logics with a conditional probability calculus and particularly of those that rule out third-order interference. The conditional probability calculus is a mathematical model of the Lüders-von Neumann quantum measurement process, and third-order interference is a property of the conditional probabilities which was discovered by Sorkin (Mod Phys Lett A 9:3119-3127, 1994) and which is ruled out by quantum mechanics. It is shown then that the postulates that a dynamical correspondence exists and that the square of any algebra element is positive still characterize, in the class considered, those algebras that emerge from the selfadjoint parts of C*-algebras equipped with the Jordan product. Within this class, the two postulates thus result in ordinary quantum mechanics using the complex Hilbert space or, vice versa, a genuine generalization of quantum theory must omit at least one of them.

  15. Quantum fluctuations in beam dynamics.

    SciTech Connect

    Kim, K.-J.

    1998-06-04

    Quantum effects could become important for particle and photon beams used in high-luminosity and high brightness applications in the current and next generation accelerators and radiation sources. This paper is a review of some of these effects.

  16. Infinite variance in fermion quantum Monte Carlo calculations

    NASA Astrophysics Data System (ADS)

    Shi, Hao; Zhang, Shiwei

    2016-03-01

    For important classes of many-fermion problems, quantum Monte Carlo (QMC) methods allow exact calculations of ground-state and finite-temperature properties without the sign problem. The list spans condensed matter, nuclear physics, and high-energy physics, including the half-filled repulsive Hubbard model, the spin-balanced atomic Fermi gas, and lattice quantum chromodynamics calculations at zero density with Wilson Fermions, and is growing rapidly as a number of problems have been discovered recently to be free of the sign problem. In these situations, QMC calculations are relied on to provide definitive answers. Their results are instrumental to our ability to understand and compute properties in fundamental models important to multiple subareas in quantum physics. It is shown, however, that the most commonly employed algorithms in such situations have an infinite variance problem. A diverging variance causes the estimated Monte Carlo statistical error bar to be incorrect, which can render the results of the calculation unreliable or meaningless. We discuss how to identify the infinite variance problem. An approach is then proposed to solve the problem. The solution does not require major modifications to standard algorithms, adding a "bridge link" to the imaginary-time path integral. The general idea is applicable to a variety of situations where the infinite variance problem may be present. Illustrative results are presented for the ground state of the Hubbard model at half-filling.

  17. Infinite variance in fermion quantum Monte Carlo calculations.

    PubMed

    Shi, Hao; Zhang, Shiwei

    2016-03-01

    For important classes of many-fermion problems, quantum Monte Carlo (QMC) methods allow exact calculations of ground-state and finite-temperature properties without the sign problem. The list spans condensed matter, nuclear physics, and high-energy physics, including the half-filled repulsive Hubbard model, the spin-balanced atomic Fermi gas, and lattice quantum chromodynamics calculations at zero density with Wilson Fermions, and is growing rapidly as a number of problems have been discovered recently to be free of the sign problem. In these situations, QMC calculations are relied on to provide definitive answers. Their results are instrumental to our ability to understand and compute properties in fundamental models important to multiple subareas in quantum physics. It is shown, however, that the most commonly employed algorithms in such situations have an infinite variance problem. A diverging variance causes the estimated Monte Carlo statistical error bar to be incorrect, which can render the results of the calculation unreliable or meaningless. We discuss how to identify the infinite variance problem. An approach is then proposed to solve the problem. The solution does not require major modifications to standard algorithms, adding a "bridge link" to the imaginary-time path integral. The general idea is applicable to a variety of situations where the infinite variance problem may be present. Illustrative results are presented for the ground state of the Hubbard model at half-filling.

  18. Calculation of Cross Sections in Electron-Nuclear Dynamics

    NASA Astrophysics Data System (ADS)

    Cabrera-Trujillo, R.; Sabin, John R.; Deumens, E.; Öhrn, Y.

    In this work, we present an overview of the study of total and differential cross section calculations within the electron-nuclear dynamics (END). END is a method to solve the time-dependent Schrödinger equation in a non-adiabatic approach to direct dynamics. The method takes advantage of a coherent state representation of the molecular wave function. A quantum-mechanical Lagrangian formulation is employed to approximate the Schrödinger equation, via the time-dependent variational principle, to a set of coupled first-order differential equations in time for the END. We obtain the final wave function for the system allowing the determination of collisional properties of interest, as for example, deflection functions, charge exchange probabilities and amplitudes, and differential cross sections. We discuss the use and selection of basis sets for both the electronic description of the colliding systems as well as for their importance in the description of electron capture. As quantum effects are important in many cases and lacking for classical nuclei, we discuss the Schiff methodology and its advantages over other traditional methods for including semiclassical corrections. Time-lapse rendering of the dynamics of the participating electrons and atomic nuclei provides for a detailed view of dynamical and reactive processes. Comparison to experimental and other theoretical results is provided where appropriate data are available.

  19. Quantum simulation of molecular interaction and dynamics at surfaces

    NASA Astrophysics Data System (ADS)

    Ding, Zi-Jing; Jiao, Yang; Meng, Sheng

    2011-09-01

    The interaction between molecules and solid surfaces plays important roles in various applications, including catalysis, sensors, nanoelectronics, and solar cells. Surprisingly, a full understanding of molecule-surface interaction at the quantum mechanical level has not been achieved even for very simple molecules, such as water. In this mini-review, we report recent progresses and current status of studies on interaction between representative molecules and surfaces. Taking water/metal, DNA bases/carbon nanotube, and organic dye molecule/oxide as examples, we focus on the understanding on the microstructure, electronic property, and electron-ion dynamics involved in these systems obtained from first-principles quantum mechanical calculations. We find that a quantum mechanical description of molecule-surface interaction is essential for understanding interface phenomenon at the microscopic level, such as wetting. New theoretical developments, including van der Waals density functional and quantum nuclei treatment, improve further our understanding of surface interactions.

  20. Quantum Monte Carlo calculations with chiral effective field theory interactions.

    PubMed

    Gezerlis, A; Tews, I; Epelbaum, E; Gandolfi, S; Hebeler, K; Nogga, A; Schwenk, A

    2013-07-19

    We present the first quantum Monte Carlo (QMC) calculations with chiral effective field theory (EFT) interactions. To achieve this, we remove all sources of nonlocality, which hamper the inclusion in QMC calculations, in nuclear forces to next-to-next-to-leading order. We perform auxiliary-field diffusion Monte Carlo (AFDMC) calculations for the neutron matter energy up to saturation density based on local leading-order, next-to-leading order, and next-to-next-to-leading order nucleon-nucleon interactions. Our results exhibit a systematic order-by-order convergence in chiral EFT and provide nonperturbative benchmarks with theoretical uncertainties. For the softer interactions, perturbative calculations are in excellent agreement with the AFDMC results. This work paves the way for QMC calculations with systematic chiral EFT interactions for nuclei and nuclear matter, for testing the perturbativeness of different orders, and allows for matching to lattice QCD results by varying the pion mass.

  1. Spectrum analysis with quantum dynamical systems

    NASA Astrophysics Data System (ADS)

    Ng, Shilin; Ang, Shan Zheng; Wheatley, Trevor A.; Yonezawa, Hidehiro; Furusawa, Akira; Huntington, Elanor H.; Tsang, Mankei

    2016-04-01

    Measuring the power spectral density of a stochastic process, such as a stochastic force or magnetic field, is a fundamental task in many sensing applications. Quantum noise is becoming a major limiting factor to such a task in future technology, especially in optomechanics for temperature, stochastic gravitational wave, and decoherence measurements. Motivated by this concern, here we prove a measurement-independent quantum limit to the accuracy of estimating the spectrum parameters of a classical stochastic process coupled to a quantum dynamical system. We demonstrate our results by analyzing the data from a continuous-optical-phase-estimation experiment and showing that the experimental performance with homodyne detection is close to the quantum limit. We further propose a spectral photon-counting method that can attain quantum-optimal performance for weak modulation and a coherent-state input, with an error scaling superior to that of homodyne detection at low signal-to-noise ratios.

  2. PT-Symmetric Quantum Liouvillean Dynamics

    NASA Astrophysics Data System (ADS)

    Prosen, Tomaž

    2012-08-01

    We discuss a combination of unitary and antiunitary symmetry of quantum Liouvillean dynamics, in the context of open quantum systems, which implies a D2 symmetry of the complex Liouvillean spectrum. For sufficiently weak system-bath coupling, it implies a uniform decay rate for all coherences, i.e., off-diagonal elements of the system’s density matrix taken in the eigenbasis of the Hamiltonian. As an example, we discuss symmetrically boundary driven open XXZ spin 1/2 chains.

  3. Quantum model for the price dynamics

    NASA Astrophysics Data System (ADS)

    Choustova, Olga

    2008-10-01

    We apply methods of quantum mechanics to mathematical modelling of price dynamics in a financial market. We propose to describe behavioral financial factors (e.g., expectations of traders) by using the pilot wave (Bohmian) model of quantum mechanics. Our model is a quantum-like model of the financial market, cf. with works of W. Segal, I.E. Segal, E. Haven. In this paper we study the problem of smoothness of price-trajectories in the Bohmian financial model. We show that even the smooth evolution of the financial pilot wave [psi](t,x) (representing expectations of traders) can induce jumps of prices of shares.

  4. Efficient quantum computing of complex dynamics.

    PubMed

    Benenti, G; Casati, G; Montangero, S; Shepelyansky, D L

    2001-11-26

    We propose a quantum algorithm which uses the number of qubits in an optimal way and efficiently simulates a physical model with rich and complex dynamics described by the quantum sawtooth map. The numerical study of the effect of static imperfections in the quantum computer hardware shows that the main elements of the phase space structures are accurately reproduced up to a time scale which is polynomial in the number of qubits. The errors generated by these imperfections are more significant than the errors of random noise in gate operations.

  5. Origin of Dynamical Quantum Non-locality

    NASA Astrophysics Data System (ADS)

    Pachon, Cesar E.; Pachon, Leonardo A.

    2014-03-01

    Non-locality is one of the hallmarks of quantum mechanics and is responsible for paradigmatic features such as entanglement and the Aharonov-Bohm effect. Non-locality comes in two ``flavours'': a kinematic non-locality- arising from the structure of the Hilbert space- and a dynamical non-locality- arising from the quantum equations of motion-. Kinematic non-locality is unable to induce any change in the probability distributions, so that the ``action-at-a-distance'' cannot manifest. Conversely, dynamical non-locality does create explicit changes in probability, though in a ``causality-preserving'' manner. The origin of non-locality of quantum measurements and its relations to the fundamental postulates of quantum mechanics, such as the uncertainty principle, have been only recently elucidated. Here we trace the origin of dynamical non-locality to the superposition principle. This relation allows us to establish and identify how the uncertainty and the superposition principles determine the non-local character of the outcome of a quantum measurement. Being based on group theoretical and path integral formulations, our formulation admits immediate generalizations and extensions to to, e.g., quantum field theory. This work was supported by the Departamento Administrativo de Ciencia, Tecnologia e Innovacion -COLCIENCIAS- of Colombia under the grant number 111556934912.

  6. Quantum Simulation for Open-System Dynamics

    NASA Astrophysics Data System (ADS)

    Wang, Dong-Sheng; de Oliveira, Marcos Cesar; Berry, Dominic; Sanders, Barry

    2013-03-01

    Simulations are essential for predicting and explaining properties of physical and mathematical systems yet so far have been restricted to classical and closed quantum systems. Although forays have been made into open-system quantum simulation, the strict algorithmic aspect has not been explored yet is necessary to account fully for resource consumption to deliver bounded-error answers to computational questions. An open-system quantum simulator would encompass classical and closed-system simulation and also solve outstanding problems concerning, e.g. dynamical phase transitions in non-equilibrium systems, establishing long-range order via dissipation, verifying the simulatability of open-system dynamics on a quantum Turing machine. We construct an efficient autonomous algorithm for designing an efficient quantum circuit to simulate many-body open-system dynamics described by a local Hamiltonian plus decoherence due to separate baths for each particle. The execution time and number of gates for the quantum simulator both scale polynomially with the system size. DSW funded by USARO. MCO funded by AITF and Brazilian agencies CNPq and FAPESP through Instituto Nacional de Ciencia e Tecnologia-Informacao Quantica (INCT-IQ). DWB funded by ARC Future Fellowship (FT100100761). BCS funded by AITF, CIFAR, NSERC and USARO.

  7. The potential, limitations, and challenges of divide and conquer quantum electronic structure calculations on energetic materials.

    SciTech Connect

    Tucker, Jon R.; Magyar, Rudolph J.

    2012-02-01

    High explosives are an important class of energetic materials used in many weapons applications. Even with modern computers, the simulation of the dynamic chemical reactions and energy release is exceedingly challenging. While the scale of the detonation process may be macroscopic, the dynamic bond breaking responsible for the explosive release of energy is fundamentally quantum mechanical. Thus, any method that does not adequately describe bonding is destined to lack predictive capability on some level. Performing quantum mechanics calculations on systems with more than dozens of atoms is a gargantuan task, and severe approximation schemes must be employed in practical calculations. We have developed and tested a divide and conquer (DnC) scheme to obtain total energies, forces, and harmonic frequencies within semi-empirical quantum mechanics. The method is intended as an approximate but faster solution to the full problem and is possible due to the sparsity of the density matrix in many applications. The resulting total energy calculation scales linearly as the number of subsystems, and the method provides a path-forward to quantum mechanical simulations of millions of atoms.

  8. Quantum Monte Carlo Calculations of Nanostructure Optical Properties

    NASA Astrophysics Data System (ADS)

    Williamson, Andrew

    2003-03-01

    Near linear scaling Quantum Monte Carlo (QMC) calculations[1] are used to calculate the optical gaps, electron affinities, and ionization potentials of silicon and germanium quantum dots ranging in size from 0 to 2 nm[2]. These QMC results are used to examine the accuracy of semi-empirical and density functional (DFT) calculations. We find optical gaps are underestimated by DFT by 1-2 eV depending on choice of functional. Corrections introduced by the time dependent formalisms are found to be minimal in these systems. Our results also show that quantum confinement in germanium is significantly greater than in silicon leading to a crossover of their optical gaps in dots between 2 and 3 nm in size, verifying recent experiment observations. [1] A. J. Williamson, R.Q. Hood and J.C. Grossman, Phys. Rev. Lett. 87, 246406-1 (2001). [2] A.J. Williamson J.C. Grossman, R.Q. Hood, A. Puzder and Giulia Galli, Phys. Rev. Lett, 89, 196803 (2002).

  9. Bias in Dynamic Monte Carlo Alpha Calculations

    SciTech Connect

    Sweezy, Jeremy Ed; Nolen, Steven Douglas; Adams, Terry R.; Trahan, Travis John

    2015-02-06

    A 1/N bias in the estimate of the neutron time-constant (commonly denoted as α) has been seen in dynamic neutronic calculations performed with MCATK. In this paper we show that the bias is most likely caused by taking the logarithm of a stochastic quantity. We also investigate the known bias due to the particle population control method used in MCATK. We conclude that this bias due to the particle population control method is negligible compared to other sources of bias.

  10. Stochastic solution to quantum dynamics

    NASA Technical Reports Server (NTRS)

    John, Sarah; Wilson, John W.

    1994-01-01

    The quantum Liouville equation in the Wigner representation is solved numerically by using Monte Carlo methods. For incremental time steps, the propagation is implemented as a classical evolution in phase space modified by a quantum correction. The correction, which is a momentum jump function, is simulated in the quasi-classical approximation via a stochastic process. The technique, which is developed and validated in two- and three- dimensional momentum space, extends an earlier one-dimensional work. Also, by developing a new algorithm, the application to bound state motion in an anharmonic quartic potential shows better agreement with exact solutions in two-dimensional phase space.

  11. Hierarchy of Stochastic Pure States for Open Quantum System Dynamics

    NASA Astrophysics Data System (ADS)

    Suess, D.; Eisfeld, A.; Strunz, W. T.

    2014-10-01

    We derive a hierarchy of stochastic evolution equations for pure states (quantum trajectories) for open quantum system dynamics with non-Markovian structured environments. This hierarchy of pure states (HOPS) is generally applicable and provides the exact reduced density operator as an ensemble average over normalized states. The corresponding nonlinear equations are presented. We demonstrate that HOPS provides an efficient theoretical tool and apply it to the spin-boson model, the calculation of absorption spectra of molecular aggregates, and energy transfer in a photosynthetic pigment-protein complex.

  12. Cavity-assisted dynamical quantum phase transition in superconducting quantum simulators

    NASA Astrophysics Data System (ADS)

    Tian, Lin

    Coupling a quantum many-body system to a cavity can create bifurcation points in the phase diagram, where the many-body system switches between different phases. Here I will discuss the dynamical quantum phase transitions at the bifurcation points of a one-dimensional transverse field Ising model coupled to a cavity. The Ising model can be emulated with various types of superconducting qubits connected in a chain. With a time-dependent Bogoliubov method, we show that an infinitesimal quench of the driving field can cause gradual evolution of the transverse field on the Ising spins to pass through the quantum critical point. Our calculation shows that the cavity-induced nonlinearity plays an important role in the dynamics of this system. Quasiparticles can be excited in the Ising chain during this process, which results in the deviation of the system from its adiabatic ground state. This work is supported by the National Science Foundation under Award Number 0956064.

  13. Quantum Monte Carlo Calculations in Solids with Downfolded Hamiltonians

    NASA Astrophysics Data System (ADS)

    Ma, Fengjie; Purwanto, Wirawan; Zhang, Shiwei; Krakauer, Henry

    2015-06-01

    We present a combination of a downfolding many-body approach with auxiliary-field quantum Monte Carlo (AFQMC) calculations for extended systems. Many-body calculations operate on a simpler Hamiltonian which retains material-specific properties. The Hamiltonian is systematically improvable and allows one to dial, in principle, between the simplest model and the original Hamiltonian. As a by-product, pseudopotential errors are essentially eliminated using frozen orbitals constructed adaptively from the solid environment. The computational cost of the many-body calculation is dramatically reduced without sacrificing accuracy. Excellent accuracy is achieved for a range of solids, including semiconductors, ionic insulators, and metals. We apply the method to calculate the equation of state of cubic BN under ultrahigh pressure, and determine the spin gap in NiO, a challenging prototypical material with strong electron correlation effects.

  14. Dynamic programming algorithms as quantum circuits: symmetric function realization

    NASA Astrophysics Data System (ADS)

    Maslov, Dmitri A.

    2004-08-01

    The work starts with a general idea of how to realize a dynamic programming algorithm as a quantum circuit. This realization is not tied to a specific design model, technology or a class of dynamic algorithms, it shows an approach for such synthesis. As an illustration of the efficiency of this approach, the class of all multiple-output symmetric functions is realized in a dynamic programming algorithm manner as a reversible circuit of Toffoli type elements (NOT, CNOT, and Toffoli gates). The garbage and quantum cost (found based on Barenco et al. paper) of the presented implementation are calculated and compared to the costs of previously described reversible synthesis methods. The summary of results of this comparison is as follows. The quantum cost of the proposed method is less than the quantum cost of any other reported systematic approach. The garbage is usually lower, except for comparison with the synthesis methods, whose primary goal is synthesis with theoretically minimal garbage. The presented algorithm application to the symmetric function synthesis results in circuits suitable for quantum technology realizations.

  15. Relaxation dynamics in correlated quantum dots

    SciTech Connect

    Andergassen, S.; Schuricht, D.; Pletyukhov, M.; Schoeller, H.

    2014-12-04

    We study quantum many-body effects on the real-time evolution of the current through quantum dots. By using a non-equilibrium renormalization group approach, we provide analytic results for the relaxation dynamics into the stationary state and identify the microscopic cutoff scales that determine the transport rates. We find rich non-equilibrium physics induced by the interplay of the different energy scales. While the short-time limit is governed by universal dynamics, the long-time behavior features characteristic oscillations as well as an interplay of exponential and power-law decay.

  16. Quantum dynamics of Lorentzian spacetime foam

    NASA Astrophysics Data System (ADS)

    Redmount, Ian H.; Suen, Wai-Mo

    1994-05-01

    A simple spacetime wormhole, which evolves classically from zero throat radius to a maximum value and recontracts, can be regarded as one possible mode of fluctuation in the microscopic ``spacetime foam'' first suggested by Wheeler. The dynamics of a particularly simple version of such a wormhole can be reduced to that of a single quantity, its throat radius; this wormhole thus provides a ``minisuperspace model'' for a mode of Lorentzian-signature foam. The classical equation of motion for the wormhole throat is obtained from the Einstein field equations and a suitable equation of state for the matter at the throat. Analysis of the quantum behavior of the hole then proceeds from an action corresponding to that equation of motion. The action obtained simply by calculating the scalar curvature of the hole spacetime yields a model with features like those of the relativistic free particle. In particular the Hamiltonian is nonlocal, and for the wormhole cannot even be given as a differential operator in closed form. Nonetheless the general solution of the Schrödinger equation for wormhole wave functions, i.e., the wave-function propagator, can be expressed as a path integral. Too complicated to perform exactly, this can yet be evaluated via a WKB approximation. The result indicates that the wormhole, classically stable, is quantum-mechanically unstable: A Feynman-Kac decomposition of the WKB propagator yields no spectrum of bound states. Although an initially localized wormhole wave function may oscillate for many classical expansion and recontraction periods, it must eventually leak to large radius values. The possibility of such a mode unstable against growth, combined with the observed absence of macroscopic wormholes, suggests that stability considerations may place constraints on the nature or even the existence of Planck-scale foamlike structure, at least of Lorentzian signature.

  17. Quantum dynamics of hydrogen atoms on graphene. II. Sticking

    NASA Astrophysics Data System (ADS)

    Bonfanti, Matteo; Jackson, Bret; Hughes, Keith H.; Burghardt, Irene; Martinazzo, Rocco

    2015-09-01

    Following our recent system-bath modeling of the interaction between a hydrogen atom and a graphene surface [Bonfanti et al., J. Chem. Phys. 143, 124703 (2015)], we present the results of converged quantum scattering calculations on the activated sticking dynamics. The focus of this study is the collinear scattering on a surface at zero temperature, which is treated with high-dimensional wavepacket propagations with the multi-configuration time-dependent Hartree method. At low collision energies, barrier-crossing dominates the sticking and any projectile that overcomes the barrier gets trapped in the chemisorption well. However, at high collision energies, energy transfer to the surface is a limiting factor, and fast H atoms hardly dissipate their excess energy and stick on the surface. As a consequence, the sticking coefficient is maximum (˜0.65) at an energy which is about one and half larger than the barrier height. Comparison of the results with classical and quasi-classical calculations shows that quantum fluctuations of the lattice play a primary role in the dynamics. A simple impulsive model describing the collision of a classical projectile with a quantum surface is developed which reproduces the quantum results remarkably well for all but the lowest energies, thereby capturing the essential physics of the activated sticking dynamics investigated.

  18. Quantum dynamics of hydrogen atoms on graphene. II. Sticking

    SciTech Connect

    Bonfanti, Matteo; Jackson, Bret; Hughes, Keith H.; Burghardt, Irene

    2015-09-28

    Following our recent system-bath modeling of the interaction between a hydrogen atom and a graphene surface [Bonfanti et al., J. Chem. Phys. 143, 124703 (2015)], we present the results of converged quantum scattering calculations on the activated sticking dynamics. The focus of this study is the collinear scattering on a surface at zero temperature, which is treated with high-dimensional wavepacket propagations with the multi-configuration time-dependent Hartree method. At low collision energies, barrier-crossing dominates the sticking and any projectile that overcomes the barrier gets trapped in the chemisorption well. However, at high collision energies, energy transfer to the surface is a limiting factor, and fast H atoms hardly dissipate their excess energy and stick on the surface. As a consequence, the sticking coefficient is maximum (∼0.65) at an energy which is about one and half larger than the barrier height. Comparison of the results with classical and quasi-classical calculations shows that quantum fluctuations of the lattice play a primary role in the dynamics. A simple impulsive model describing the collision of a classical projectile with a quantum surface is developed which reproduces the quantum results remarkably well for all but the lowest energies, thereby capturing the essential physics of the activated sticking dynamics investigated.

  19. Quantum dynamics of hydrogen atoms on graphene. II. Sticking.

    PubMed

    Bonfanti, Matteo; Jackson, Bret; Hughes, Keith H; Burghardt, Irene; Martinazzo, Rocco

    2015-09-28

    Following our recent system-bath modeling of the interaction between a hydrogen atom and a graphene surface [Bonfanti et al., J. Chem. Phys. 143, 124703 (2015)], we present the results of converged quantum scattering calculations on the activated sticking dynamics. The focus of this study is the collinear scattering on a surface at zero temperature, which is treated with high-dimensional wavepacket propagations with the multi-configuration time-dependent Hartree method. At low collision energies, barrier-crossing dominates the sticking and any projectile that overcomes the barrier gets trapped in the chemisorption well. However, at high collision energies, energy transfer to the surface is a limiting factor, and fast H atoms hardly dissipate their excess energy and stick on the surface. As a consequence, the sticking coefficient is maximum (∼0.65) at an energy which is about one and half larger than the barrier height. Comparison of the results with classical and quasi-classical calculations shows that quantum fluctuations of the lattice play a primary role in the dynamics. A simple impulsive model describing the collision of a classical projectile with a quantum surface is developed which reproduces the quantum results remarkably well for all but the lowest energies, thereby capturing the essential physics of the activated sticking dynamics investigated.

  20. Accelerating quantum instanton calculations of the kinetic isotope effects

    SciTech Connect

    Karandashev, Konstantin; Vaníček, Jiří

    2015-11-21

    Path integral implementation of the quantum instanton approximation currently belongs among the most accurate methods for computing quantum rate constants and kinetic isotope effects, but its use has been limited due to the rather high computational cost. Here, we demonstrate that the efficiency of quantum instanton calculations of the kinetic isotope effects can be increased by orders of magnitude by combining two approaches: The convergence to the quantum limit is accelerated by employing high-order path integral factorizations of the Boltzmann operator, while the statistical convergence is improved by implementing virial estimators for relevant quantities. After deriving several new virial estimators for the high-order factorization and evaluating the resulting increase in efficiency, using ⋅H{sub α} + H{sub β}H{sub γ} → H{sub α}H{sub β} + ⋅ H{sub γ} reaction as an example, we apply the proposed method to obtain several kinetic isotope effects on CH{sub 4} + ⋅ H ⇌ ⋅ CH{sub 3} + H{sub 2} forward and backward reactions.

  1. Molecular dynamics of large systems with quantum corrections for the nuclei

    SciTech Connect

    Gu, Bing; Garashchuk, Sophya

    2015-12-31

    This paper describes an approximate approach to quantum dynamics based on the quantum trajectory formulation of the Schrödinger equation. The quantum-mechanical effects are incorporated through the quantum potential of the mean-field type, acting on a trajectory ensemble in addition to the classical potential. Efficiency for large systems is achieved by using the quantum corrections for selected degrees of freedom and introduction of empirical friction into the ground-state energy calculations. The classical potential, if needed, can be computed on-the-fly using the Density Functional Tight Binding method of electronic structure merged with the quantum trajectory dynamics code. The approach is practical for a few hundred atoms. Applications include a study of adsorption of quantum hydrogen colliding with the graphene model, C{sub 37}H{sub 15} and a calculation of the ground state of solid {sup 4}He simulated by a cell 180-atoms.

  2. Communication: Constant uncertainty molecular dynamics: A simple and efficient algorithm to incorporate quantum nature into a real-time molecular dynamics simulation

    NASA Astrophysics Data System (ADS)

    Hasegawa, Taisuke

    2016-11-01

    We propose a novel molecular dynamics (MD) algorithm for approximately dealing with a nuclear quantum dynamics in a real-time MD simulation. We have found that real-time dynamics of the ensemble of classical particles acquires quantum nature by introducing a constant quantum mechanical uncertainty constraint on its classical dynamics. The constant uncertainty constraint is handled by the Lagrange multiplier method and implemented into a conventional MD algorithm. The resulting constant uncertainty molecular dynamics (CUMD) is applied to the calculation of quantum position autocorrelation functions on quartic and Morse potentials. The test calculations show that CUMD gives better performance than ring-polymer MD because of the inclusion of the quantum zero-point energy during real-time evolution as well as the quantum imaginary-time statistical effect stored in an initial condition. The CUMD approach will be a possible starting point for new real-time quantum dynamics simulation in condensed phase.

  3. Communication: Constant uncertainty molecular dynamics: A simple and efficient algorithm to incorporate quantum nature into a real-time molecular dynamics simulation.

    PubMed

    Hasegawa, Taisuke

    2016-11-07

    We propose a novel molecular dynamics (MD) algorithm for approximately dealing with a nuclear quantum dynamics in a real-time MD simulation. We have found that real-time dynamics of the ensemble of classical particles acquires quantum nature by introducing a constant quantum mechanical uncertainty constraint on its classical dynamics. The constant uncertainty constraint is handled by the Lagrange multiplier method and implemented into a conventional MD algorithm. The resulting constant uncertainty molecular dynamics (CUMD) is applied to the calculation of quantum position autocorrelation functions on quartic and Morse potentials. The test calculations show that CUMD gives better performance than ring-polymer MD because of the inclusion of the quantum zero-point energy during real-time evolution as well as the quantum imaginary-time statistical effect stored in an initial condition. The CUMD approach will be a possible starting point for new real-time quantum dynamics simulation in condensed phase.

  4. Nonequilibrium quantum dynamics in optomechanical systems

    NASA Astrophysics Data System (ADS)

    Patil, Yogesh Sharad; Cheung, Hil F. H.; Shaffer, Airlia; Wang, Ke; Vengalattore, Mukund

    2016-05-01

    The thermalization dynamics of isolated quantum systems has so far been explored in the context of cold atomic systems containing a large number of particles and modes. Quantum optomechanical systems offer prospects of studying such dynamics in a qualitatively different regime - with few individually addressable modes amenable to continuous quantum measurement and thermalization times that vastly exceed those observed in cold atomic systems. We have experimentally realized a dynamical continuous phase transition in a quantum compatible nondegenerate mechanical parametric oscillator. This system is formally equivalent to the optical parametric amplifiers whose dynamics have been a subject of intense theoretical study. We experimentally verify its phase diagram and observe nonequilibrium behavior that was only theorized, but never directly observed, in the context of optical parametric amplifiers. We discuss prospects of using nonequilibrium protocols such as quenches in optomechanical systems to amplify weak nonclassical correlations and to realize macroscopic nonclassical states. This work was supported by the DARPA QuASAR program through a Grant from the ARO and the ARO MURI on non-equilibrium manybody dynamics.

  5. Nuclear quantum dynamics in dense hydrogen

    PubMed Central

    Kang, Dongdong; Sun, Huayang; Dai, Jiayu; Chen, Wenbo; Zhao, Zengxiu; Hou, Yong; Zeng, Jiaolong; Yuan, Jianmin

    2014-01-01

    Nuclear dynamics in dense hydrogen, which is determined by the key physics of large-angle scattering or many-body collisions between particles, is crucial for the dynamics of planet's evolution and hydrodynamical processes in inertial confinement confusion. Here, using improved ab initio path-integral molecular dynamics simulations, we investigated the nuclear quantum dynamics regarding transport behaviors of dense hydrogen up to the temperatures of 1 eV. With the inclusion of nuclear quantum effects (NQEs), the ionic diffusions are largely higher than the classical treatment by the magnitude from 20% to 146% as the temperature is decreased from 1 eV to 0.3 eV at 10 g/cm3, meanwhile, electrical and thermal conductivities are significantly lowered. In particular, the ionic diffusion is found much larger than that without NQEs even when both the ionic distributions are the same at 1 eV. The significant quantum delocalization of ions introduces remarkably different scattering cross section between protons compared with classical particle treatments, which explains the large difference of transport properties induced by NQEs. The Stokes-Einstein relation, Wiedemann-Franz law, and isotope effects are re-examined, showing different behaviors in nuclear quantum dynamics. PMID:24968754

  6. Phase space representation of quantum dynamics

    SciTech Connect

    Polkovnikov, Anatoli

    2010-08-15

    We discuss a phase space representation of quantum dynamics of systems with many degrees of freedom. This representation is based on a perturbative expansion in quantum fluctuations around one of the classical limits. We explicitly analyze expansions around three such limits: (i) corpuscular or Newtonian limit in the coordinate-momentum representation, (ii) wave or Gross-Pitaevskii limit for interacting bosons in the coherent state representation, and (iii) Bloch limit for the spin systems. We discuss both the semiclassical (truncated Wigner) approximation and further quantum corrections appearing in the form of either stochastic quantum jumps along the classical trajectories or the nonlinear response to such jumps. We also discuss how quantum jumps naturally emerge in the analysis of non-equal time correlation functions. This representation of quantum dynamics is closely related to the phase space methods based on the Wigner-Weyl quantization and to the Keldysh technique. We show how such concepts as the Wigner function, Weyl symbol, Moyal product, Bopp operators, and others automatically emerge from the Feynmann's path integral representation of the evolution in the Heisenberg representation. We illustrate the applicability of this expansion with various examples mostly in the context of cold atom systems including sine-Gordon model, one- and two-dimensional Bose-Hubbard model, Dicke model and others.

  7. Dynamics of streaming instability with quantum correction

    NASA Astrophysics Data System (ADS)

    Goutam, H. P.; Karmakar, P. K.

    2017-05-01

    A modified quantum hydrodynamic model (m-QHD) is herein proposed on the basis of the Thomas-Fermi (TF) theory of many fermionic quantum systems to investigate the dynamics of electrostatic streaming instability modes in a complex (dusty) quantum plasma system. The newly formulated m-QHD, as an amelioration over the existing usual QHD, employs a dimensionality-dependent Bohmian quantum correction prefactor, γ = [(D-2)/3D], in the electron quantum dynamics, where D symbolizing the problem dimensionality under consideration. The normal mode analysis of the coupled structure equations reveals the excitation of two distinct streaming modes associated with the flowing ions (against electrons and dust) and the flowing dust particulates (against the electrons and ions). It is mainly shown that the γ-factor introduces a new source of stability and dispersive effects to the ion-streaming instability solely; but not to the dust counterparts. A non-trivial application of our investigation in electrostatic beam-plasma (flow-driven) coupled dynamics leading to the development of self-sustained intense electric current, and hence, of strong magnetic field in compact astrophysical objects (in dwarf-family stars) is summarily indicated.

  8. Compressing measurements in quantum dynamic parameter estimation

    NASA Astrophysics Data System (ADS)

    Magesan, Easwar; Cooper, Alexandre; Cappellaro, Paola

    2013-12-01

    We present methods that can provide an exponential savings in the resources required to perform dynamic parameter estimation using quantum systems. The key idea is to merge classical compressive sensing techniques with quantum control methods to significantly reduce the number of signal coefficients that are required for reconstruction of time-varying parameters with high fidelity. We show that incoherent measurement bases and, more generally, suitable random measurement matrices can be created by performing simple control sequences on the quantum system. Random measurement matrices satisfying the restricted isometry property can be used efficiently to reconstruct signals that are sparse in any basis. Because many physical processes are approximately sparse in some basis, these methods can benefit a variety of applications such as quantum sensing and magnetometry with nitrogen-vacancy centers.

  9. Spin Dynamics of Charged Colloidal Quantum Dots

    NASA Astrophysics Data System (ADS)

    Stern, N. P.

    2005-03-01

    Colloidal semiconductor quantum dots are promising structures for controlling spin phenomena because of their highly size- tunable physical properties, ease of manufacture, and nanosecond-scale spin lifetimes at room temperature. Recent experiments have succeeded in controlling the charging of the lowest electronic state of colloidal quantum dots ootnotetextC. Wang, B. L. Wehrenberg, C. Y. Woo, and P. Guyot-Sionnest, J. Phys. Chem B 108, 9027 (2004).. Here we use time-resolved Faraday rotation measurements in the Voigt geometry to investigate the spin dynamics of colloidal CdSe quantum dot films in both a charged and uncharged state at room temperature. The charging of the film is controlled by applying a voltage in an electrochemical cell and is confirmed by absorbance measurements. Significant changes in the spin precession are observed upon charging, reflecting the voltage- controlled electron occupation of the quantum dot states and filling of surface states.

  10. Understanding molecular dynamics quantum-state by quantum-state

    SciTech Connect

    Lawrance, W.D.; Moore, C.B.; Petek, H.

    1985-02-22

    It is now possible to resolve completely the initial and final quantum states in chemical processes. Spectra of reactive intermediates, of highly vibrationally excited molecules, and even of molecules in the process of falling apart have been recorded. This information has led to greater understanding of the molecular structure and dynamics of small gas-phase molecules. Many of the concepts and spectroscopic techniques that have been developed will be valuable throughout chemistry.

  11. Delay time calculation for dual-wavelength quantum cascade lasers

    SciTech Connect

    Hamadou, A.; Lamari, S.; Thobel, J.-L.

    2013-11-28

    In this paper, we calculate the turn-on delay (t{sub th}) and buildup (Δt) times of a midinfrared quantum cascade laser operating simultaneously on two laser lines having a common upper level. The approach is based on the four-level rate equations model describing the variation of the electron number in the states and the photon number present within the cavity. We obtain simple analytical formulae for the turn-on delay and buildup times that determine the delay times and numerically apply our results to both the single and bimode states of a quantum cascade laser, in addition the effects of current injection on t{sub th} and Δt are explored.

  12. Distributed quantum chemistry calculations via Web-GUI

    SciTech Connect

    Schnupf, U.; Friedman-Hill, E.; Durant, J.L.

    1996-12-31

    We will discuss the development of an expert-system that will allow the non-professional to run quantum chemistry software on distributed computers platforms from a Web-GUI. The basic idea is to create an expert-system which will handle the fundamental steps for any given computational problem, e.g. choice of software, choice of computer resources, control of the actual computational process and output display. As interface between user and expert-system we have chosen a Web-GUI in which the user can formulate his/her problem in a simple manner. At the heart of the expert-system are intelligent agents, which are responsible for the overall control of the computational task. This combined approach will enormously simplify the use of a heterogeneous computing environment for quantum chemical calculations.

  13. Precision decay rate calculations in quantum field theory

    NASA Astrophysics Data System (ADS)

    Andreassen, Anders; Farhi, David; Frost, William; Schwartz, Matthew D.

    2017-04-01

    Tunneling in quantum field theory is worth understanding properly, not least because it controls the long-term fate of our Universe. There are, however, a number of features of tunneling rate calculations which lack a desirable transparency, such as the necessity of analytic continuation, the appropriateness of using an effective instead of classical potential, and the sensitivity to short-distance physics. This paper attempts to review in pedagogical detail the physical origin of tunneling and its connection to the path integral. Both the traditional potential-deformation method and a recent, more direct, propagator-based method are discussed. Some new insights from using approximate semiclassical solutions are presented. In addition, we explore the sensitivity of the lifetime of our Universe to short-distance physics, such as quantum gravity, emphasizing a number of important subtleties.

  14. Dynamical correlations after a quantum quench.

    PubMed

    Essler, Fabian H L; Evangelisti, Stefano; Fagotti, Maurizio

    2012-12-14

    We consider dynamic (non-equal-time) correlation functions of local observables after a quantum quench. We show that, in the absence of long-range interactions in the final Hamiltonian, the dynamics is determined by the same ensemble that describes static (equal-time) correlations. For many integrable models, static correlation functions of local observables after a quantum quench relax to stationary values, which are described by a generalized Gibbs ensemble. The same generalized Gibbs ensemble then determines dynamic correlation functions, and the basic form of the fluctuation dissipation theorem holds, although the absorption and emission spectra are not simply related as in the thermal case. For quenches in the transverse field Ising chain, we derive explicit expressions for the time evolution of dynamic order parameter correlators after a quench.

  15. Spectroscopic and quantum chemical calculation study on 2-ethoxythiazole molecule

    NASA Astrophysics Data System (ADS)

    Avcı, Davut; Dede, Bülent; Bahçeli, Semiha; Varkal, Döndü

    2017-06-01

    In this study, the 2-ethoxythiazole molecule (C5H7NSO) which is a member of the five-membered heterocyles with one nitrogen atom group has been investigated by using the experimental UV-vis (in three different solvents) and FT-IR spectral results as well as some magnetic properties. Furthermore, the calculated molecular geometric parameters, vibrational wavenumbers, HOMO-LUMO energies, 1H and 13C NMR chemical shift values and natural bond orbitals (NBO) of the title molecule have been calculated at the B3LYP and HSEH1PBE levels of theory with the 6-311++G(d,p) basis set. The spectral results obtained from the quantum chemical calculations are in good agreement with the experimental results.

  16. Quantum diffusive dynamics of macromolecular transitions

    NASA Astrophysics Data System (ADS)

    Beccara, S. a.; Garberoglio, G.; Faccioli, P.

    2011-07-01

    We study the role of quantum fluctuations of atomic nuclei in the real-time dynamics of non-equilibrium macro-molecular transitions. To this goal we introduce an extension of the dominant reaction pathways formalism, in which the quantum corrections to the classical overdamped Langevin dynamics are rigorously taken into account to order ℏ2. We first illustrate our approach in simple cases, and compare with the results of the instanton theory. Then we apply our method to study the C7eq → C7ax transition of alanine dipeptide. We find that the inclusion of quantum fluctuations can significantly modify the reaction mechanism for peptides. For example, the energy difference which is overcome along the most probable pathway is reduced by as much as 50%.

  17. Intrinsic spin dynamics in semiconductor quantum dots

    NASA Astrophysics Data System (ADS)

    Valín-Rodríguez, Manuel

    2005-12-01

    We investigate the characteristic spin dynamics corresponding to semiconductor quantum dots within the multiband envelope function approximation (EFA). By numerically solving an 8 × 8 k·p Hamiltonian we treat systems based on different III-V semiconductor materials. It is shown that, even in the absence of an applied magnetic field, these systems show intrinsic spin dynamics governed by intraband and interband transitions leading to characteristic spin frequencies ranging from THz to optical frequencies.

  18. Efficient first-principles calculation of the quantum kinetic energy and momentum distribution of nuclei.

    PubMed

    Ceriotti, Michele; Manolopoulos, David E

    2012-09-07

    Light nuclei at room temperature and below exhibit a kinetic energy which significantly deviates from the predictions of classical statistical mechanics. This quantum kinetic energy is responsible for a wide variety of isotope effects of interest in fields ranging from chemistry to climatology. It also furnishes the second moment of the nuclear momentum distribution, which contains subtle information about the chemical environment and has recently become accessible to deep inelastic neutron scattering experiments. Here, we show how, by combining imaginary time path integral dynamics with a carefully designed generalized Langevin equation, it is possible to dramatically reduce the expense of computing the quantum kinetic energy. We also introduce a transient anisotropic Gaussian approximation to the nuclear momentum distribution which can be calculated with negligible additional effort. As an example, we evaluate the structural properties, the quantum kinetic energy, and the nuclear momentum distribution for a first-principles simulation of liquid water.

  19. Mixed Quantum-Classical Liouville Approach for Calculating Proton-Coupled Electron-Transfer Rate Constants.

    PubMed

    Shakib, Farnaz; Hanna, Gabriel

    2016-07-12

    In this work, we derive a general mixed quantum-classical formula for calculating thermal proton-coupled electron-transfer (PCET) rate constants, starting from the time integral of the quantum flux-flux correlation function. This formula allows for the direct simulation of PCET reaction dynamics via the mixed quantum-classical Liouville approach. Owing to the general nature of the derivation, this formula does not rely on any prior mechanistic assumptions and can be applied across a wide range of electronic and protonic coupling regimes. To test the validity of this formula, we applied it to a reduced model of a condensed-phase PCET reaction. Good agreement with the numerically exact rate constant is obtained, demonstrating the accuracy of our formalism. We believe that this approach constitutes a solid foundation for future investigations of the rates and mechanisms of a wide range of PCET reactions.

  20. Dynamical initial conditions in quantum cosmology.

    PubMed

    Bojowald, M

    2001-09-17

    Loop quantum cosmology is shown to provide both the dynamical law and initial conditions for the wave function of a universe by one discrete evolution equation. Accompanied by the condition that semiclassical behavior is obtained at large volume, a unique wave function is predicted.

  1. Quantum Monte Carlo calculations of A=8 nuclei

    NASA Astrophysics Data System (ADS)

    Wiringa, R. B.; Pieper, Steven C.; Carlson, J.; Pandharipande, V. R.

    2000-07-01

    We report quantum Monte Carlo calculations of ground and low-lying excited states for A=8 nuclei using a realistic Hamiltonian containing the Argonne v18 two-nucleon and Urbana IX three-nucleon potentials. The calculations begin with correlated eight-body wave functions that have a filled α-like core and four p-shell nucleons LS coupled to the appropriate (JπT) quantum numbers for the state of interest. After optimization, these variational wave functions are used as input to a Green's function Monte Carlo calculation made with a new constrained path algorithm. We find that the Hamiltonian produces a 8Be ground state that is within 2 MeV of the experimental resonance, but the other eight-body energies are progressively worse as the neutron-proton asymmetry increases. The 8Li ground state is stable against breakup into subclusters, but the 8He ground state is not. The excited state spectra are in fair agreement with experiment, with both the single-particle behavior of 8He and 8Li and the collective rotational behavior of 8Be being reproduced. We also examine energy differences in the T=1,2 isomultiplets and isospin-mixing matrix elements in the excited states of 8Be. Finally, we present densities, momentum distributions, and studies of the intrinsic shapes of these nuclei, with 8Be exhibiting a definite 2α cluster structure.

  2. Annular tautomerism: experimental observations and quantum mechanics calculations

    NASA Astrophysics Data System (ADS)

    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.

  3. Chaotic Behaviour in Quantum Dynamics.

    DTIC Science & Technology

    1986-12-01

    1.6 Relevance of Classical Analisys to the Problem of Microwave Ionization The other nonconservative system discussed in this report - the H-atom in...a microwave field - had never been sublected to quantum analisys , neither theoretical nor computational, up to the start of our program. Nevertheless...m, . A2) can tie expanded in a double Fourier series in the angle variables Xi, X2: (I,, A, ,klk2 Z= > (ni, n,, n) e i(0 K C) The coefficeuts z ,i can

  4. Importance of parametrizing constraints in quantum-mechanical variational calculations

    NASA Technical Reports Server (NTRS)

    Chung, Kwong T.; Bhatia, A. K.

    1992-01-01

    In variational calculations of quantum mechanics, constraints are sometimes imposed explicitly on the wave function. These constraints, which are deduced by physical arguments, are often not uniquely defined. In this work, the advantage of parametrizing constraints and letting the variational principle determine the best possible constraint for the problem is pointed out. Examples are carried out to show the surprising effectiveness of the variational method if constraints are parameterized. It is also shown that misleading results may be obtained if a constraint is not parameterized.

  5. Importance of parametrizing constraints in quantum-mechanical variational calculations

    NASA Technical Reports Server (NTRS)

    Chung, Kwong T.; Bhatia, A. K.

    1992-01-01

    In variational calculations of quantum mechanics, constraints are sometimes imposed explicitly on the wave function. These constraints, which are deduced by physical arguments, are often not uniquely defined. In this work, the advantage of parametrizing constraints and letting the variational principle determine the best possible constraint for the problem is pointed out. Examples are carried out to show the surprising effectiveness of the variational method if constraints are parameterized. It is also shown that misleading results may be obtained if a constraint is not parameterized.

  6. Pseudospectral Gaussian quantum dynamics: Efficient sampling of potential energy surfaces.

    PubMed

    Heaps, Charles W; Mazziotti, David A

    2016-04-28

    Trajectory-based Gaussian basis sets have been tremendously successful in describing high-dimensional quantum molecular dynamics. In this paper, we introduce a pseudospectral Gaussian-based method that achieves accurate quantum dynamics using efficient, real-space sampling of the time-dependent basis set. As in other Gaussian basis methods, we begin with a basis set expansion using time-dependent Gaussian basis functions guided by classical mechanics. Unlike other Gaussian methods but characteristic of the pseudospectral and collocation methods, the basis set is tested with N Dirac delta functions, where N is the number of basis functions, rather than using the basis function as test functions. As a result, the integration for matrix elements is reduced to function evaluation. Pseudospectral Gaussian dynamics only requires O(N) potential energy calculations, in contrast to O(N(2)) evaluations in a variational calculation. The classical trajectories allow small basis sets to sample high-dimensional potentials. Applications are made to diatomic oscillations in a Morse potential and a generalized version of the Henon-Heiles potential in two, four, and six dimensions. Comparisons are drawn to full analytical evaluation of potential energy integrals (variational) and the bra-ket averaged Taylor (BAT) expansion, an O(N) approximation used in Gaussian-based dynamics. In all cases, the pseudospectral Gaussian method is competitive with full variational calculations that require a global, analytical, and integrable potential energy surface. Additionally, the BAT breaks down when quantum mechanical coherence is particularly strong (i.e., barrier reflection in the Morse oscillator). The ability to obtain variational accuracy using only the potential energy at discrete points makes the pseudospectral Gaussian method a promising avenue for on-the-fly dynamics, where electronic structure calculations become computationally significant.

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

    PubMed

    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.

  8. Fully Quantum Description of the Zundel Ion: Combining Variational Quantum Monte Carlo with Path Integral Langevin Dynamics.

    PubMed

    Mouhat, Félix; Sorella, Sandro; Vuilleumier, Rodolphe; Saitta, Antonino Marco; Casula, Michele

    2017-06-13

    We introduce a novel approach for a fully quantum description of coupled electron-ion systems from first principles. It combines the variational quantum Monte Carlo solution of the electronic part with the path integral formalism for the quantum nuclear dynamics. On the one hand, the path integral molecular dynamics includes nuclear quantum effects by adding a set of fictitious classical particles (beads) aimed at reproducing nuclear quantum fluctuations via a harmonic kinetic term. On the other hand, variational quantum Monte Carlo can provide Born-Oppenheimer potential energy surfaces with a precision comparable to the most-advanced post-Hartree-Fock approaches, and with a favorable scaling with the system size. In order to cope with the intrinsic noise due to the stochastic nature of quantum Monte Carlo methods, we generalize the path integral molecular dynamics using a Langevin thermostat correlated according to the covariance matrix of quantum Monte Carlo nuclear forces. The variational parameters of the quantum Monte Carlo wave function are evolved during the nuclear dynamics, such that the Born-Oppenheimer potential energy surface is unbiased. Statistical errors on the wave function parameters are reduced by resorting to bead grouping average, which we show to be accurate and well-controlled. Our general algorithm relies on a Trotter breakup between the dynamics driven by ionic forces and the one set by the harmonic interbead couplings. The latter is exactly integrated, even in the presence of the Langevin thermostat, thanks to the mapping onto an Ornstein-Uhlenbeck process. This framework turns out to be also very efficient in the case of noiseless (deterministic) ionic forces. The new implementation is validated on the Zundel ion (H5O2(+)) by direct comparison with standard path integral Langevin dynamics calculations made with a coupled cluster potential energy surface. Nuclear quantum effects are confirmed to be dominant over thermal effects well beyond

  9. Loop quantum cosmology: from pre-inflationary dynamics to observations

    NASA Astrophysics Data System (ADS)

    Ashtekar, Abhay; Barrau, Aurélien

    2015-12-01

    The Planck collaboration has provided us rich information about the early Universe, and a host of new observational missions will soon shed further light on the ‘anomalies’ that appear to exist on the largest angular scales. From a quantum gravity perspective, it is natural to inquire if one can trace back the origin of such puzzling features to Planck scale physics. Loop quantum cosmology provides a promising avenue to explore this issue because of its natural resolution of the big bang singularity. Thanks to advances over the last decade, the theory has matured sufficiently to allow concrete calculations of the phenomenological consequences of its pre-inflationary dynamics. In this article we summarize the current status of the ensuing two-way dialog between quantum gravity and observations.

  10. Calculation of exchange interaction for modified Gaussian coupled quantum dots

    NASA Astrophysics Data System (ADS)

    Khordad, R.

    2017-08-01

    A system of two laterally coupled quantum dots with modified Gaussian potential has been considered. Each quantum dot has an electron under electric and magnetic field. The quantum dots have been considered as hydrogen-like atoms. The physical picture has translated into the Heisenberg spin Hamiltonian. The Schrödinger equation using finite element method has been numerically solved. The exchange energy factor has been calculated as a functions of electric field, magnetic field, and the separation distance between the centers of the dots ( d). According to the results, it is found that there is the transition from anti-ferromagnetic to ferromagnetic for constant electric field. Also, the transition occurs from ferromagnetic to anti-ferromagnetic for constant magnetic field (B>1 T). With decreasing the distance between the centers of the dots and increasing magnetic field, the transition occurs from anti-ferromagnetic to ferromagnetic. It is found that a switching of exchange energy factor is presented without canceling the interactions of the electric and magnetic fields on the system.

  11. Calculation of exchange interaction for modified Gaussian coupled quantum dots

    NASA Astrophysics Data System (ADS)

    Khordad, R.

    2017-03-01

    A system of two laterally coupled quantum dots with modified Gaussian potential has been considered. Each quantum dot has an electron under electric and magnetic field. The quantum dots have been considered as hydrogen-like atoms. The physical picture has translated into the Heisenberg spin Hamiltonian. The Schrödinger equation using finite element method has been numerically solved. The exchange energy factor has been calculated as a functions of electric field, magnetic field, and the separation distance between the centers of the dots (d). According to the results, it is found that there is the transition from anti-ferromagnetic to ferromagnetic for constant electric field. Also, the transition occurs from ferromagnetic to anti-ferromagnetic for constant magnetic field (B>1 T). With decreasing the distance between the centers of the dots and increasing magnetic field, the transition occurs from anti-ferromagnetic to ferromagnetic. It is found that a switching of exchange energy factor is presented without canceling the interactions of the electric and magnetic fields on the system.

  12. Thermodynamics and quantum corrections from molecular dynamics for liquid water

    NASA Astrophysics Data System (ADS)

    Berens, Peter H.; Mackay, Donald H. J.; White, Gary M.; Wilson, Kent R.

    1983-09-01

    In principle, given the potential energy function, the values of thermodynamic variables can be computed from statistical mechanics for a system of molecules. In practice for the liquid state, however, two barriers must be overcome. This paper treats the first problem, how to quantum correct the classical mechanical thermodynamic values available from molecular dynamics, Monte Carlo, perturbation, or integral methods in order to compare with experimental quantum reality. A subsequent paper will focus on the second difficulty, the effective computation of free energy and entropy. A simple technique, derived from spectral analysis of the atomic velocity time histories, is presented here for the frequency domain quantum correction of classical thermodynamic values. This technique is based on the approximation that potential anharmonicities mainly affect the lower frequencies in the velocity spectrum where the system behaves essentially classically, while the higher spectral frequencies, where the deviation from classical mechanics is most pronounced, involve sufficiently harmonic atomic motions that harmonic quantum corrections apply. Thus, a harmonic quantum correction can be applied at all frequencies: at low frequencies where it is inaccurate it will be small, while at high frequencies where it is large it will also be relatively accurate. The approach is demonstrated by computation of the energy and constant volume heat capacity for water from classical molecular dynamics followed by quantum correction. The potential used to describe the interactions of the system of water molecules includes internal vibrational degrees of freedom and thus strong quantum effects. Comparison of the quantum corrected theoretical values with experimental measurements shows good agreement. The quantum corrections to classical thermodynamics (which are also derived for free energy and entropy) are shown to be important not only for internal vibrational motion, but also for

  13. Stochastic unraveling of positive quantum dynamics

    NASA Astrophysics Data System (ADS)

    Caiaffa, Matteo; Smirne, Andrea; Bassi, Angelo

    2017-06-01

    Stochastic unravelings represent a useful tool to describe the dynamics of open quantum systems, and standard methods, such as quantum state diffusion (QSD), call for the complete positivity of the open-system dynamics. Here, we present a generalization of QSD, which also applies to positive, but not completely positive evolutions. The rate and the action of the diffusive processes involved in the unraveling are obtained by applying a proper transformation to the operators which define the master equation. The unraveling is first defined for semigroup dynamics and then extended to a definite class of time-dependent generators. We test our approach on a prototypical model for the description of exciton transfer, keeping track of relevant phenomena, which are instead disregarded within the standard, completely positive framework.

  14. Quantum dynamics in the thermodynamic limit

    SciTech Connect

    Wezel, Jasper van

    2008-08-01

    The description of spontaneous symmetry breaking that underlies the connection between classically ordered objects in the thermodynamic limit and their individual quantum-mechanical building blocks is one of the cornerstones of modern condensed-matter theory and has found applications in many different areas of physics. The theory of spontaneous symmetry breaking, however, is inherently an equilibrium theory, which does not address the dynamics of quantum systems in the thermodynamic limit. Here, we will use the example of a particular antiferromagnetic model system to show that the presence of a so-called thin spectrum of collective excitations with vanishing energy - one of the well-known characteristic properties shared by all symmetry-breaking objects - can allow these objects to also spontaneously break time-translation symmetry in the thermodynamic limit. As a result, that limit is found to be able, not only to reduce quantum-mechanical equilibrium averages to their classical counterparts, but also to turn individual-state quantum dynamics into classical physics. In the process, we find that the dynamical description of spontaneous symmetry breaking can also be used to shed some light on the possible origins of Born's rule. We conclude by describing an experiment on a condensate of exciton polaritons which could potentially be used to experimentally test the proposed mechanism.

  15. Role of controllability in optimizing quantum dynamics

    SciTech Connect

    Wu Rebing; Hsieh, Michael A.; Rabitz, Herschel

    2011-06-15

    This paper reveals an important role that controllability plays in the complexity of optimizing quantum control dynamics. We show that the loss of controllability generally leads to multiple locally suboptimal controls when gate fidelity in a quantum control system is maximized, which does not happen if the system is controllable. Such local suboptimal controls may attract an optimization algorithm into a local trap when a global optimal solution is sought, even if the target gate can be perfectly realized. This conclusion results from an analysis of the critical topology of the corresponding quantum control landscape, which refers to the gate fidelity objective as a functional of the control fields. For uncontrollable systems, due to SU(2) and SU(3) dynamical symmetries, the control landscape corresponding to an implementable target gate is proven to possess multiple locally optimal critical points, and its ruggedness can be further increased if the target gate is not realizable. These results imply that the optimization of quantum dynamics can be seriously impeded when operating with local search algorithms under these conditions, and thus full controllability is demanded.

  16. Instability of quantum equilibrium in Bohm's dynamics

    PubMed Central

    Colin, Samuel; Valentini, Antony

    2014-01-01

    We consider Bohm's second-order dynamics for arbitrary initial conditions in phase space. In principle, Bohm's dynamics allows for ‘extended’ non-equilibrium, with initial momenta not equal to the gradient of phase of the wave function (as well as initial positions whose distribution departs from the Born rule). We show that extended non-equilibrium does not relax in general and is in fact unstable. This is in sharp contrast with de Broglie's first-order dynamics, for which non-standard momenta are not allowed and which shows an efficient relaxation to the Born rule for positions. On this basis, we argue that, while de Broglie's dynamics is a tenable physical theory, Bohm's dynamics is not. In a world governed by Bohm's dynamics, there would be no reason to expect to see an effective quantum theory today (even approximately), in contradiction with observation. PMID:25383020

  17. A Calculation of Cosmological Scale from Quantum Coherence

    SciTech Connect

    Lindesay, J

    2004-07-23

    We use general arguments to examine the energy scales for which a quantum coherent description of gravitating quantum energy units is necessary. The cosmological dark energy density is expected to decouple from the Friedman-Lemaitre energy density when the Friedman-Robertson-Walker scale expansion becomes sub-luminal at R = c, at which time the usual microscopic interactions of relativistic quantum mechanics (QED, QCD, etc) open new degrees of freedom. We assume that these microscopic interactions cannot signal with superluminal exchanges, only superluminal quantum correlations. The expected gravitational vacuum energy density at that scale would be expected to freeze out due to the loss of gravitational coherence. We define the vacuum energy which generates this cosmological constant to be that of a zero temperature Bose condensate at this gravitational de-coherence scale. We presume a universality throughout the universe in the available degrees of freedom determined by fundamental constants during its evolution. Examining the reverse evolution of the universe from the present, long before reaching Planck scale dynamics one expects major modifications from the de-coherent thermal equations of state, suggesting that the pre-coherent phase has global coherence properties. Since the arguments presented involve primarily counting of degrees of freedom, we expect the statistical equilibrium states of causally disconnected regions of space to be independently identical. Thus, there is no horizon problem associated with the lack of causal influences between spatially separated regions in this approach. The scale of the amplitude of fluctuations produced during de-coherence of cosmological vacuum energy are found to evolve to values consistent with those observed in cosmic microwave background radiation and galactic clustering.

  18. Quantum dynamics of light-driven chiral molecular motors.

    PubMed

    Yamaki, Masahiro; Nakayama, Shin-ichiro; Hoki, Kunihito; Kono, Hirohiko; Fujimura, Yuichi

    2009-03-21

    The results of theoretical studies on quantum dynamics of light-driven molecular motors with internal rotation are presented. Characteristic features of chiral motors driven by a non-helical, linearly polarized electric field of light are explained on the basis of symmetry argument. The rotational potential of the chiral motor is characterized by a ratchet form. The asymmetric potential determines the directional motion: the rotational direction is toward the gentle slope of the asymmetric potential. This direction is called the intuitive direction. To confirm the unidirectional rotational motion, results of quantum dynamical calculations of randomly-oriented molecular motors are presented. A theoretical design of the smallest light-driven molecular machine is presented. The smallest chiral molecular machine has an optically driven engine and a running propeller on its body. The mechanisms of transmission of driving forces from the engine to the propeller are elucidated by using a quantum dynamical treatment. The results provide a principle for control of optically-driven molecular bevel gears. Temperature effects are discussed using the density operator formalism. An effective method for ultrafast control of rotational motions in any desired direction is presented with the help of a quantum control theory. In this method, visible or UV light pulses are applied to drive the motor via an electronic excited state. A method for driving a large molecular motor consisting of an aromatic hydrocarbon is presented. The molecular motor is operated by interactions between the induced dipole of the molecular motor and the electric field of light pulses.

  19. Quantum dynamics in strong fluctuating fields

    NASA Astrophysics Data System (ADS)

    Goychuk, Igor; Hänggi, Peter

    A large number of multifaceted quantum transport processes in molecular systems and physical nanosystems, such as e.g. nonadiabatic electron transfer in proteins, can be treated in terms of quantum relaxation processes which couple to one or several fluctuating environments. A thermal equilibrium environment can conveniently be modelled by a thermal bath of harmonic oscillators. An archetype situation provides a two-state dissipative quantum dynamics, commonly known under the label of a spin-boson dynamics. An interesting and nontrivial physical situation emerges, however, when the quantum dynamics evolves far away from thermal equilibrium. This occurs, for example, when a charge transferring medium possesses nonequilibrium degrees of freedom, or when a strong time-dependent control field is applied externally. Accordingly, certain parameters of underlying quantum subsystem acquire stochastic character. This may occur, for example, for the tunnelling coupling between the donor and acceptor states of the transferring electron, or for the corresponding energy difference between electronic states which assume via the coupling to the fluctuating environment an explicit stochastic or deterministic time-dependence. Here, we review the general theoretical framework which is based on the method of projector operators, yielding the quantum master equations for systems that are exposed to strong external fields. This allows one to investigate on a common basis, the influence of nonequilibrium fluctuations and periodic electrical fields on those already mentioned dynamics and related quantum transport processes. Most importantly, such strong fluctuating fields induce a whole variety of nonlinear and nonequilibrium phenomena. A characteristic feature of such dynamics is the absence of thermal (quantum) detailed balance.ContentsPAGE1. Introduction5262. Quantum dynamics in stochastic fields531 2.1. Stochastic Liouville equation531 2.2. Non-Markovian vs. Markovian discrete

  20. Dynamic holography in quantum well cavities

    NASA Astrophysics Data System (ADS)

    Sun, H.; Nolte, D. D.; Hyland, Jim; Harmon, Eric

    2013-03-01

    High efficiency dynamic holography at 1.55 microns is achieved on a broad-area InP based multiple quantum well devices. The quantum well cavity is sandwiched between a DBR and amorphous mirror, and consists of a number of wells. High energy pulsed writing beams at 1.06 microns generate free carrier gratings which are probed by a 1.55 micron tunable laser in a four wave mixing configuration. Diffraction efficiency into a single order of 30% has been achieved by contribution of a phase grating, mode pulling and asymmetric Fabry-Perot reflection.

  1. Communication: quantum dynamics in classical spin baths.

    PubMed

    Sergi, Alessandro

    2013-07-21

    A formalism for studying the dynamics of quantum systems embedded in classical spin baths is introduced. The theory is based on generalized antisymmetric brackets and predicts the presence of open-path off-diagonal geometric phases in the evolution of the density matrix. The weak coupling limit of the equation can be integrated by standard algorithms and provides a non-Markovian approach to the computer simulation of quantum systems in classical spin environments. It is expected that the theory and numerical schemes presented here have a wide applicability.

  2. Communication: Quantum dynamics in classical spin baths

    NASA Astrophysics Data System (ADS)

    Sergi, Alessandro

    2013-07-01

    A formalism for studying the dynamics of quantum systems embedded in classical spin baths is introduced. The theory is based on generalized antisymmetric brackets and predicts the presence of open-path off-diagonal geometric phases in the evolution of the density matrix. The weak coupling limit of the equation can be integrated by standard algorithms and provides a non-Markovian approach to the computer simulation of quantum systems in classical spin environments. It is expected that the theory and numerical schemes presented here have a wide applicability.

  3. Method for discovering relationships in data by dynamic quantum clustering

    DOEpatents

    Weinstein, Marvin; Horn, David

    2017-05-09

    Data clustering is provided according to a dynamical framework based on quantum mechanical time evolution of states corresponding to data points. To expedite computations, we can approximate the time-dependent Hamiltonian formalism by a truncated calculation within a set of Gaussian wave-functions (coherent states) centered around the original points. This allows for analytic evaluation of the time evolution of all such states, opening up the possibility of exploration of relationships among data-points through observation of varying dynamical-distances among points and convergence of points into clusters. This formalism may be further supplemented by preprocessing, such as dimensional reduction through singular value decomposition and/or feature filtering.

  4. Method for discovering relationships in data by dynamic quantum clustering

    DOEpatents

    Weinstein, Marvin; Horn, David

    2014-10-28

    Data clustering is provided according to a dynamical framework based on quantum mechanical time evolution of states corresponding to data points. To expedite computations, we can approximate the time-dependent Hamiltonian formalism by a truncated calculation within a set of Gaussian wave-functions (coherent states) centered around the original points. This allows for analytic evaluation of the time evolution of all such states, opening up the possibility of exploration of relationships among data-points through observation of varying dynamical-distances among points and convergence of points into clusters. This formalism may be further supplemented by preprocessing, such as dimensional reduction through singular value decomposition and/or feature filtering.

  5. Quantum Monte Carlo Calculations of Nucleon-Nucleus Scattering

    NASA Astrophysics Data System (ADS)

    Wiringa, R. B.; Nollett, Kenneth M.; Pieper, Steven C.; Brida, I.

    2009-10-01

    We report recent quantum Monte Carlo (variational and Green's function) calculations of elastic nucleon-nucleus scattering. We are adding the cases of proton-^4He, neutron-^3H and proton-^3He scattering to a previous GFMC study of neutron-^4He scattering [1]. To do this requires generalizing our methods to include long-range Coulomb forces and to treat coupled channels. The two four-body cases can be compared to other accurate four-body calculational methods such as the AGS equations and hyperspherical harmonic expansions. We will present results for the Argonne v18 interaction alone and with Urbana and Illinois three-nucleon potentials. [4pt] [1] K.M. Nollett, S. C. Pieper, R.B. Wiringa, J. Carlson, and G.M. Hale, Phys. Rev. Lett. 99, 022502 (2007)

  6. Accelerating atomistic calculations of quantum energy eigenstates on graphic cards

    NASA Astrophysics Data System (ADS)

    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).

  7. Automated quantum conductance calculations using maximally-localised Wannier functions

    NASA Astrophysics Data System (ADS)

    Shelley, Matthew; Poilvert, Nicolas; Mostofi, Arash A.; Marzari, Nicola

    2011-10-01

    A robust, user-friendly, and automated method to determine quantum conductance in quasi-one-dimensional systems is presented. The scheme relies upon an initial density-functional theory calculation in a specific geometry after which the ground-state eigenfunctions are transformed to a maximally-localised Wannier function (MLWF) basis. In this basis, our novel algorithms manipulate and partition the Hamiltonian for the calculation of coherent electronic transport properties within the Landauer-Buttiker formalism. Furthermore, we describe how short-ranged Hamiltonians in the MLWF basis can be combined to build model Hamiltonians of large (>10,000 atom) disordered systems without loss of accuracy. These automated algorithms have been implemented in the Wannier90 code (Mostofi et al., 2008) [1], which is interfaced to a number of electronic structure codes such as Quantum-ESPRESSO, AbInit, Wien2k, SIESTA and FLEUR. We apply our methods to an Al atomic chain with a Na defect, an axially heterostructured Si/Ge nanowire and to a spin-polarised defect on a zigzag graphene nanoribbon.

  8. Classical and quantum dynamics of the sphere

    NASA Astrophysics Data System (ADS)

    Lasukov, Vladimir; Moldovanova, Evgeniia; Abdrashitova, Maria; Malik, Hitendra; Gorbacheva, Ekaterina

    2016-07-01

    In Minkowski space, there has been developed the mathematic quantum model of the real particle located on the sphere evolving owing to the negative pressure inside the sphere. The developed model is analogous to the geometrodynamic model of the Lemaitre-Friedmann primordial atom in superspace-time, whose spatial coordinate is the scale factor functioning as a radial coordinate. There is a formulation of quantum geometrodynamics in which the spatial coordinate is an offset of the scale factor and wave function at the same time. With the help of the Dirac procedure for extracting the root from the Hamiltonian operator we have constructed a Dirac quantum dynamics of the sphere with fractional spin.

  9. Dynamical Response near Quantum Critical Points

    NASA Astrophysics Data System (ADS)

    Lucas, Andrew; Gazit, Snir; Podolsky, Daniel; Witczak-Krempa, William

    2017-02-01

    We study high-frequency response functions, notably the optical conductivity, in the vicinity of quantum critical points (QCPs) by allowing for both detuning from the critical coupling and finite temperature. We consider general dimensions and dynamical exponents. This leads to a unified understanding of sum rules. In systems with emergent Lorentz invariance, powerful methods from quantum field theory allow us to fix the high-frequency response in terms of universal coefficients. We test our predictions analytically in the large-N O (N ) model and using the gauge-gravity duality and numerically via quantum Monte Carlo simulations on a lattice model hosting the interacting superfluid-insulator QCP. In superfluid phases, interacting Goldstone bosons qualitatively change the high-frequency optical conductivity and the corresponding sum rule.

  10. Quantum dynamics of a semi-infinite homogeneous harmonic chain

    NASA Astrophysics Data System (ADS)

    Prato, Domingo; Lamberti, Pedro W.

    1993-07-01

    The quantum dynamics of a semi-infinite homogeneous harmonic chain is studied. Assuming the system to be in its ground state, a harmonic motion, A sin(ω t), is imposed on the mass at the beginning of the chain. The quantum state of the system for t>0 is calculated by means of the evolution operator. Two different regimes occur: one for angular frequencies ω outside the allowed band ω>ω 0 and the other one for ω inside the band. After a transient the time derivative of the total energy of the chain vanishes for the first regime and tends to a constant for the second one. The mean values of the displacements from their equilibrium position are also calculated for masses along the chain. These averaged displacements and the time derivative of the total energy are shown to give exactly the same expression as in the classical case.

  11. Direct grid-based quantum dynamics on propagated diabatic potential energy surfaces

    NASA Astrophysics Data System (ADS)

    Richings, Gareth W.; Habershon, Scott

    2017-09-01

    We present a method for performing non-adiabatic, grid-based nuclear quantum dynamics calculations using diabatic potential energy surfaces (PESs) generated ;on-the-fly;. Gaussian process regression is used to interpolate PESs by using electronic structure energies, calculated at points in configuration space determined by the nuclear dynamics, and diabatising the results using the propagation diabatisation method reported recently (Richings and Worth, 2015). Our new method is successfully demonstrated using a grid-based approach to model the non-adiabatic dynamics of the butatriene cation. Overall, our scheme offers a route towards accurate quantum dynamics on diabatic PESs learnt on-the-fly.

  12. Dynamics of quantum wave packets

    SciTech Connect

    Gosnell, T.R.; Taylor, A.J.; Rodriguez, G.; Clement, T.S.

    1998-11-01

    This is the final report of a three-year, Laboratory Directed Research and Development (LDRD) project at the Los Alamos National Laboratory (LANL). The objective of this project was to develop ultrafast laser techniques for the creation and measurement of quantum vibrational wave packets in gas phase diatomic molecules. Moreover, the authors sought to manipulate the constitution of these wave packets in terms of harmonic-oscillator basis wavefunctions by manipulating the time-dependent amplitude and phase of the incident ultrashort laser pulse. They specifically investigated gaseous diatomic potassium (K{sub 2}), and discovered variations in the shape of the wave packets as a result of changing the linear chirp in the ultrashort preparation pulse. In particular, they found evidence for wave-packet compression for a specific degree of chirp. Important ancillary results include development of new techniques for denoising and deconvolution of femtosecond time traces and techniques for diagnosing the phase and amplitude of the electric field of femtosecond laser pulses.

  13. Quantum Monte Carlo Calculations Applied to Magnetic Molecules

    SciTech Connect

    Engelhardt, Larry

    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

  14. Quantum dynamics in ultracold atomic physics

    NASA Astrophysics Data System (ADS)

    He, Qiong-Yi; Reid, Margaret D.; Opanchuk, Bogdan; Polkinghorne, Rodney; Rosales-Zárate, Laura E. C.; Drummond, Peter D.

    2012-02-01

    We review recent developments in the theory of quantum dynamics in ultracold atomic physics, including exact techniques and methods based on phase-space mappings that are applicable when the complexity becomes exponentially large. Phase-space representations include the truncated Wigner, positive- P and general Gaussian operator representations which can treat both bosons and fermions. These phase-space methods include both traditional approaches using a phase-space of classical dimension, and more recent methods that use a non-classical phase-space of increased dimensionality. Examples used include quantum Einstein-Podolsky-Rosen (EPR) entanglement of a four-mode BEC, time-reversal tests of dephasing in single-mode traps, BEC quantum collisions with up to 106 modes and 105 interacting particles, quantum interferometry in a multi-mode trap with nonlinear absorption, and the theory of quantum entropy in phase-space. We also treat the approach of variational optimization of the sampling error, giving an elementary example of a nonlinear oscillator.

  15. First-principles anharmonic quantum calculations for peptide spectroscopy: VSCF calculations and comparison with experiments.

    PubMed

    Roy, Tapta Kanchan; Sharma, Rahul; Gerber, R Benny

    2016-01-21

    First-principles quantum calculations for anharmonic vibrational spectroscopy of three protected dipeptides are carried out and compared with experimental data. Using hybrid HF/MP2 potentials, the Vibrational Self-Consistent Field with Second-Order Perturbation Correction (VSCF-PT2) algorithm is used to compute the spectra without any ad hoc scaling or fitting. All of the vibrational modes (135 for the largest system) are treated quantum mechanically and anharmonically using full pair-wise coupling potentials to represent the interaction between different modes. In the hybrid potential scheme the MP2 method is used for the harmonic part of the potential and a modified HF method is used for the anharmonic part. The overall agreement between computed spectra and experiment is very good and reveals different signatures for different conformers. This study shows that first-principles spectroscopic calculations of good accuracy are possible for dipeptides hence it opens possibilities for determination of dipeptide conformer structures by comparison of spectroscopic calculations with experiment.

  16. Separability and dynamical symmetry of Quantum Dots

    SciTech Connect

    Zhang, P.-M.; Zou, L.-P.; Horvathy, P.A.; Gibbons, G.W.

    2014-02-15

    The separability and Runge–Lenz-type dynamical symmetry of the internal dynamics of certain two-electron Quantum Dots, found by Simonović et al. (2003), are traced back to that of the perturbed Kepler problem. A large class of axially symmetric perturbing potentials which allow for separation in parabolic coordinates can easily be found. Apart from the 2:1 anisotropic harmonic trapping potential considered in Simonović and Nazmitdinov (2013), they include a constant electric field parallel to the magnetic field (Stark effect), the ring-shaped Hartmann potential, etc. The harmonic case is studied in detail. -- Highlights: • The separability of Quantum Dots is derived from that of the perturbed Kepler problem. • Harmonic perturbation with 2:1 anisotropy is separable in parabolic coordinates. • The system has a conserved Runge–Lenz type quantity.

  17. Polaronic quantum diffusion in dynamic localization regime

    NASA Astrophysics Data System (ADS)

    Yao, Yao

    2017-04-01

    We investigate the quantum dynamics in a disordered electronic lattice by the time-dependent density matrix renormalization group algorithm. The on-site energy in the lattice follows the Fibonacci sequence and the electron off-diagonally couples to a sub-Ohmic phonon bath. It is found that the slope of the inverse participation ratio versus the coupling strength undergoes a sudden change that indicates a transition from static to dynamic localization, and that the generated polarons coherently diffuse via hopping-like processes, evidenced by the saturated entanglement entropy, providing a novel scenario for a transportation mechanism in strongly disordered systems. Moreover, the mean-square displacement is revealed to be insensitive to the coupling strength, implying the quantum diffusion behavior survives the energy disorder that prevails in real organic materials.

  18. Quantum phase transitions with dynamical flavors

    NASA Astrophysics Data System (ADS)

    Bea, Yago; Jokela, Niko; Ramallo, Alfonso V.

    2016-07-01

    We study the properties of a D6-brane probe in the Aharony-Bergman-Jafferis-Maldacena (ABJM) background with smeared massless dynamical quarks in the Veneziano limit. Working at zero temperature and nonvanishing charge density, we show that the system undergoes a quantum phase transition in which the topology of the brane embedding changes from a black hole to a Minkowski embedding. In the unflavored background the phase transition is of second order and takes place when the charge density vanishes. We determine the corresponding critical exponents and show that the scaling behavior near the quantum critical point has multiplicative logarithmic corrections. In the background with dynamical quarks the phase transition is of first order and occurs at nonzero charge density. In this case we compute the discontinuity of several physical quantities as functions of the number Nf of unquenched quarks of the background.

  19. Dynamic Dimensionality Identification for Quantum Control

    NASA Astrophysics Data System (ADS)

    Roslund, Jonathan; Rabitz, Herschel

    2014-04-01

    The control of quantum systems with shaped laser pulses presents a paradox since the relative ease with which solutions are discovered appears incompatible with the enormous variety of pulse shapes accessible with a standard pulse shaper. Quantum landscape theory indicates that the relevant search dimensionality is not dictated by the number of pulse shaper elements, but rather is related to the number of states participating in the controlled dynamics. The actual dimensionality is encoded within the sensitivity of the observed yield to all of the pulse shaper elements. To investigate this proposition, the Hessian matrix is measured for controlled transitions amongst states of atomic rubidium, and its eigendecomposition reveals a dimensionality consistent with that predicted by landscape theory. Additionally, this methodology furnishes a low-dimensional picture that captures the essence of the light-matter interaction and the ensuing system dynamics.

  20. Quantum dynamics at finite temperature: Time-dependent quantum Monte Carlo study

    SciTech Connect

    Christov, Ivan P.

    2016-08-15

    In this work we investigate the ground state and the dissipative quantum dynamics of interacting charged particles in an external potential at finite temperature. The recently devised time-dependent quantum Monte Carlo (TDQMC) method allows a self-consistent treatment of the system of particles together with bath oscillators first for imaginary-time propagation of Schrödinger type of equations where both the system and the bath converge to their finite temperature ground state, and next for real time calculation where the dissipative dynamics is demonstrated. In that context the application of TDQMC appears as promising alternative to the path-integral related techniques where the real time propagation can be a challenge.

  1. Computer Visualization of Many-Particle Quantum Dynamics

    SciTech Connect

    Ozhigov, A. Y.

    2009-03-10

    In this paper I show the importance of computer visualization in researching of many-particle quantum dynamics. Such a visualization becomes an indispensable illustrative tool for understanding the behavior of dynamic swarm-based quantum systems. It is also an important component of the corresponding simulation framework, and can simplify the studies of underlying algorithms for multi-particle quantum systems.

  2. Phantom field dynamics in loop quantum cosmology

    SciTech Connect

    Samart, Daris; Gumjudpai, Burin

    2007-08-15

    We consider a dynamical system of phantom scalar field under exponential potential in the background of loop quantum cosmology. In our analysis, there is neither stable node nor repeller unstable node but only two saddle points, hence no big rip singularity. Physical solutions always possess potential energy greater than the magnitude of the negative kinetic energy. We found that the universe bounces after accelerating even in the domination of the phantom field. After bouncing, the universe finally enters the oscillatory regime.

  3. Dynamical systems and quantum bicrossproduct algebras

    NASA Astrophysics Data System (ADS)

    Arratia, Oscar; del Olmo, Mariano A.

    2002-06-01

    We present a unified study of some aspects of quantum bicrossproduct algebras of inhomogeneous Lie algebras, such as Poincaré, Galilei and Euclidean in N dimensions. The action associated with the bicrossproduct structure allows us to obtain a nonlinear action over a new group linked to the translations. This new nonlinear action associates a dynamical system with each generator which is the object of our study.

  4. Wigner flow reveals topological order in quantum phase space dynamics.

    PubMed

    Steuernagel, Ole; Kakofengitis, Dimitris; Ritter, Georg

    2013-01-18

    The behavior of classical mechanical systems is characterized by their phase portraits, the collections of their trajectories. Heisenberg's uncertainty principle precludes the existence of sharply defined trajectories, which is why traditionally only the time evolution of wave functions is studied in quantum dynamics. These studies are quite insensitive to the underlying structure of quantum phase space dynamics. We identify the flow that is the quantum analog of classical particle flow along phase portrait lines. It reveals hidden features of quantum dynamics and extra complexity. Being constrained by conserved flow winding numbers, it also reveals fundamental topological order in quantum dynamics that has so far gone unnoticed.

  5. Quantum dynamical simulations of local field enhancement in metal nanoparticles.

    PubMed

    Negre, Christian F A; Perassi, Eduardo M; Coronado, Eduardo A; Sánchez, Cristián G

    2013-03-27

    Field enhancements (Γ) around small Ag nanoparticles (NPs) are calculated using a quantum dynamical simulation formalism and the results are compared with electrodynamic simulations using the discrete dipole approximation (DDA) in order to address the important issue of the intrinsic atomistic structure of NPs. Quite remarkably, in both quantum and classical approaches the highest values of Γ are located in the same regions around single NPs. However, by introducing a complete atomistic description of the metallic NPs in optical simulations, a different pattern of the Γ distribution is obtained. Knowing the correct pattern of the Γ distribution around NPs is crucial for understanding the spectroscopic features of molecules inside hot spots. The enhancement produced by surface plasmon coupling is studied by using both approaches in NP dimers for different inter-particle distances. The results show that the trend of the variation of Γ versus inter-particle distance is different for classical and quantum simulations. This difference is explained in terms of a charge transfer mechanism that cannot be obtained with classical electrodynamics. Finally, time dependent distribution of the enhancement factor is simulated by introducing a time dependent field perturbation into the Hamiltonian, allowing an assessment of the localized surface plasmon resonance quantum dynamics.

  6. Exact quantum dynamics study of the O{sup +}+H{sub 2}(v=0,j=0){yields}OH{sup +}+H ion-molecule reaction and comparison with quasiclassical trajectory calculations

    SciTech Connect

    Martinez, Rodrigo; Lucas, Josep M.; Gimenez, Xavier; Aguilar, Antonio; Gonzalez, Miguel

    2006-04-14

    The close-coupling hyperspherical (CCH) exact quantum method was used to study the title barrierless reaction up to a collision energy (E{sub T}) of 0.75 eV, and the results compared with quasiclassical trajectory (QCT) calculations to determine the importance of quantum effects. The CCH integral cross section decreased with E{sub T} and, although the QCT results were in general quite similar to the CCH ones, they presented a significant deviation from the CCH data within the 0.2-0.6 eV collision energy range, where the QCT method did not correctly describe the reaction probability. A very good accord between both methods was obtained for the OH{sup +} vibrational distribution, where no inversion of population was found. For the OH{sup +} rotational distributions, the agreement between the CCH and QCT results was not as good as in the vibrational case, but it was satisfactory in many conditions. The kk{sup '} angular distribution showed a preferential forward character, and the CCH method produced higher forward peaks than the QCT one. All the results were interpreted considering the potential energy surface and plots of a representative sampling of reactive trajectories.

  7. Using the Chebychev expansion in quantum transport calculations.

    PubMed

    Popescu, Bogdan; Rahman, Hasan; Kleinekathöfer, Ulrich

    2015-04-21

    Irradiation by laser pulses and a fluctuating surrounding liquid environment can, for example, lead to time-dependent effects in the transport through molecular junctions. From the theoretical point of view, time-dependent theories of quantum transport are still challenging. In one of these existing transport theories, the energy-dependent coupling between molecule and leads is decomposed into Lorentzian functions. This trick has successfully been combined with quantum master approaches, hierarchical formalisms, and non-equilibrium Green's functions. The drawback of this approach is, however, its serious limitation to certain forms of the molecule-lead coupling and to higher temperatures. Tian and Chen [J. Chem. Phys. 137, 204114 (2012)] recently employed a Chebychev expansion to circumvent some of these latter problems. Here, we report on a similar approach also based on the Chebychev expansion but leading to a different set of coupled differential equations using the fact that a derivative of a zeroth-order Bessel function can again be given in terms of Bessel functions. Test calculations show the excellent numerical accuracy and stability of the presented formalism. The time span for which this Chebychev expansion scheme is valid without any restrictions on the form of the spectral density or temperature can be determined a priori.

  8. Using the Chebychev expansion in quantum transport calculations

    SciTech Connect

    Popescu, Bogdan; Rahman, Hasan; Kleinekathöfer, Ulrich

    2015-04-21

    Irradiation by laser pulses and a fluctuating surrounding liquid environment can, for example, lead to time-dependent effects in the transport through molecular junctions. From the theoretical point of view, time-dependent theories of quantum transport are still challenging. In one of these existing transport theories, the energy-dependent coupling between molecule and leads is decomposed into Lorentzian functions. This trick has successfully been combined with quantum master approaches, hierarchical formalisms, and non-equilibrium Green’s functions. The drawback of this approach is, however, its serious limitation to certain forms of the molecule-lead coupling and to higher temperatures. Tian and Chen [J. Chem. Phys. 137, 204114 (2012)] recently employed a Chebychev expansion to circumvent some of these latter problems. Here, we report on a similar approach also based on the Chebychev expansion but leading to a different set of coupled differential equations using the fact that a derivative of a zeroth-order Bessel function can again be given in terms of Bessel functions. Test calculations show the excellent numerical accuracy and stability of the presented formalism. The time span for which this Chebychev expansion scheme is valid without any restrictions on the form of the spectral density or temperature can be determined a priori.

  9. Electron Dynamics in Finite Quantum Systems

    NASA Astrophysics Data System (ADS)

    McDonald, Christopher R.

    The multiconfiguration time-dependent Hartree-Fock (MCTDHF) and multiconfiguration time-dependent Hartree (MCTDH) methods are employed to investigate nonperturbative multielectron dynamics in finite quantum systems. MCTDHF is a powerful tool that allows for the investigation of multielectron dynamics in strongly perturbed quantum systems. We have developed an MCTDHF code that is capable of treating problems involving three dimensional (3D) atoms and molecules exposed to strong laser fields. This code will allow for the theoretical treatment of multielectron phenomena in attosecond science that were previously inaccessible. These problems include complex ionization processes in pump-probe experiments on noble gas atoms, the nonlinear effects that have been observed in Ne atoms in the presence of an x-ray free-electron laser (XFEL) and the molecular rearrangement of cations after ionization. An implementation of MCTDH that is optimized for two electrons, each moving in two dimensions (2D), is also presented. This implementation of MCTDH allows for the efficient treatment of 2D spin-free systems involving two electrons; however, it does not scale well to 3D or to systems containing more that two electrons. Both MCTDHF and MCTDH were used to treat 2D problems in nanophysics and attosecond science. MCTDHF is used to investigate plasmon dynamics and the quantum breathing mode for several electrons in finite lateral quantum dots. MCTDHF is also used to study the effects of manipulating the potential of a double lateral quantum dot containing two electrons; applications to quantum computing are discussed. MCTDH is used to examine a diatomic model molecular system exposed to a strong laser field; nonsequential double ionization and high harmonic generation are studied and new processes identified and explained. An implementation of MCTDHF is developed for nonuniform tensor product grids; this will allow for the full 3D implementation of MCTDHF and will provide a means to

  10. Molecular thermodynamics of metabolism: quantum thermochemical calculations for key metabolites.

    PubMed

    Hadadi, N; Ataman, M; Hatzimanikatis, V; Panayiotou, C

    2015-04-28

    The present work is the first of a series of papers aiming at a coherent and unified development of the thermodynamics of metabolism and the rationalization of feasibility analysis of metabolic pathways. The focus in this part is on high-level quantum chemical calculations of the thermochemical quantities of relatively heavy metabolites such as amino acids/oligopeptides, nucleosides, saccharides and their derivatives in the ideal gas state. The results of this study will be combined with the corresponding hydration/solvation results in subsequent parts of this work in order to derive the desired thermochemical quantities in aqueous solutions. The above metabolites exist in a vast conformational/isomerization space including rotational conformers, tautomers or anomers exhibiting often multiple or cooperative intramolecular hydrogen bonding. We examine the challenges posed by these features for the reliable estimation of thermochemical quantities. We discuss conformer search, conformer distribution and averaging processes. We further consider neutral metabolites as well as protonated and deprotonated metabolites. In addition to the traditional presentation of gas-phase acidities, basicities and proton affinities, we also examine heats and free energies of ionic species. We obtain simple linear relations between the thermochemical quantities of ions and the formation quantities of their neutral counterparts. Furthermore, we compare our calculations with reliable experimental measurements and predictive calculations from the literature, when available. Finally, we discuss the next steps and perspectives for this work.

  11. Quantum plasmonics: from jellium models to ab initio calculations

    NASA Astrophysics Data System (ADS)

    Varas, Alejandro; García-González, Pablo; Feist, Johannes; García-Vidal, F. J.; Rubio, Angel

    2016-08-01

    Light-matter interaction in plasmonic nanostructures is often treated within the realm of classical optics. However, recent experimental findings show the need to go beyond the classical models to explain and predict the plasmonic response at the nanoscale. A prototypical system is a nanoparticle dimer, extensively studied using both classical and quantum prescriptions. However, only very recently, fully ab initio time-dependent density functional theory (TDDFT) calculations of the optical response of these dimers have been carried out. Here, we review the recent work on the impact of the atomic structure on the optical properties of such systems. We show that TDDFT can be an invaluable tool to simulate the time evolution of plasmonic modes, providing fundamental understanding into the underlying microscopical mechanisms.

  12. Conformational analysis of small molecules: NMR and quantum mechanics calculations.

    PubMed

    Tormena, Cláudio F

    2016-08-01

    This review deals with conformational analysis in small organic molecules, and describes the stereoelectronic interactions responsible for conformational stability. Conformational analysis is usually performed using NMR spectroscopy through measurement of coupling constants at room or low temperature in different solvents to determine the populations of conformers in solution. Quantum mechanical calculations are used to address the interactions responsible for conformer stability. The conformational analysis of a large number of small molecules is described, using coupling constant measurements in different solvents and at low temperature, as well as recent applications of through-space and through-hydrogen bond coupling constants JFH as tools for the conformational analysis of fluorinated molecules. Besides NMR parameters, stereoelectronic interactions such as conjugative, hyperconjugative, steric and intramolecular hydrogen bond interactions involved in conformational preferences are discussed.

  13. Vibrational spectra and quantum mechanical calculations of antiretroviral drugs: Nevirapine

    NASA Astrophysics Data System (ADS)

    Ayala, A. P.; Siesler, H. W.; Wardell, S. M. S. V.; Boechat, N.; Dabbene, V.; Cuffini, S. L.

    2007-02-01

    Nevirapine (11-cyclopropyl-5,11-dihydro-4-methyl-6H-dipyrido[3,2-b:2',3'e][1,4]diazepin-6-one) is an antiretroviral drug belonging to the class of the non-nucleoside inhibitors of the HIV-1 virus reverse transcriptase. As most of this kind of antiretroviral drugs, nevirapine displays a butterfly-like conformation which is preserved in complexes with the HIV-1 reverse transcriptase. In this work, we present a detailed vibrational spectroscopy investigation of nevirapine by using mid-infrared, near-infrared, and Raman spectroscopies. These data are supported by quantum mechanical calculations, which allow us to characterize completely the vibrational spectra of this compound. Based on these results, we discuss the correlation between the vibrational modes and the crystalline structure of the most stable form of nevirapine.

  14. Quasienergy spectra of quantum dynamical systems

    NASA Astrophysics Data System (ADS)

    Cerdeira, Hilda A.; da Silva, E. Z.; Huberman, B. A.

    1984-10-01

    We present a technique that yields in analytic fashion the quasienergy spectrum of bounded quantum systems in the presence of time-periodic perturbations. It also allows for the calculation of statistical averages using simple algebraic manipulations and provides tractable solutions even for systems with a large number of levels. We also report on numerical calculations for systems with few number of levels in and out of resonance, and which show the recurrences predicted by the Hogg-Huberman theorem

    [Phys. Rev. Lett. 48, 711 (1982); Phys. Rev. A 28, 22 (1983)].

  15. Structure an dynamics in cavity quantum electrodynamics

    SciTech Connect

    Kimble, H.J.

    1994-12-31

    Much of the theoretical background related to the radiative processes for atoms in the presence of boundaries comes from two often disjoint areas, namely cavity quantum electrodynamics and optical bistability with two-state atoms. While the former of these areas has been associated to a large degree with studies in a perturbative domain of altered associated to a large degree with studies in a perturbative domain of altered emission processes in the presence of boundaries other than those of free space, the latter is often viewed from the perspective of hysteresis cycles and device applications. With the exception of the laser, however, perhaps the most extensive investigations of quantum statistical processes in quantum optics are to be found in the literature on bistability with two-state atoms and on cavity QED. Unfortunately, the degree of overlap of these two areas has not always been fully appreciated. This circumstance is perhaps due in part to the fact that the investigation of dynamical processes in cavity QED has had as its cornerstone the Jaynes-Cummings problem, with extensions to include, for example, small amounts of dissipation. On the other hand, a principle aspect of the bistability literature has been the study of quantum fluctuations in open systems for which dissipation plays a central role, but for which the coherent quantum dynamics of the Haynes-Cummings model are to a large measure lost due to the usual assumption of large system size and weak coupling (as in the standard theory of the laser). 132 refs., 26 figs., 1 tab.

  16. The quantum dynamics of chemical reactions

    NASA Astrophysics Data System (ADS)

    Kuppermann, A.

    1983-03-01

    In this project, we developed accurate and approximate methods for calculating cross sections of elementary reactions. These methods were applied to systems of importance for the fundamental aspects of chemical dynamics and for advanced technologies of interest to the United States Air Force. The application included calculations of three-atom exchange reactions, break-up and three-body recombination collisions and vibrational quenching by reaction. These calculations improved our understanding of such processes and permitted an assessment of some approximate methods.

  17. Large Scale Electronic Structure Calculations using Quantum Chemistry Methods

    NASA Astrophysics Data System (ADS)

    Scuseria, Gustavo E.

    1998-03-01

    This talk will address our recent efforts in developing fast, linear scaling electronic structure methods for large scale applications. Of special importance is our fast multipole method( M. C. Strain, G. E. Scuseria, and M. J. Frisch, Science 271), 51 (1996). (FMM) for achieving linear scaling for the quantum Coulomb problem (GvFMM), the traditional bottleneck in quantum chemistry calculations based on Gaussian orbitals. Fast quadratures(R. E. Stratmann, G. E. Scuseria, and M. J. Frisch, Chem. Phys. Lett. 257), 213 (1996). combined with methods that avoid the Hamiltonian diagonalization( J. M. Millam and G. E. Scuseria, J. Chem. Phys. 106), 5569 (1997) have resulted in density functional theory (DFT) programs that can be applied to systems containing many hundreds of atoms and ---depending on computational resources or level of theory-- to many thousands of atoms.( A. D. Daniels, J. M. Millam and G. E. Scuseria, J. Chem. Phys. 107), 425 (1997). Three solutions for the diagonalization bottleneck will be analyzed and compared: a conjugate gradient density matrix search (CGDMS), a Hamiltonian polynomial expansion of the density matrix, and a pseudo-diagonalization method. Besides DFT, our near-field exchange method( J. C. Burant, G. E. Scuseria, and M. J. Frisch, J. Chem. Phys. 105), 8969 (1996). for linear scaling Hartree-Fock calculations will be discussed. Based on these improved capabilities, we have also developed programs to obtain vibrational frequencies (via analytic energy second derivatives) and excitation energies (through time-dependent DFT) of large molecules like porphyn or C_70. Our GvFMM has been extended to periodic systems( K. N. Kudin and G. E. Scuseria, Chem. Phys. Lett., in press.) and progress towards a Gaussian-based DFT and HF program for polymers and solids will be reported. Last, we will discuss our progress on a Laplace-transformed \\cal O(N^2) second-order pertubation theory (MP2) method.

  18. Fragment quantum mechanical calculation of proteins and its applications.

    PubMed

    He, Xiao; Zhu, Tong; Wang, Xianwei; Liu, Jinfeng; Zhang, John Z H

    2014-09-16

    Conspectus The desire to study molecular systems that are much larger than what the current state-of-the-art ab initio or density functional theory methods could handle has naturally led to the development of novel approximate methods, including semiempirical approaches, reduced-scaling methods, and fragmentation methods. The major computational limitation of ab initio methods is the scaling problem, because the cost of ab initio calculation scales nth power or worse with system size. In the past decade, the fragmentation approach based on chemical locality has opened a new door for developing linear-scaling quantum mechanical (QM) methods for large systems and for applications to large molecular systems such as biomolecules. The fragmentation approach is highly attractive from a computational standpoint. First, the ab initio calculation of individual fragments can be conducted almost independently, which makes it suitable for massively parallel computations. Second, the electron properties, such as density and energy, are typically combined in a linear fashion to reproduce those for the entire molecular system, which makes the overall computation scale linearly with the size of the system. In this Account, two fragmentation methods and their applications to macromolecules are described. They are the electrostatically embedded generalized molecular fractionation with conjugate caps (EE-GMFCC) method and the automated fragmentation quantum mechanics/molecular mechanics (AF-QM/MM) approach. The EE-GMFCC method is developed from the MFCC approach, which was initially used to obtain accurate protein-ligand QM interaction energies. The main idea of the MFCC approach is that a pair of conjugate caps (concaps) is inserted at the location where the subsystem is divided by cutting the chemical bond. In addition, the pair of concaps is fused to form molecular species such that the overcounted effect from added concaps can be properly removed. By introducing the electrostatic

  19. The effect of molecular dynamics sampling on the calculated observable gas-phase structures.

    PubMed

    Tikhonov, Denis S; Otlyotov, Arseniy A; Rybkin, Vladimir V

    2016-07-21

    In this study, we compare the performance of various ab initio molecular dynamics (MD) sampling methods for the calculation of the observable vibrationally-averaged gas-phase structures of benzene, naphthalene and anthracene molecules. Nose-Hoover (NH), canonical and quantum generalized-Langevin-equation (GLE) thermostats as well as the a posteriori quantum correction to the classical trajectories have been tested and compared to the accurate path-integral molecular dynamics (PIMD), static anharmonic vibrational calculations as well as to the experimental gas electron diffraction data. Classical sampling methods neglecting quantum effects (NH and canonical GLE thermostats) dramatically underestimate vibrational amplitudes for the bonded atom pairs, both C-H and C-C, the resulting radial distribution functions exhibit nonphysically narrow peaks. This deficiency is almost completely removed by taking the quantum effects on the nuclei into account. The quantum GLE thermostat and a posteriori correction to the canonical GLE and NH thermostatted trajectories capture most vibrational quantum effects and closely reproduce computationally expensive PIMD and experimental radial distribution functions. These methods are both computationally feasible and accurate and are therefore recommended for calculations of the observable gas-phase structures. A good performance of the quantum GLE thermostat for the gas-phase calculations is encouraging since its parameters have been originally fitted for the condensed-phase calculations. Very accurate molecular structures can be predicted by combining the equilibrium geometry obtained at a high level of electronic structure theory with vibrational amplitudes and corrections calculated using MD driven by a lower level of electronic structure theory.

  20. Dissipative dynamics of a quantum two-state system in presence of nonequilibrium quantum noise

    NASA Astrophysics Data System (ADS)

    Mann, Niklas; Brüggemann, Jochen; Thorwart, Michael

    2016-12-01

    We analyze the real-time dynamics of a quantum two-state system in the presence of nonequilibrium quantum fluctuations. The latter are generated by a coupling of the two-state system to a single electronic level of a quantum dot which carries a nonequilibrium tunneling current. We restrict to the sequential tunneling regime and calculate the dynamics of the two-state system, of the dot population, and of the nonequilibrium charge current on the basis of a diagrammatic perturbative method valid for a weak tunneling coupling. We find a nontrivial dependence of the relaxation and dephasing rates of the two-state system due to the nonequilibrium fluctuations which is directly linked to the structure of the unperturbed central system. In addition, a Heisenberg-Langevin-equation of motion allows us to calculate the correlation function of the nonequilibrium fluctuations. By this, we obtain a generalized nonequilibrium fluctuation relation which includes the equilibrium fluctuation-dissipation theorem in the limit of zero transport voltage. A straightforward extension to the case with a time-periodic ac voltage is shown.

  1. Conditional and unconditional Gaussian quantum dynamics

    NASA Astrophysics Data System (ADS)

    Genoni, Marco G.; Lami, Ludovico; Serafini, Alessio

    2016-07-01

    This article focuses on the general theory of open quantum systems in the Gaussian regime and explores a number of diverse ramifications and consequences of the theory. We shall first introduce the Gaussian framework in its full generality, including a classification of Gaussian (also known as 'general-dyne') quantum measurements. In doing so, we will give a compact proof for the parametrisation of the most general Gaussian completely positive map, which we believe to be missing in the existing literature. We will then move on to consider the linear coupling with a white noise bath, and derive the diffusion equations that describe the evolution of Gaussian states under such circumstances. Starting from these equations, we outline a constructive method to derive general master equations that apply outside the Gaussian regime. Next, we include the general-dyne monitoring of the environmental degrees of freedom and recover the Riccati equation for the conditional evolution of Gaussian states. Our derivation relies exclusively on the standard quantum mechanical update of the system state, through the evaluation of Gaussian overlaps. The parametrisation of the conditional dynamics we obtain is novel and, at variance with existing alternatives, directly ties in to physical detection schemes. We conclude our study with two examples of conditional dynamics that can be dealt with conveniently through our formalism, demonstrating how monitoring can suppress the noise in optical parametric processes as well as stabilise systems subject to diffusive scattering.

  2. Quantum critical point revisited by dynamical mean-field theory

    DOE PAGES

    Xu, Wenhu; Kotliar, Gabriel; Tsvelik, Alexei M.

    2017-03-31

    Dynamical mean-field theory is used to study the quantum critical point (QCP) in the doped Hubbard model on a square lattice. We characterize the QCP by a universal scaling form of the self-energy and a spin density wave instability at an incommensurate wave vector. The scaling form unifies the low-energy kink and the high-energy waterfall feature in the spectral function, while the spin dynamics includes both the critical incommensurate and high-energy antiferromagnetic paramagnons. Here, we use the frequency-dependent four-point correlation function of spin operators to calculate the momentum-dependent correction to the electron self-energy. Furthermore, by comparing with the calculations basedmore » on the spin-fermion model, our results indicate the frequency dependence of the quasiparticle-paramagnon vertices is an important factor to capture the momentum dependence in quasiparticle scattering.« less

  3. Self-consistent magnetization dynamics of a ferromagnetic quantum dot driven by a spin bias

    NASA Astrophysics Data System (ADS)

    Siu, Z. B.; Jalil, M. B. A.; Tan, S. G.

    2012-04-01

    We present an iterative scheme which combines the non-equilibrium Green's function (NEGF) for evaluating the quantum spin transport in a ferromagnetic quantum dot device and the Landau-Lifshitz (LL) equation for modeling the magnetization dynamics of the dot. For a given initial magnetization, the spin polarization of current and the resulting spin torque in the dot are calculated using the NEGF formalism. The torque acts on the magnetic moment of the dot, and the resultant magnetization dynamics is obtained from the LL equation. The new value of the dot's magnetization is then used as an input for the next round of NEGF calculation, and the whole process is repeated iteratively. The spin torque is thus calculated self-consistently with the dynamics of the magnetic moment of the dot. We apply this self-consistent iterative scheme to study the magnetization dynamics in an exemplary quantum dot system with an induced spin bias in the leads under varying damping conditions.

  4. Nature computes: information processing in quantum dynamical systems.

    PubMed

    Wiesner, Karoline

    2010-09-01

    Nature intrinsically computes. It has been suggested that the entire universe is a computer, in particular, a quantum computer. To corroborate this idea we require tools to quantify the information processing. Here we review a theoretical framework for quantifying information processing in a quantum dynamical system. So-called intrinsic quantum computation combines tools from dynamical systems theory, information theory, quantum mechanics, and computation theory. We will review how far the framework has been developed and what some of the main open questions are. On the basis of this framework we discuss upper and lower bounds for intrinsic information storage in a quantum dynamical system.

  5. Reversing quantum dynamics with near-optimal quantum and classical fidelity

    NASA Astrophysics Data System (ADS)

    Barnum, H.; Knill, E.

    2002-05-01

    We consider the problem of reversing quantum dynamics, with the goal of preserving an initial state's quantum entanglement or classical correlation with a reference system. We exhibit an approximate reversal operation, adapted to the initial density operator and the "noise" dynamics to be reversed. We show that its error in preserving either quantum or classical information is no more than twice that of the optimal reversal operation. Applications to quantum algorithms and information transmission are discussed.

  6. Numerically Exact Dynamics of Functional Quantum Systems - Applications to GaAs Quantum Dot Qubits and 2-DIMENSIONAL Spectra of Very Large Photosyntheitc Complexes

    NASA Astrophysics Data System (ADS)

    Dattani, Nikesh S.

    2013-06-01

    Functional quantum systems is an emerging research field which includes quantum engineering (the design of technologies that make use of quantum mechanics to outperform their classical counterparts, such as quantum computers, quantum communication devices, quantum thermometers, quantum telescopes, etc.) and the study of natural processes where quantum mechanics provides some improvement that cannot be realized with classical mechanics (possible examples are photosynthesis, animal navigation, the sense of smell, etc.). Being able to predict how a quantum mechanical system changes (ie, how its density matrix changes), given its hamiltonian, is paramount in quantum engineering as one needs to know which hamiltonian will give the desired outcome. Likewise, being able to predict density matrix dynamics in natural systems can help in understanding the system's mechanism, in controlling the system's processes, and can be helpful if designing a technology which attempts to mimic a natural process. State of the art techniques for calculating density matrix dynamics of functional quantum systems in real-time, and with numerically exact accuracy, have been developed over the last year. These techniques will be presented, followed by applications for quantum dot based quantum computing, and for calculating the 2D spectra of large biological systems.

  7. Feynman’s clock, a new variational principle, and parallel-in-time quantum dynamics

    PubMed Central

    McClean, Jarrod R.; Parkhill, John A.; Aspuru-Guzik, Alán

    2013-01-01

    We introduce a discrete-time variational principle inspired by the quantum clock originally proposed by Feynman and use it to write down quantum evolution as a ground-state eigenvalue problem. The construction allows one to apply ground-state quantum many-body theory to quantum dynamics, extending the reach of many highly developed tools from this fertile research area. Moreover, this formalism naturally leads to an algorithm to parallelize quantum simulation over time. We draw an explicit connection between previously known time-dependent variational principles and the time-embedded variational principle presented. Sample calculations are presented, applying the idea to a hydrogen molecule and the spin degrees of freedom of a model inorganic compound, demonstrating the parallel speedup of our method as well as its flexibility in applying ground-state methodologies. Finally, we take advantage of the unique perspective of this variational principle to examine the error of basis approximations in quantum dynamics. PMID:24062428

  8. Feynman's clock, a new variational principle, and parallel-in-time quantum dynamics.

    PubMed

    McClean, Jarrod R; Parkhill, John A; Aspuru-Guzik, Alán

    2013-10-08

    We introduce a discrete-time variational principle inspired by the quantum clock originally proposed by Feynman and use it to write down quantum evolution as a ground-state eigenvalue problem. The construction allows one to apply ground-state quantum many-body theory to quantum dynamics, extending the reach of many highly developed tools from this fertile research area. Moreover, this formalism naturally leads to an algorithm to parallelize quantum simulation over time. We draw an explicit connection between previously known time-dependent variational principles and the time-embedded variational principle presented. Sample calculations are presented, applying the idea to a hydrogen molecule and the spin degrees of freedom of a model inorganic compound, demonstrating the parallel speedup of our method as well as its flexibility in applying ground-state methodologies. Finally, we take advantage of the unique perspective of this variational principle to examine the error of basis approximations in quantum dynamics.

  9. Quantum corrections to inflaton and curvaton dynamics

    SciTech Connect

    Markkanen, Tommi; Tranberg, Anders E-mail: anders.tranberg@nbi.dk

    2012-11-01

    We compute the fully renormalized one-loop effective action for two interacting and self-interacting scalar fields in FRW space-time. We then derive and solve the quantum corrected equations of motion both for fields that dominate the energy density (such as an inflaton) and fields that do not (such as a subdominant curvaton). In particular, we introduce quantum corrected Friedmann equations that determine the evolution of the scale factor. We find that in general, gravitational corrections are negligible for the field dynamics. For the curvaton-type fields this leaves only the effect of the flat-space Coleman-Weinberg-type effective potential, and we find that these can be significant. For the inflaton case, both the corrections to the potential and the Friedmann equations can lead to behaviour very different from the classical evolution. Even to the point that inflation, although present at tree level, can be absent at one-loop order.

  10. Nonclassical dynamics induced by a quantum meter

    SciTech Connect

    Clausen, J.; Akulin, V. M.; Salo, J.; Stenholm, S.

    2005-12-15

    Conventionally, the effect of measurements on a quantum system is assumed to introduce decoherence, which renders the system classical-like. We consider here a microscopic meter, that is, an auxiliary essentially quantum system whose state is measured repeatedly, and show that it can be employed to induce transitions from classical states into inherently quantumlike states. The meter state is assumed to be lost in the environment and we derive a non-Markovian master equation for the dynamic system in the case of nondemolition coupling to the meter; this equation can be cast in the form of an (N{sub a})th-order differential equation in time, where N{sub a} is the dimension of the meter basis. We apply the approach to a harmonic oscillator coupled to a spin-(1/2) meter and demonstrate how it can be used to engineer effective Hamiltonian evolution, subject to decoherence induced by the projective meter measurements.

  11. Excited State Quantum-Classical Molecular Dynamics

    NASA Astrophysics Data System (ADS)

    Krstic, Predrag

    2005-05-01

    The development of a new theoretical, algorithmic, and computational framework is reported describing the corresponding excited state many-body dynamics by applying multiphysics described by classical equations of motion for nuclei and Hartree-Fock/Multi-Configuration Hartree-Fock and multiresolution techniques for solving the quantum part of the problem (i.e. the motion of the electrons). We primarily have in mind reactive and electron-transition dynamics which involves molecular clusters, containing hundreds of atoms, perturbed by a slow ionic/atomic/molecular projectile, with possible applications in plasma-surface interactions, cluster physics, chemistry and biotechnology. The validation of the developed technique is performed at three-body systems. Application to the transition dynamics in small carbon clusters and hydrocarbons perturbed by slow carbon ions resolves some long-standing issues in the ion-surface interactions in fusion tokamaks.

  12. Quantum walk coherences on a dynamical percolation graph.

    PubMed

    Elster, Fabian; Barkhofen, Sonja; Nitsche, Thomas; Novotný, Jaroslav; Gábris, Aurél; Jex, Igor; Silberhorn, Christine

    2015-08-27

    Coherent evolution governs the behaviour of all quantum systems, but in nature it is often subjected to influence of a classical environment. For analysing quantum transport phenomena quantum walks emerge as suitable model systems. In particular, quantum walks on percolation structures constitute an attractive platform for studying open system dynamics of random media. Here, we present an implementation of quantum walks differing from the previous experiments by achieving dynamical control of the underlying graph structure. We demonstrate the evolution of an optical time-multiplexed quantum walk over six double steps, revealing the intricate interplay between the internal and external degrees of freedom. The observation of clear non-Markovian signatures in the coin space testifies the high coherence of the implementation and the extraordinary degree of control of all system parameters. Our work is the proof-of-principle experiment of a quantum walk on a dynamical percolation graph, paving the way towards complex simulation of quantum transport in random media.

  13. Wave-packet dynamics of Bogoliubov quasiparticles: Quantum metric effects

    NASA Astrophysics Data System (ADS)

    Liang, Long; Peotta, Sebastiano; Harju, Ari; Törmä, Päivi

    2017-08-01

    We study the dynamics of the Bogoliubov wave packet in superconductors and calculate the supercurrent carried by the wave packet. We discover an anomalous contribution to the supercurrent, related to the quantum metric of the Bloch wave function. This anomalous contribution is most important for flat or quasiflat bands, as exemplified by the attractive Hubbard models on the Creutz ladder and sawtooth lattice. Our theoretical framework is general and can be used to study a wide variety of phenomena, such as spin transport and exciton transport.

  14. Optimal control of molecular motion expressed through quantum fluid dynamics

    NASA Astrophysics Data System (ADS)

    Dey, Bijoy K.; Rabitz, Herschel; Askar, Attila

    2000-04-01

    A quantum fluid-dynamic (QFD) control formulation is presented for optimally manipulating atomic and molecular systems. In QFD the control quantum system is expressed in terms of the probability density ρ and the quantum current j. This choice of variables is motivated by the generally expected slowly varying spatial-temporal dependence of the fluid-dynamical variables. The QFD approach is illustrated for manipulation of the ground electronic state dynamics of HCl induced by an external electric field.

  15. Calculation of strain compensation thickness for III-V semiconductor quantum dot superlattices

    NASA Astrophysics Data System (ADS)

    Polly, S. J.; Bailey, C. G.; Grede, A. J.; Forbes, D. V.; Hubbard, S. M.

    2016-11-01

    Models based on continuum elasticity theory are discussed to calculate the necessary thickness of a strain compensation (SC) layer for a superlattice (SL) of strained quantum wells (QW) or quantum dots (QD). These models are then expanded to cover material systems (substrates, QW or QD, and SC) composed of AlP, AlAs, AlSb, GaP, GaAs, GaSb, InP, InAs, or InSb, as well as the ternary, quaternary, and higher order material alloys possible in the Al/Ga/In/P/As/Sb systems. SC thickness calculation methods were compared against dynamical scattering simulations and experimental X-ray diffraction measurements of the InAs/GaP/GaAs QD/SC/Substrate superlattices of varying SC thickness. Based on the reduced (but not eliminated) strain present, a further modified strain compensation thickness is calculated to maximize the number of SL repeat units before the onset of misfit dislocations is also calculated. These models have been assembled into a free application on nanoHUB for use by the community.

  16. Quantum Phase Transition and Universal Dynamics in the Rabi Model.

    PubMed

    Hwang, Myung-Joong; Puebla, Ricardo; Plenio, Martin B

    2015-10-30

    We consider the Rabi Hamiltonian, which exhibits a quantum phase transition (QPT) despite consisting only of a single-mode cavity field and a two-level atom. We prove QPT by deriving an exact solution in the limit where the atomic transition frequency in the unit of the cavity frequency tends to infinity. The effect of a finite transition frequency is studied by analytically calculating finite-frequency scaling exponents as well as performing a numerically exact diagonalization. Going beyond this equilibrium QPT setting, we prove that the dynamics under slow quenches in the vicinity of the critical point is universal; that is, the dynamics is completely characterized by critical exponents. Our analysis demonstrates that the Kibble-Zurek mechanism can precisely predict the universal scaling of residual energy for a model without spatial degrees of freedom. Moreover, we find that the onset of the universal dynamics can be observed even with a finite transition frequency.

  17. Recombination Dynamics in Quantum Well Semiconductor Structures

    NASA Astrophysics Data System (ADS)

    Fouquet, Julie Elizabeth

    Time-resolved and time-integrated photoluminescence as a function of excitation energy density have been observed in order to study recombination dynamics in GaAs/Al(,x)Ga(,1 -x)As quantum well structures. The study of room temperature photoluminescence from the molecular beam epitaxy (MBE) -grown multiple quantum well structure and photoluminescence peak energy as a function of tem- perature shows that room temperature recombination at excitation densities above the low 10('16) cm('-3) level is due to free carriers, not excitons. This is the first study of time-resolved photoluminescence of impurities in quantum wells; data taken at different emission wave- lengths at low temperatures shows that the impurity-related states at photon energies lower than the free exciton peaks luminesce much more slowly than the free exciton states. Results from a similar structure grown by metal -organic chemical vapor deposition (MOCVD) are explained by saturation of traps. An unusual increase in decay rate observed tens of nanoseconds after excitation is probably due to carriers falling out of the trap states. Since this is the first study of time-resolved photoluminescence of MOCVD-grown quantum well structures, this unusual behavior may be realted to the MOCVD growth process. Further investigations indi- cate that the traps are not active at low temperatures; they become active at approximately 150 K. The traps are probably associated with the (hetero)interfaces rather than the bulk Al(,x)Ga(,1-x)As material. The 34 K photoluminescence spectrum of this sample revealed a peak shifted down by approximately 36 meV from the main peak. Time-resolved and time-integrated photoluminescence results here show that this peak is not a stimulated phonon emission sideband, but rather is an due to an acceptor impurity, probably carbon. Photo- luminescence for excitation above and below the barrier bandgap shows that carriers are efficiently collected in the wells in both single and multiple

  18. Warm dense iron equation of state from quantum molecular dynamics

    NASA Astrophysics Data System (ADS)

    Sjostrom, Travis; Crockett, Scott

    Through quantum molecular dynamics (QMD), utilizing both Kohn-Sham (orbital-based) and orbital-free density functional theory, we calculate the equation of state of warm dense iron in the density range 7-30 g/cm3 and temperatures from 1 to 100 eV. A critical examination of the iron pseudopotential is made, from which we find the previous QMD calculations of Wang et al. [Phys. Rev. E 89, 023101 (2014)] to be in error. Our results also significantly extend the ranges of density and temperature which are attempted in that prior work. We calculate the shock Hugoniot and find very good agreement with experimental results to pressures over 20 TPa. Additionally we have utilized the QMD results to generate a new SESAME tabular equation of state for fluid iron, accurate in the warm dense matter region, and also extending to much broader regions of density and temperature than can be accessed by the QMD alone.

  19. Topological blocking in quantum quench dynamics

    NASA Astrophysics Data System (ADS)

    Kells, G.; Sen, D.; Slingerland, J. K.; Vishveshwara, S.

    2014-06-01

    We study the nonequilibrium dynamics of quenching through a quantum critical point in topological systems, focusing on one of their defining features: ground-state degeneracies and associated topological sectors. We present the notion of "topological blocking," experienced by the dynamics due to a mismatch in degeneracies between two phases, and we argue that the dynamic evolution of the quench depends strongly on the topological sector being probed. We demonstrate this interplay between quench and topology in models stemming from two extensively studied systems, the transverse Ising chain and the Kitaev honeycomb model. Through nonlocal maps of each of these systems, we effectively study spinless fermionic p-wave paired topological superconductors. Confining the systems to ring and toroidal geometries, respectively, enables us to cleanly address degeneracies, subtle issues of fermion occupation and parity, and mismatches between topological sectors. We show that various features of the quench, which are related to Kibble-Zurek physics, are sensitive to the topological sector being probed, in particular, the overlap between the time-evolved initial ground state and an appropriate low-energy state of the final Hamiltonian. While most of our study is confined to translationally invariant systems, where momentum is a convenient quantum number, we briefly consider the effect of disorder and illustrate how this can influence the quench in a qualitatively different way depending on the topological sector considered.

  20. Colloquium: Non-Markovian dynamics in open quantum systems

    NASA Astrophysics Data System (ADS)

    Breuer, Heinz-Peter; Laine, Elsi-Mari; Piilo, Jyrki; Vacchini, Bassano

    2016-04-01

    The dynamical behavior of open quantum systems plays a key role in many applications of quantum mechanics, examples ranging from fundamental problems, such as the environment-induced decay of quantum coherence and relaxation in many-body systems, to applications in condensed matter theory, quantum transport, quantum chemistry, and quantum information. In close analogy to a classical Markovian stochastic process, the interaction of an open quantum system with a noisy environment is often modeled phenomenologically by means of a dynamical semigroup with a corresponding time-independent generator in Lindblad form, which describes a memoryless dynamics of the open system typically leading to an irreversible loss of characteristic quantum features. However, in many applications open systems exhibit pronounced memory effects and a revival of genuine quantum properties such as quantum coherence, correlations, and entanglement. Here recent theoretical results on the rich non-Markovian quantum dynamics of open systems are discussed, paying particular attention to the rigorous mathematical definition, to the physical interpretation and classification, as well as to the quantification of quantum memory effects. The general theory is illustrated by a series of physical examples. The analysis reveals that memory effects of the open system dynamics reflect characteristic features of the environment which opens a new perspective for applications, namely, to exploit a small open system as a quantum probe signifying nontrivial features of the environment it is interacting with. This Colloquium further explores the various physical sources of non-Markovian quantum dynamics, such as structured environmental spectral densities, nonlocal correlations between environmental degrees of freedom, and correlations in the initial system-environment state, in addition to developing schemes for their local detection. Recent experiments addressing the detection, quantification, and control of

  1. Quantum gravity, dynamical phase-space and string theory

    NASA Astrophysics Data System (ADS)

    Freidel, Laurent; Leigh, Robert G.; Minic, Djordje

    2014-08-01

    In a natural extension of the relativity principle, we speculate that a quantum theory of gravity involves two fundamental scales associated with both dynamical spacetime as well as dynamical momentum space. This view of quantum gravity is explicitly realized in a new formulation of string theory which involves dynamical phase-space and in which spacetime is a derived concept. This formulation naturally unifies symplectic geometry of Hamiltonian dynamics, complex geometry of quantum theory and real geometry of general relativity. The spacetime and momentum space dynamics, and thus dynamical phase-space, is governed by a new version of the renormalization group (RG).

  2. Scheme for accelerating quantum tunneling dynamics

    NASA Astrophysics Data System (ADS)

    Khujakulov, Anvar; Nakamura, Katsuhiro

    2016-02-01

    We propose a scheme of the exact fast forwarding of standard quantum dynamics for a charged particle. The present idea allows the acceleration of both the amplitude and the phase of the wave function throughout the fast-forward time range and is distinct from that of Masuda and Nakamura [Proc. R. Soc. A 466, 1135 (2010), 10.1098/rspa.2009.0446], which enabled acceleration of only the amplitude of the wave function on the way. We apply the proposed method to the quantum tunneling phenomena and obtain the electromagnetic field to ensure the rapid penetration of wave functions through a tunneling barrier. Typical examples described here are (1) an exponential wave packet passing through the δ -function barrier and (2) the opened Moshinsky shutter with a δ -function barrier just behind the shutter. We elucidate the tunneling current in the vicinity of the barrier and find a remarkable enhancement of the tunneling rate (tunneling power) due to the fast forwarding. In the case of a very high barrier, in particular, we present the asymptotic analysis and exhibit a suitable driving force to recover a recognizable tunneling current. The analysis is also carried out on the exact acceleration of macroscopic quantum tunneling with use of the nonlinear Schrödinger equation, which accommodates a tunneling barrier.

  3. Quantum dynamics of a plane pendulum

    SciTech Connect

    Leibscher, Monika; Schmidt, Burkhard

    2009-07-15

    A semianalytical approach to the quantum dynamics of a plane pendulum is developed, based on Mathieu functions which appear as stationary wave functions. The time-dependent Schroedinger equation is solved for pendular analogs of coherent and squeezed states of a harmonic oscillator, induced by instantaneous changes of the periodic potential energy function. Coherent pendular states are discussed between the harmonic limit for small displacements and the inverted pendulum limit, while squeezed pendular states are shown to interpolate between vibrational and free rotational motion. In the latter case, full and fractional revivals as well as spatiotemporal structures in the time evolution of the probability densities (quantum carpets) are quantitatively analyzed. Corresponding expressions for the mean orientation are derived in terms of Mathieu functions in time. For periodic double well potentials, different revival schemes, and different quantum carpets are found for the even and odd initial states forming the ground tunneling doublet. Time evolution of the mean alignment allows the separation of states with different parity. Implications for external (rotational) and internal (torsional) motion of molecules induced by intense laser fields are discussed.

  4. Quantum Monte Carlo Algorithms for Diagrammatic Vibrational Structure Calculations

    NASA Astrophysics Data System (ADS)

    Hermes, Matthew; Hirata, So

    2015-06-01

    Convergent hierarchies of theories for calculating many-body vibrational ground and excited-state wave functions, such as Møller-Plesset perturbation theory or coupled cluster theory, tend to rely on matrix-algebraic manipulations of large, high-dimensional arrays of anharmonic force constants, tasks which require large amounts of computer storage space and which are very difficult to implement in a parallel-scalable fashion. On the other hand, existing quantum Monte Carlo (QMC) methods for vibrational wave functions tend to lack robust techniques for obtaining excited-state energies, especially for large systems. By exploiting analytical identities for matrix elements of position operators in a harmonic oscillator basis, we have developed stochastic implementations of the size-extensive vibrational self-consistent field (MC-XVSCF) and size-extensive vibrational Møller-Plesset second-order perturbation (MC-XVMP2) theories which do not require storing the potential energy surface (PES). The programmable equations of MC-XVSCF and MC-XVMP2 take the form of a small number of high-dimensional integrals evaluated using Metropolis Monte Carlo techniques. The associated integrands require independent evaluations of only the value, not the derivatives, of the PES at many points, a task which is trivial to parallelize. However, unlike existing vibrational QMC methods, MC-XVSCF and MC-XVMP2 can calculate anharmonic frequencies directly, rather than as a small difference between two noisy total energies, and do not require user-selected coordinates or nodal surfaces. MC-XVSCF and MC-XVMP2 can also directly sample the PES in a given approximation without analytical or grid-based approximations, enabling us to quantify the errors induced by such approximations.

  5. A new ab initio potential energy surface of LiClH (1A') system and quantum dynamics calculation for Li + HCl (v = 0, j = 0-2) → LiCl + H reaction

    NASA Astrophysics Data System (ADS)

    Tan, Rui Shan; Zhai, Huan Chen; Yan, Wei; Gao, Feng; Lin, Shi Ying

    2017-04-01

    A new ab initio potential energy surface (PES) for the ground state of Li + HCl reactive system has been constructed by three-dimensional cubic spline interpolation of 36 654 ab initio points computed at the MRCI+Q/aug-cc-pV5Z level of theory. The title reaction is found to be exothermic by 5.63 kcal/mol (9 kcal/mol with zero point energy corrections), which is very close to the experimental data. The barrier height, which is 2.99 kcal/mol (0.93 kcal/mol for the vibrationally adiabatic barrier height), and the depth of van der Waals minimum located near the entrance channel are also in excellent agreement with the experimental findings. This study also identified two more van der Waals minima. The integral cross sections, rate constants, and their dependence on initial rotational states are calculated using an exact quantum wave packet method on the new PES. They are also in excellent agreement with the experimental measurements.

  6. Quantum Monte Carlo calculations of magnetic couplings in cuprates

    NASA Astrophysics Data System (ADS)

    Foyevtsova, Kateryna; Krogel, Jaron; Kim, Jeongnim; Reboredo, Fernando

    2014-03-01

    Spin excitations are generally believed to play a fundamental role in the mechanism of high temperature superconductivity in cuprates. However, accurate description of the cuprates' magnetic properties and, in particular, calculation of spin exchange couplings have been a long-standing challenge to the electronic structure theory. While the quantum-mechanically more rigorous cluster methods suffer from finite-size effects, the density functional theory approach, on the other hand, is ambiguous due to a rich variety of approximations to the exchange-correlation functional available which often give very different numbers for the spin exchange constants. For example, in some cuprates the theoretically predicted values of the nearest-neighbor superexchange range from 1 eV (local density approximation) to 0.05 eV (periodic unrestricted Hartree Fock) [C. de Graaf et al, PRB 63 014404 (2000)]. We compute spin exchange constants with the fixed-node diffusion Monte Carlo method (FN-DMC). In one-dimensional cuprates, we find that the FN-DMC computed nearest-neighbor spin superexchange is in an excellent agreement with experiment. This both demonstrates that FN-DMC is capable of describing properly the magnetism of strongly correlated oxides as well as positions this technique as the method of choice for theoretical parameterization of spin models. Research supported by the U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division.

  7. Spectroscopic, quantum chemical calculation and molecular docking of dipfluzine

    NASA Astrophysics Data System (ADS)

    Srivastava, Karnica; Srivastava, Anubha; Tandon, Poonam; Sinha, Kirti; Wang, Jing

    2016-12-01

    Molecular structure and vibrational analysis of dipfluzine (C27H29FN2O) were presented using FT-IR and FT-Raman spectroscopy and quantum chemical calculations. The theoretical ground state geometry and electronic structure of dipfluzine are optimized by the DFT/B3LYP/6-311++G (d,p) method and compared with those of the crystal data. The 1D potential energy scan was performed by varying the dihedral angle using B3LYP functional at 6-31G(d,p) level of theory and thus the most stable conformer of the compound were determined. Molecular electrostatic potential surface (MEPS), frontier orbital analysis and electronic reactivity descriptor were used to predict the chemical reactivity of molecule. Energies of intra- and inter-molecular hydrogen bonds in molecule and their electronic aspects were investigated by natural bond orbital (NBO). To find out the anti-apoptotic activity of the title compound molecular docking studies have been performed against protein Fas.

  8. Dynamical Causal Modeling from a Quantum Dynamical Perspective

    SciTech Connect

    Demiralp, Emre; Demiralp, Metin

    2010-09-30

    Recent research suggests that any set of first order linear vector ODEs can be converted to a set of specific vector ODEs adhering to what we have called ''Quantum Harmonical Form (QHF)''. QHF has been developed using a virtual quantum multi harmonic oscillator system where mass and force constants are considered to be time variant and the Hamiltonian is defined as a conic structure over positions and momenta to conserve the Hermiticity. As described in previous works, the conversion to QHF requires the matrix coefficient of the first set of ODEs to be a normal matrix. In this paper, this limitation is circumvented using a space extension approach expanding the potential applicability of this method. Overall, conversion to QHF allows the investigation of a set of ODEs using mathematical tools available to the investigation of the physical concepts underlying quantum harmonic oscillators. The utility of QHF in the context of dynamical systems and dynamical causal modeling in behavioral and cognitive neuroscience is briefly discussed.

  9. A quantum molecular dynamics study of aqueous solvation dynamics

    NASA Astrophysics Data System (ADS)

    Videla, Pablo E.; Rossky, Peter J.; Laria, D.

    2013-10-01

    Ring polymer molecular dynamics experiments have been carried out to examine effects derived from nuclear quantum fluctuations at ambient conditions on equilibrium and non-equilibrium dynamical characteristics of charge solvation by a popular simple, rigid, water model, SPC/E, and for a more recent, and flexible, q-TIP4P/F model, to examine the generality of conclusions. In particular, we have recorded the relaxation of the solvent energy gap following instantaneous, ±e charge jumps in an initially uncharged Lennard-Jones-like solute. In both charge cases, quantum effects are reflected in sharper decays at the initial stages of the relaxation, which produce up to a ˜20% reduction in the characteristic timescales describing the solvation processes. For anionic solvation, the magnitude of polarization fluctuations controlling the extent of the water proton localization in the first solvation shell is somewhat more marked than for cations, bringing the quantum solvation process closer to the classical case. Effects on the solvation response from the explicit incorporation of flexibility in the water Hamiltonian are also examined. Predictions from linear response theories for the overall relaxation profile and for the corresponding characteristic timescales are reasonably accurate for the solvation of cations, whereas we find that they are much less satisfactory for the anionic case.

  10. Heats of Segregation of BCC Binaries from ab Initio and Quantum Approximate Calculations

    NASA Technical Reports Server (NTRS)

    Good, Brian S.

    2004-01-01

    We compare dilute-limit heats of segregation for selected BCC transition metal binaries computed using ab initio and quantum approximate energy methods. Ab initio calculations are carried out using the CASTEP plane-wave pseudopotential computer code, while quantum approximate results are computed using the Bozzolo-Ferrante-Smith (BFS) method with the most recent LMTO-based parameters. Quantum approximate segregation energies are computed with and without atomistic relaxation, while the ab initio calculations are performed without relaxation. Results are discussed within the context of a segregation model driven by strain and bond-breaking effects. We compare our results with full-potential quantum calculations and with available experimental results.

  11. Calculation of heat capacities of light and heavy water by path-integral molecular dynamics

    NASA Astrophysics Data System (ADS)

    Shiga, Motoyuki; Shinoda, Wataru

    2005-10-01

    As an application of atomistic simulation methods to heat capacities, path-integral molecular dynamics has been used to calculate the constant-volume heat capacities of light and heavy water in the gas, liquid, and solid phases. While the classical simulation based on conventional molecular dynamics has estimated the heat capacities too high, the quantum simulation based on path-integral molecular dynamics has given reasonable results based on the simple point-charge/flexible potential model. The calculated heat capacities (divided by the Boltzmann constant) in the quantum simulation are 3.1 in the vapor H2O at 300 K, 6.9 in the liquid H2O at 300 K, and 4.1 in the ice IhH2O at 250 K, respectively, which are comparable to the experimental data of 3.04, 8.9, and 4.1, respectively. The quantum simulation also reproduces the isotope effect. The heat capacity in the liquid D2O has been calculated to be 10% higher than that of H2O, while it is 13% higher in the experiment. The results demonstrate that the path-integral simulation is a promising approach to quantitatively evaluate the heat capacities for molecular systems, taking account of quantum-mechanical vibrations as well as strongly anharmonic motions.

  12. Quantum nature of the big bang: Improved dynamics

    SciTech Connect

    Ashtekar, Abhay; Pawlowski, Tomasz; Singh, Parampreet

    2006-10-15

    An improved Hamiltonian constraint operator is introduced in loop quantum cosmology. Quantum dynamics of the spatially flat, isotropic model with a massless scalar field is then studied in detail using analytical and numerical methods. The scalar field continues to serve as ''emergent time'', the big bang is again replaced by a quantum bounce, and quantum evolution remains deterministic across the deep Planck regime. However, while with the Hamiltonian constraint used so far in loop quantum cosmology the quantum bounce can occur even at low matter densities, with the new Hamiltonian constraint it occurs only at a Planck-scale density. Thus, the new quantum dynamics retains the attractive features of current evolutions in loop quantum cosmology but, at the same time, cures their main weakness.

  13. Quantum Entanglement Growth under Random Unitary Dynamics

    NASA Astrophysics Data System (ADS)

    Nahum, Adam; Ruhman, Jonathan; Vijay, Sagar; Haah, Jeongwan

    2017-07-01

    Characterizing how entanglement grows with time in a many-body system, for example, after a quantum quench, is a key problem in nonequilibrium quantum physics. We study this problem for the case of random unitary dynamics, representing either Hamiltonian evolution with time-dependent noise or evolution by a random quantum circuit. Our results reveal a universal structure behind noisy entanglement growth, and also provide simple new heuristics for the "entanglement tsunami" in Hamiltonian systems without noise. In 1D, we show that noise causes the entanglement entropy across a cut to grow according to the celebrated Kardar-Parisi-Zhang (KPZ) equation. The mean entanglement grows linearly in time, while fluctuations grow like (time )1/3 and are spatially correlated over a distance ∝(time )2/3. We derive KPZ universal behavior in three complementary ways, by mapping random entanglement growth to (i) a stochastic model of a growing surface, (ii) a "minimal cut" picture, reminiscent of the Ryu-Takayanagi formula in holography, and (iii) a hydrodynamic problem involving the dynamical spreading of operators. We demonstrate KPZ universality in 1D numerically using simulations of random unitary circuits. Importantly, the leading-order time dependence of the entropy is deterministic even in the presence of noise, allowing us to propose a simple coarse grained minimal cut picture for the entanglement growth of generic Hamiltonians, even without noise, in arbitrary dimensionality. We clarify the meaning of the "velocity" of entanglement growth in the 1D entanglement tsunami. We show that in higher dimensions, noisy entanglement evolution maps to the well-studied problem of pinning of a membrane or domain wall by disorder.

  14. Optimal dynamic discrimination of similar quantum systems

    NASA Astrophysics Data System (ADS)

    Li, Baiqing

    2005-07-01

    The techniques for identifying and separating similar molecules have always been very important to chemistry and other branches of science and engineering. Similar quantum systems share comparable Hamiltonians, so their eigenenergy levels, transition dipole moments, and therefore their ordinary observable properties are alike. Traditional analytical methods have mostly been restricted by working with the subtle differences in the physical and chemical properties of the similar species. Optimal Dynamic Discrimination (ODD) aims at magnifying the dissimilarity of the agents by actively controlling their quantum evolution, drawing on the extremely rich information embedded in their dynamics. ODD is developed based on the tremendous flexibility of Optimal Control Theory (OCT) and on the practical implementation of closed-loop learning control, which has become a more and more indispensable tool for controlling quantum processes. The ODD experimental paradigm is designed to combat a number of factors that are detrimental to the discrimination of similar molecules: laser pulse noise, signal detection errors, finite time resolution in the signals, and environmental decoherence effects. It utilizes either static signals or time series signal, the latter capable of providing more information. Simulations are performed in this dissertation progressing from the wave function to the density matrix formulation, in order to study the decoherence effects. Analysis of the results reveals the roles of the adverse factors, unravels the underlying mechanisms of ODD, and provides insights on laboratory implementation. ODD emphasizes the incorporation of algorithmic development and laboratory design, and seeks to bridge the gap between theoretical/computational chemistry and experimental chemistry, with the help from applied mathematics and computer science.

  15. Modeling quantum fluid dynamics at nonzero temperatures

    PubMed Central

    Berloff, Natalia G.; Brachet, Marc; Proukakis, Nick P.

    2014-01-01

    The detailed understanding of the intricate dynamics of quantum fluids, in particular in the rapidly growing subfield of quantum turbulence which elucidates the evolution of a vortex tangle in a superfluid, requires an in-depth understanding of the role of finite temperature in such systems. The Landau two-fluid model is the most successful hydrodynamical theory of superfluid helium, but by the nature of the scale separations it cannot give an adequate description of the processes involving vortex dynamics and interactions. In our contribution we introduce a framework based on a nonlinear classical-field equation that is mathematically identical to the Landau model and provides a mechanism for severing and coalescence of vortex lines, so that the questions related to the behavior of quantized vortices can be addressed self-consistently. The correct equation of state as well as nonlocality of interactions that leads to the existence of the roton minimum can also be introduced in such description. We review and apply the ideas developed for finite-temperature description of weakly interacting Bose gases as possible extensions and numerical refinements of the proposed method. We apply this method to elucidate the behavior of the vortices during expansion and contraction following the change in applied pressure. We show that at low temperatures, during the contraction of the vortex core as the negative pressure grows back to positive values, the vortex line density grows through a mechanism of vortex multiplication. This mechanism is suppressed at high temperatures. PMID:24704874

  16. Dynamical phase transitions in quantum mechanics

    NASA Astrophysics Data System (ADS)

    Rotter, Ingrid

    2012-02-01

    The nucleus is described as an open many-body quantum system with a non-Hermitian Hamilton operator the eigenvalues of which are complex, in general. The eigenvalues may cross in the complex plane (exceptional points), the phases of the eigenfunctions are not rigid in approaching the crossing points and the widths bifurcate. By varying only one parameter, the eigenvalue trajectories usually avoid crossing and width bifurcation occurs at the critical value of avoided crossing. An analog spectroscopic redistribution takes place for discrete states below the particle decay threshold. By this means, a dynamical phase transition occurs in the many-level system starting at a critical value of the level density. Hence the properties of the low-lying nuclear states (described well by the shell model) and those of highly excited nuclear states (described by random ensembles) differ fundamentally from one another. The statement of Niels Bohr on the collective features of compound nucleus states at high level density is therefore not in contradiction to the shell-model description of nuclear (and atomic) states at low level density. Dynamical phase transitions are observed experimentally in different quantum mechanical systems by varying one or two parameters.

  17. Modeling quantum fluid dynamics at nonzero temperatures.

    PubMed

    Berloff, Natalia G; Brachet, Marc; Proukakis, Nick P

    2014-03-25

    The detailed understanding of the intricate dynamics of quantum fluids, in particular in the rapidly growing subfield of quantum turbulence which elucidates the evolution of a vortex tangle in a superfluid, requires an in-depth understanding of the role of finite temperature in such systems. The Landau two-fluid model is the most successful hydrodynamical theory of superfluid helium, but by the nature of the scale separations it cannot give an adequate description of the processes involving vortex dynamics and interactions. In our contribution we introduce a framework based on a nonlinear classical-field equation that is mathematically identical to the Landau model and provides a mechanism for severing and coalescence of vortex lines, so that the questions related to the behavior of quantized vortices can be addressed self-consistently. The correct equation of state as well as nonlocality of interactions that leads to the existence of the roton minimum can also be introduced in such description. We review and apply the ideas developed for finite-temperature description of weakly interacting Bose gases as possible extensions and numerical refinements of the proposed method. We apply this method to elucidate the behavior of the vortices during expansion and contraction following the change in applied pressure. We show that at low temperatures, during the contraction of the vortex core as the negative pressure grows back to positive values, the vortex line density grows through a mechanism of vortex multiplication. This mechanism is suppressed at high temperatures.

  18. Dynamics of open quantum spin systems: An assessment of the quantum master equation approach.

    PubMed

    Zhao, P; De Raedt, H; Miyashita, S; Jin, F; Michielsen, K

    2016-08-01

    Data of the numerical solution of the time-dependent Schrödinger equation of a system containing one spin-1/2 particle interacting with a bath of up to 32 spin-1/2 particles is used to construct a Markovian quantum master equation describing the dynamics of the system spin. The procedure of obtaining this quantum master equation, which takes the form of a Bloch equation with time-independent coefficients, accounts for all non-Markovian effects inasmuch the general structure of the quantum master equation allows. Our simulation results show that, with a few rather exotic exceptions, the Bloch-type equation with time-independent coefficients provides a simple and accurate description of the dynamics of a spin-1/2 particle in contact with a thermal bath. A calculation of the coefficients that appear in the Redfield master equation in the Markovian limit shows that this perturbatively derived equation quantitatively differs from the numerically estimated Markovian master equation, the results of which agree very well with the solution of the time-dependent Schrödinger equation.

  19. A quantifier of genuine multipartite quantum correlations and its dynamics

    NASA Astrophysics Data System (ADS)

    Wang, Xin; Qiu, Liang

    2015-03-01

    By using measurement-induced disturbance (S Luo 2008 Phys. Rev. A 77 022301), we propose a quantifier for genuine multipartite quantum correlations. The connection between this quantum correlations measure and the quantum advantage in multiport dense coding for pure three-qubit states is established. It is also used to investigate the dynamics of quantum correlations in a four-partite system. The phenomena of generation of quantum correlations and holding of quantum correlations in some time windows are found. As a byproduct, the monogamy score based on measurement-induced disturbance is related to the generalized geometric measure for pure three-qubit states.

  20. Continuous-time quantum Monte Carlo calculation of multiorbital vertex asymptotics

    NASA Astrophysics Data System (ADS)

    Kaufmann, Josef; Gunacker, Patrik; Held, Karsten

    2017-07-01

    We derive the equations for calculating the high-frequency asymptotics of the local two-particle vertex function for a multiorbital impurity model. These relate the asymptotics for a general local interaction to equal-time two-particle Green's functions, which we sample using continuous-time quantum Monte Carlo simulations with a worm algorithm. As specific examples we study the single-orbital Hubbard model and the three t2 g orbitals of SrVO3 within dynamical mean-field theory (DMFT). We demonstrate how the knowledge of the high-frequency asymptotics reduces the statistical uncertainties of the vertex and further eliminates finite-box-size effects. The proposed method benefits the calculation of nonlocal susceptibilities in DMFT and diagrammatic extensions of DMFT.

  1. Progesterone and testosterone studies by neutron scattering and nuclear magnetic resonance methods and quantum chemistry calculations

    NASA Astrophysics Data System (ADS)

    Szyczewski, A.; Hołderna-Natkaniec, K.; Natkaniec, I.

    2004-05-01

    Inelastic incoherent neutron scattering spectra of progesterone and testosterone measured at 20 and 290 K were compared with the IR spectra measured at 290 K. The Phonon Density of States spectra display well resolved peaks of low frequency internal vibration modes up to 1200 cm -1. The quantum chemistry calculations were performed by semiempirical PM3 method and by the density functional theory method with different basic sets for isolated molecule, as well as for the dimer system of testosterone. The proposed assignment of internal vibrations of normal modes enable us to conclude about the sequence of the onset of the torsion movements of the CH 3 groups. These conclusions were correlated with the results of proton molecular dynamics studies performed by NMR method. The GAUSSIAN program had been used for calculations.

  2. Dynamics in the quantum/classical limit based on selective use of the quantum potential

    SciTech Connect

    Garashchuk, Sophya Dell’Angelo, David; Rassolov, Vitaly A.

    2014-12-21

    A classical limit of quantum dynamics can be defined by compensation of the quantum potential in the time-dependent Schrödinger equation. The quantum potential is a non-local quantity, defined in the trajectory-based form of the Schrödinger equation, due to Madelung, de Broglie, and Bohm, which formally generates the quantum-mechanical features in dynamics. Selective inclusion of the quantum potential for the degrees of freedom deemed “quantum,” defines a hybrid quantum/classical dynamics, appropriate for molecular systems comprised of light and heavy nuclei. The wavefunction is associated with all of the nuclei, and the Ehrenfest, or mean-field, averaging of the force acting on the classical degrees of freedom, typical of the mixed quantum/classical methods, is avoided. The hybrid approach is used to examine evolution of light/heavy systems in the harmonic and double-well potentials, using conventional grid-based and approximate quantum-trajectory time propagation. The approximate quantum force is defined on spatial domains, which removes unphysical coupling of the wavefunction fragments corresponding to distinct classical channels or configurations. The quantum potential, associated with the quantum particle, generates forces acting on both quantum and classical particles to describe the backreaction.

  3. Quantum mechanical binding free energy calculation for phosphopeptide inhibitors of the Lck SH2 domain.

    PubMed

    Anisimov, Victor M; Cavasotto, Claudio N

    2011-07-30

    The accurate and efficient calculation of binding free energies is essential in computational biophysics. We present a linear-scaling quantum mechanical (QM)-based end-point method termed MM/QM-COSMO to calculate binding free energies in biomolecular systems, with an improved description of entropic changes. Molecular dynamics trajectories are re-evaluated using a semiempirical Hamiltonian and a continuum solvent model; translational and rotational entropies are calculated using configurational integrals, and internal entropy is calculated using the harmonic oscillator approximation. As an application, we studied the binding of a series of phosphotyrosine tetrapeptides to the human Lck SH2 domain, a key component in intracellular signal transduction, modulation of which can have therapeutic relevance in the treatment of cancer, osteoporosis, and autoimmune diseases. Calculations with molecular mechanics Poisson-Boltzmann, and generalized Born surface area methods showed large discrepancies with experimental data stemming from the enthalpic component, in agreement with an earlier report. The empirical force field-based solvent interaction energy scoring function yielded improved results, with average unsigned error of 3.6 kcal/mol, and a better ligand ranking. The MM/QM-COSMO method exhibited the best agreement both for absolute (average unsigned error = 0.7 kcal/mol) and relative binding free energy calculations. These results show the feasibility and promise of a full QM-based end-point method with an adequate balance of accuracy and computational efficiency. Copyright © 2011 Wiley Periodicals, Inc.

  4. Walking in the woods with quantum chemistry--applications of quantum chemical calculations in natural products research.

    PubMed

    Tantillo, Dean J

    2013-08-01

    This Highlight describes applications of quantum chemical calculations to problems in natural products chemistry, including the elucidation of natural product structures (distinguishing between constitutional isomers, distinguishing between diastereomers, and assigning absolute configuration) and determination of reasonable mechanisms for their formation.

  5. Dynamics of Quantum Matter with Long-Range Entanglement

    DTIC Science & Technology

    2013-06-07

    REPORT Final Report: Dynamics of quantum matter with long-range entanglement. 14. ABSTRACT 16. SECURITY CLASSIFICATION OF: Recent experiments on...ultracold atoms in optical lattices have opened a remarkable new window on the dynamics of quantum matter with long-range entanglement. The simplest...paradigm of this is the boson superfluid-insulator quantum phase transition in two spatial dimensions. This project will study the theoretical

  6. Dynamics of open bosonic quantum systems in coherent state representation

    SciTech Connect

    Dalvit, D. A. R.; Berman, G. P.; Vishik, M.

    2006-01-15

    We consider the problem of decoherence and relaxation of open bosonic quantum systems from a perspective alternative to the standard master equation or quantum trajectories approaches. Our method is based on the dynamics of expectation values of observables evaluated in a coherent state representation. We examine a model of a quantum nonlinear oscillator with a density-density interaction with a collection of environmental oscillators at finite temperature. We derive the exact solution for dynamics of observables and demonstrate a consistent perturbation approach.

  7. De Sitter Space Without Dynamical Quantum Fluctuations

    NASA Astrophysics Data System (ADS)

    Boddy, Kimberly K.; Carroll, Sean M.; Pollack, Jason

    2016-06-01

    We argue that, under certain plausible assumptions, de Sitter space settles into a quiescent vacuum in which there are no dynamical quantum fluctuations. Such fluctuations require either an evolving microstate, or time-dependent histories of out-of-equilibrium recording devices, which we argue are absent in stationary states. For a massive scalar field in a fixed de Sitter background, the cosmic no-hair theorem implies that the state of the patch approaches the vacuum, where there are no fluctuations. We argue that an analogous conclusion holds whenever a patch of de Sitter is embedded in a larger theory with an infinite-dimensional Hilbert space, including semiclassical quantum gravity with false vacua or complementarity in theories with at least one Minkowski vacuum. This reasoning provides an escape from the Boltzmann brain problem in such theories. It also implies that vacuum states do not uptunnel to higher-energy vacua and that perturbations do not decohere while slow-roll inflation occurs, suggesting that eternal inflation is much less common than often supposed. On the other hand, if a de Sitter patch is a closed system with a finite-dimensional Hilbert space, there will be Poincaré recurrences and dynamical Boltzmann fluctuations into lower-entropy states. Our analysis does not alter the conventional understanding of the origin of density fluctuations from primordial inflation, since reheating naturally generates a high-entropy environment and leads to decoherence, nor does it affect the existence of non-dynamical vacuum fluctuations such as those that give rise to the Casimir effect.

  8. Dissipative quantum dynamics in low-energy collisions of complex nuclei

    SciTech Connect

    Diaz-Torres, A.; Hinde, D. J.; Dasgupta, M.; Milburn, G. J.; Tostevin, J. A.

    2008-12-15

    Model calculations that include the effects of irreversible, environmental couplings on top of a coupled-channels dynamical description of the collision of two complex nuclei are presented. The Liouville-von Neumann equation for the time evolution of the density matrix of a dissipative system is solved numerically providing a consistent transition from coherent to decoherent (and dissipative) dynamics during the collision. Quantum decoherence and dissipation are clearly manifested in the model calculations. Energy dissipation, due to the irreversible decay of giant-dipole vibrational states of the colliding nuclei, is shown to result in a hindrance of quantum tunneling and fusion.

  9. Role of quantum statistics in multi-particle decay dynamics

    SciTech Connect

    Marchewka, Avi; Granot, Er’el

    2015-04-15

    The role of quantum statistics in the decay dynamics of a multi-particle state, which is suddenly released from a confining potential, is investigated. For an initially confined double particle state, the exact dynamics is presented for both bosons and fermions. The time-evolution of the probability to measure two-particle is evaluated and some counterintuitive features are discussed. For instance, it is shown that although there is a higher chance of finding the two bosons (as oppose to fermions, and even distinguishable particles) at the initial trap region, there is a higher chance (higher than fermions) of finding them on two opposite sides of the trap as if the repulsion between bosons is higher than the repulsion between fermions. The results are demonstrated by numerical simulations and are calculated analytically in the short-time approximation. Furthermore, experimental validation is suggested.

  10. Dynamic-local-field approximation for the quantum solids

    NASA Technical Reports Server (NTRS)

    Etters, R. D.; Danilowicz, R. L.

    1974-01-01

    A local-molecular-field description for the ground-state properties of the quantum solids is presented. The dynamical behavior of atoms contributing to the local field, which acts on an arbitrary pair of test particles, is incorporated by decoupling the pair correlations between these field atoms. The energy, pressure, compressibility, single-particle-distribution function, and the rms atomic deviations about the equilibrium lattice sites are calculated for H2, He-3, and He-4 over the volume range from 5 to 24.5 cu cm/mole. The results are in close agreement with existing Monte Carlo calculations wherever comparisons are possible. At very high pressure, the results agree with simplified descriptions which depend on negligible overlap of the system wave function between neighboring lattice sites.

  11. Geometric reduction of dynamical nonlocality in nanoscale quantum circuits

    NASA Astrophysics Data System (ADS)

    Strambini, E.; Makarenko, K. S.; Abulizi, G.; de Jong, M. P.; van der Wiel, W. G.

    2016-01-01

    Nonlocality is a key feature discriminating quantum and classical physics. Quantum-interference phenomena, such as Young’s double slit experiment, are one of the clearest manifestations of nonlocality, recently addressed as dynamical to specify its origin in the quantum equations of motion. It is well known that loss of dynamical nonlocality can occur due to (partial) collapse of the wavefunction due to a measurement, such as which-path detection. However, alternative mechanisms affecting dynamical nonlocality have hardly been considered, although of crucial importance in many schemes for quantum information processing. Here, we present a fundamentally different pathway of losing dynamical nonlocality, demonstrating that the detailed geometry of the detection scheme is crucial to preserve nonlocality. By means of a solid-state quantum-interference experiment we quantify this effect in a diffusive system. We show that interference is not only affected by decoherence, but also by a loss of dynamical nonlocality based on a local reduction of the number of quantum conduction channels of the interferometer. With our measurements and theoretical model we demonstrate that this mechanism is an intrinsic property of quantum dynamics. Understanding the geometrical constraints protecting nonlocality is crucial when designing quantum networks for quantum information processing.

  12. Geometric reduction of dynamical nonlocality in nanoscale quantum circuits.

    PubMed

    Strambini, E; Makarenko, K S; Abulizi, G; de Jong, M P; van der Wiel, W G

    2016-01-06

    Nonlocality is a key feature discriminating quantum and classical physics. Quantum-interference phenomena, such as Young's double slit experiment, are one of the clearest manifestations of nonlocality, recently addressed as dynamical to specify its origin in the quantum equations of motion. It is well known that loss of dynamical nonlocality can occur due to (partial) collapse of the wavefunction due to a measurement, such as which-path detection. However, alternative mechanisms affecting dynamical nonlocality have hardly been considered, although of crucial importance in many schemes for quantum information processing. Here, we present a fundamentally different pathway of losing dynamical nonlocality, demonstrating that the detailed geometry of the detection scheme is crucial to preserve nonlocality. By means of a solid-state quantum-interference experiment we quantify this effect in a diffusive system. We show that interference is not only affected by decoherence, but also by a loss of dynamical nonlocality based on a local reduction of the number of quantum conduction channels of the interferometer. With our measurements and theoretical model we demonstrate that this mechanism is an intrinsic property of quantum dynamics. Understanding the geometrical constraints protecting nonlocality is crucial when designing quantum networks for quantum information processing.

  13. Geometric reduction of dynamical nonlocality in nanoscale quantum circuits

    PubMed Central

    Strambini, E.; Makarenko, K. S.; Abulizi, G.; de Jong, M. P.; van der Wiel, W. G.

    2016-01-01

    Nonlocality is a key feature discriminating quantum and classical physics. Quantum-interference phenomena, such as Young’s double slit experiment, are one of the clearest manifestations of nonlocality, recently addressed as dynamical to specify its origin in the quantum equations of motion. It is well known that loss of dynamical nonlocality can occur due to (partial) collapse of the wavefunction due to a measurement, such as which-path detection. However, alternative mechanisms affecting dynamical nonlocality have hardly been considered, although of crucial importance in many schemes for quantum information processing. Here, we present a fundamentally different pathway of losing dynamical nonlocality, demonstrating that the detailed geometry of the detection scheme is crucial to preserve nonlocality. By means of a solid-state quantum-interference experiment we quantify this effect in a diffusive system. We show that interference is not only affected by decoherence, but also by a loss of dynamical nonlocality based on a local reduction of the number of quantum conduction channels of the interferometer. With our measurements and theoretical model we demonstrate that this mechanism is an intrinsic property of quantum dynamics. Understanding the geometrical constraints protecting nonlocality is crucial when designing quantum networks for quantum information processing. PMID:26732751

  14. Exponential rise of dynamical complexity in quantum computing through projections

    PubMed Central

    Burgarth, Daniel Klaus; Facchi, Paolo; Giovannetti, Vittorio; Nakazato, Hiromichi; Pascazio, Saverio; Yuasa, Kazuya

    2014-01-01

    The ability of quantum systems to host exponentially complex dynamics has the potential to revolutionize science and technology. Therefore, much effort has been devoted to developing of protocols for computation, communication and metrology, which exploit this scaling, despite formidable technical difficulties. Here we show that the mere frequent observation of a small part of a quantum system can turn its dynamics from a very simple one into an exponentially complex one, capable of universal quantum computation. After discussing examples, we go on to show that this effect is generally to be expected: almost any quantum dynamics becomes universal once ‘observed’ as outlined above. Conversely, we show that any complex quantum dynamics can be ‘purified’ into a simpler one in larger dimensions. We conclude by demonstrating that even local noise can lead to an exponentially complex dynamics. PMID:25300692

  15. Exponential rise of dynamical complexity in quantum computing through projections.

    PubMed

    Burgarth, Daniel Klaus; Facchi, Paolo; Giovannetti, Vittorio; Nakazato, Hiromichi; Pascazio, Saverio; Yuasa, Kazuya

    2014-10-10

    The ability of quantum systems to host exponentially complex dynamics has the potential to revolutionize science and technology. Therefore, much effort has been devoted to developing of protocols for computation, communication and metrology, which exploit this scaling, despite formidable technical difficulties. Here we show that the mere frequent observation of a small part of a quantum system can turn its dynamics from a very simple one into an exponentially complex one, capable of universal quantum computation. After discussing examples, we go on to show that this effect is generally to be expected: almost any quantum dynamics becomes universal once 'observed' as outlined above. Conversely, we show that any complex quantum dynamics can be 'purified' into a simpler one in larger dimensions. We conclude by demonstrating that even local noise can lead to an exponentially complex dynamics.

  16. Dynamically consistent method for mixed quantum-classical simulations: A semiclassical approach.

    PubMed

    Antipov, Sergey V; Ye, Ziyu; Ananth, Nandini

    2015-05-14

    We introduce a new semiclassical (SC) framework, the Mixed Quantum-Classical Initial Value Representation (MQC-IVR), that can be tuned to reproduce existing quantum-limit and classical-limit SC approximations to quantum real-time correlation functions. Applying a modified Filinov transformation to a quantum-limit SC formulation leads to the association of a Filinov parameter with each degree of freedom in the system; varying this parameter from zero to infinity controls the extent of quantization of the corresponding mode. The resulting MQC-IVR expression provides a consistent dynamic framework for mixed quantum-classical simulations and we demonstrate its numerical accuracy in the calculation of real-time correlation functions for a model 1D system and a model 2D system over the full range of quantum- to classical-limit behaviors.

  17. Dynamically consistent method for mixed quantum-classical simulations: A semiclassical approach

    SciTech Connect

    Antipov, Sergey V.; Ye, Ziyu; Ananth, Nandini

    2015-05-14

    We introduce a new semiclassical (SC) framework, the Mixed Quantum-Classical Initial Value Representation (MQC-IVR), that can be tuned to reproduce existing quantum-limit and classical-limit SC approximations to quantum real-time correlation functions. Applying a modified Filinov transformation to a quantum-limit SC formulation leads to the association of a Filinov parameter with each degree of freedom in the system; varying this parameter from zero to infinity controls the extent of quantization of the corresponding mode. The resulting MQC-IVR expression provides a consistent dynamic framework for mixed quantum-classical simulations and we demonstrate its numerical accuracy in the calculation of real-time correlation functions for a model 1D system and a model 2D system over the full range of quantum- to classical-limit behaviors.

  18. Quantum ring-polymer contraction method: Including nuclear quantum effects at no additional computational cost in comparison to ab initio molecular dynamics

    NASA Astrophysics Data System (ADS)

    John, Christopher; Spura, Thomas; Habershon, Scott; Kühne, Thomas D.

    2016-04-01

    We present a simple and accurate computational method which facilitates ab initio path-integral molecular dynamics simulations, where the quantum-mechanical nature of the nuclei is explicitly taken into account, at essentially no additional computational cost in comparison to the corresponding calculation using classical nuclei. The predictive power of the proposed quantum ring-polymer contraction method is demonstrated by computing various static and dynamic properties of liquid water at ambient conditions using density functional theory. This development will enable routine inclusion of nuclear quantum effects in ab initio molecular dynamics simulations of condensed-phase systems.

  19. Modification of 56ACARBO force field for molecular dynamic calculations of chitosan and its derivatives.

    PubMed

    Naumov, Vladimir S; Ignatov, Stanislav K

    2017-08-01

    The GROMOS 56ACARBO force field for the description of carbohydrates was modified for calculations of chitosan (poly-1,4-(N-acetyl)-β-D-glucopyranosamine-2) with protonated and non-protonated amino groups and its derivatives. Additional parameterization was developed on the basis of quantum chemical calculations. The modified force field (56ACARBO_CHT) allows performing the molecular dynamic calculations of chitosans with different degrees of protonation corresponding to various acidity of medium. Test calculations of the conformational transitions in the chitosan rings and polymeric chains as well as the chitosan nanocrystal dissolution demonstrate good agreement with experimental data. Graphical abstract The GROMOS 56ACARBO_CHT force field allows performing the molecular dynamic calculations of chitosans with different types of amio-group: free, protonated, substituted.

  20. Quantum dynamical structure factor of liquid neon via a quasiclassical symmetrized method

    NASA Astrophysics Data System (ADS)

    Monteferrante, Michele; Bonella, Sara; Ciccotti, Giovanni

    2013-02-01

    We apply the phase integration method for quasiclassical quantum time correlation functions [M. Monteferrante, S. Bonella, and G. Ciccotti, Mol. Phys. 109, 3015 (2011), 10.1080/00268976.2011.619506] to compute the dynamic structure factor of liquid neon. So far the method had been tested only on model systems. By comparing our results for neon with experiments and previous calculations, we demonstrate that the scheme is accurate and efficient also for a realistic model of a condensed phase system showing quantum behavior.

  1. Deterministic generation of multiparticle entanglement by quantum Zeno dynamics.

    PubMed

    Barontini, Giovanni; Hohmann, Leander; Haas, Florian; Estève, Jérôme; Reichel, Jakob

    2015-09-18

    Multiparticle entangled quantum states, a key resource in quantum-enhanced metrology and computing, are usually generated by coherent operations exclusively. However, unusual forms of quantum dynamics can be obtained when environment coupling is used as part of the state generation. In this work, we used quantum Zeno dynamics (QZD), based on nondestructive measurement with an optical microcavity, to deterministically generate different multiparticle entangled states in an ensemble of 36 qubit atoms in less than 5 microseconds. We characterized the resulting states by performing quantum tomography, yielding a time-resolved account of the entanglement generation. In addition, we studied the dependence of quantum states on measurement strength and quantified the depth of entanglement. Our results show that QZD is a versatile tool for fast and deterministic entanglement generation in quantum engineering applications. Copyright © 2015, American Association for the Advancement of Science.

  2. Strong Analog Classical Simulation of Coherent Quantum Dynamics

    NASA Astrophysics Data System (ADS)

    Wang, Dong-Sheng

    2017-02-01

    A strong analog classical simulation of general quantum evolution is proposed, which serves as a novel scheme in quantum computation and simulation. The scheme employs the approach of geometric quantum mechanics and quantum informational technique of quantum tomography, which applies broadly to cases of mixed states, nonunitary evolution, and infinite dimensional systems. The simulation provides an intriguing classical picture to probe quantum phenomena, namely, a coherent quantum dynamics can be viewed as a globally constrained classical Hamiltonian dynamics of a collection of coupled particles or strings. Efficiency analysis reveals a fundamental difference between the locality in real space and locality in Hilbert space, the latter enables efficient strong analog classical simulations. Examples are also studied to highlight the differences and gaps among various simulation methods. Funding support from NSERC of Canada and a research fellowship at Department of Physics and Astronomy, University of British Columbia are acknowledged

  3. Harnessing Disordered-Ensemble Quantum Dynamics for Machine Learning

    NASA Astrophysics Data System (ADS)

    Fujii, Keisuke; Nakajima, Kohei

    2017-08-01

    The quantum computer has an amazing potential of fast information processing. However, the realization of a digital quantum computer is still a challenging problem requiring highly accurate controls and key application strategies. Here we propose a platform, quantum reservoir computing, to solve these issues successfully by exploiting the natural quantum dynamics of ensemble systems, which are ubiquitous in laboratories nowadays, for machine learning. This framework enables ensemble quantum systems to universally emulate nonlinear dynamical systems including classical chaos. A number of numerical experiments show that quantum systems consisting of 5-7 qubits possess computational capabilities comparable to conventional recurrent neural networks of 100-500 nodes. This discovery opens up a paradigm for information processing with artificial intelligence powered by quantum physics.

  4. Quantum molecular dynamics simulations of dense matter

    SciTech Connect

    Collins, L.; Kress, J.; Troullier, N.; Lenosky, T.; Kwon, I.

    1997-12-31

    The authors have developed a quantum molecular dynamics (QMD) simulation method for investigating the properties of dense matter in a variety of environments. The technique treats a periodically-replicated reference cell containing N atoms in which the nuclei move according to the classical equations-of-motion. The interatomic forces are generated from the quantum mechanical interactions of the (between?) electrons and nuclei. To generate these forces, the authors employ several methods of varying sophistication from the tight-binding (TB) to elaborate density functional (DF) schemes. In the latter case, lengthy simulations on the order of 200 atoms are routinely performed, while for the TB, which requires no self-consistency, upwards to 1000 atoms are systematically treated. The QMD method has been applied to a variety cases: (1) fluid/plasma Hydrogen from liquid density to 20 times volume-compressed for temperatures of a thousand to a million degrees Kelvin; (2) isotopic hydrogenic mixtures, (3) liquid metals (Li, Na, K); (4) impurities such as Argon in dense hydrogen plasmas; and (5) metal/insulator transitions in rare gas systems (Ar,Kr) under high compressions. The advent of parallel versions of the methods, especially for fast eigensolvers, presage LDA simulations in the range of 500--1000 atoms and TB runs for tens of thousands of particles. This leap should allow treatment of shock chemistry as well as large-scale mixtures of species in highly transient environments.

  5. Quantum chaotic dynamics and random polynomials

    SciTech Connect

    Bogomolny, E.; Bohigas, O.; Leboeuf, P.

    1996-12-01

    We investigate the distribution of roots of polynomials of high degree with random coefficients which, among others, appear naturally in the context of {open_quotes}quantum chaotic dynamics.{close_quotes} It is shown that under quite general conditions their roots tend to concentrate near the unit circle in the complex plane. In order to further increase this tendency, we study in detail the particular case of self-inversive random polynomials and show that for them a finite portion of all roots lies exactly on the unit circle. Correlation functions of these roots are also computed analytically, and compared to the correlations of eigenvalues of random matrices. The problem of ergodicity of chaotic wavefunctions is also considered. For that purpose we introduce a family of random polynomials whose roots spread uniformly over phase space. While these results are consistent with random matrix theory predictions, they provide a new and different insight into the problem of quantum ergodicity Special attention is devoted to the role of symmetries in the distribution of roots of random polynomials.

  6. Quantum Monte Carlo study of helium clusters doped with nitrous oxide: quantum solvation and rotational dynamics.

    PubMed

    Moroni, Saverio; Blinov, Nicholas; Roy, Pierre-Nicholas

    2004-08-22

    Dynamical and structural properties of small (4)He(N)-N(2)O complexes have been analyzed using ground-state and finite-temperature Monte Carlo simulations. The effective rotational constants resulting from the ground-state calculations are in excellent agreement with the results of a recent spectroscopic study [Y. Xu et al., Phys. Rev. Lett. 91, 163401 (2003)]. After an initial decrease for cluster sizes up to N=8, the rotational constant increases, signaling a transition from a molecular complex to a quantum-solvated system. Such a turnaround is not present in the rotational constants extracted from the finite-temperature Monte Carlo calculations, performed for Boltzmann statistics, thus highlighting the importance of exchange effects to explain the decoupling between a solvated dopant and the helium motion.

  7. Heats of Segregation of BCC Binaries from Ab Initio and Quantum Approximate Calculations

    NASA Technical Reports Server (NTRS)

    Good, Brian S.

    2003-01-01

    We compare dilute-limit segregation energies for selected BCC transition metal binaries computed using ab initio and quantum approximate energy methods. Ab initio calculations are carried out using the CASTEP plane-wave pseudopotential computer code, while quantum approximate results are computed using the Bozzolo-Ferrante-Smith (BFS) method with the most recent parameters. Quantum approximate segregation energies are computed with and without atomistic relaxation. Results are discussed within the context of segregation models driven by strain and bond-breaking effects. We compare our results with full-potential quantum calculations and with available experimental results.

  8. Quantum-classical Liouville dynamics in the mapping basis

    SciTech Connect

    Kim, Hyojoon; Nassimi, Ali; Kapral, Raymond

    2008-08-28

    The quantum-classical Liouville equation describes the dynamics of a quantum subsystem coupled to a classical environment. It has been simulated using various methods, notably, surface-hopping schemes. A representation of this equation in the mapping Hamiltonian basis for the quantum subsystem is derived. The resulting equation of motion, in conjunction with expressions for quantum expectation values in the mapping basis, provides another route to the computation of the nonadiabatic dynamics of observables that does not involve surface-hopping dynamics. The quantum-classical Liouville equation is exact for the spin-boson system. This well-known model is simulated using an approximation to the evolution equation in the mapping basis, and close agreement with exact quantum results is found.

  9. Quantum-classical Liouville dynamics in the mapping basis.

    PubMed

    Kim, Hyojoon; Nassimi, Ali; Kapral, Raymond

    2008-08-28

    The quantum-classical Liouville equation describes the dynamics of a quantum subsystem coupled to a classical environment. It has been simulated using various methods, notably, surface-hopping schemes. A representation of this equation in the mapping Hamiltonian basis for the quantum subsystem is derived. The resulting equation of motion, in conjunction with expressions for quantum expectation values in the mapping basis, provides another route to the computation of the nonadiabatic dynamics of observables that does not involve surface-hopping dynamics. The quantum-classical Liouville equation is exact for the spin-boson system. This well-known model is simulated using an approximation to the evolution equation in the mapping basis, and close agreement with exact quantum results is found.

  10. Dispersion dynamics of quantum cascade lasers

    SciTech Connect

    Burghoff, David; Yang, Yang; Reno, John L.; Hu, Qing

    2016-12-20

    A key parameter underlying the efficacy of any nonlinear optical process is group velocity dispersion. In quantum cascade lasers (QCLs), there have been several recent demonstrations of devices exploiting nonlinearities in both the mid-infrared and the terahertz. Though the gain of QCLs has been well studied, the dispersion has been much less investigated, and several questions remain about its dynamics and precise origin. In this work, we use time-domain spectroscopy to investigate the dispersion of broadband terahertz QCLs, and demonstrate that contributions from both the material and the intersubband transitions are relevant. We show that in contrast to the laser gain—which is clamped to a fixed value above lasing threshold—the dispersion changes with bias even above threshold, which is a consequence of shifting intersubband populations. In conclusion, we also examine the role of higher-order dispersion in QCLs and discuss the ramifications of our result for devices utilizing nonlinear effects, such as frequency combs.

  11. Switching quantum dynamics for fast stabilization

    NASA Astrophysics Data System (ADS)

    Scaramuzza, Pierre; Ticozzi, Francesco

    2015-06-01

    Control strategies for dissipative preparation of target quantum states, both pure and mixed, and subspaces are obtained by switching between a set of available semigroup generators. We show that the class of problems of interest can be recast, from a control-theoretic perspective, into a switched-stabilization problem for linear dynamics. This is attained by a suitable affine transformation of the coherence-vector representation. In particular, we propose and compare stabilizing time-based and state-based switching rules for entangled state preparation, showing that the latter not only ensure faster convergence with respect to nonswitching methods, but can be designed so that they retain robustness with respect to initialization, as long as the target is a pure state or a subspace.

  12. Advanced Quantum Mechanical Calculation of Superheavy Ions: Energy Levels, Radiation and Finite Nuclear Size Effects

    SciTech Connect

    Glushkov, Alexander V.; Gurnitskaya, E.P.; Loboda, A.V.

    2005-10-26

    Advanced quantum approach to calculation of spectra for superheavy ions with an account of relativistic, correlation, nuclear, radiative effects is developed and based on the gauge invariant quantum electrodynamics (QED) perturbation theory (PT). The Lamb shift polarization part is calculated in the Ueling approximation, self-energy part is defined within a new non-PT procedure of Ivanov-Ivanova. Calculation results for energy levels, hyperfine structure parameters of some heavy elements ions are presented.

  13. Real-time quantum dynamics of heavy-quark systems at high temperature

    NASA Astrophysics Data System (ADS)

    Akamatsu, Yukinao

    2013-02-01

    On the basis of the closed-time-path formalism of nonequilibrium quantum field theory, we derive the real-time quantum dynamics of heavy-quark systems. Even though our primary goal is the description of heavy quarkonia, our method allows a unified description of the propagation of single heavy quarks as well as their bound states. To make calculations tractable, we deploy leading-order perturbation theory and consider the nonrelativistic limit. Various dynamical equations, such as the master equation for quantum Brownian motion and the time-evolution equation for heavy-quark and quarkonium forward correlators, are obtained from a single operator: the renormalized effective Hamiltonian. We are thus able to reproduce previous results of perturbative calculations of the drag force and the complex potential simultaneously. In addition, we present stochastic time-evolution equations for the heavy-quark and quarkonium wave function, which are equivalent to the dynamical equations.

  14. Quantum and classical non-adiabatic dynamics of Li_{2}^{+}Ne photodissociation

    NASA Astrophysics Data System (ADS)

    Pouilly, Brigitte; Monnerville, Maurice; Zanuttini, David; Gervais, Benoît

    2015-01-01

    The 3D photodissociation dynamics of Li2+Ne system is investigated by quantum calculations using the multi-configuration time-dependent Hartree (MCTDH) method and by classical simulations with the trajectory surface hopping (TSH) approach. Six electronic states of A’ symmetry and two states of A” symmetry are involved in the process. Couplings in the excitation region and two conical intersections in the vicinity of the Franck-Condon zone control the non-adiabatic nuclear dynamics. A diabatic representation including all the states and the couplings is determined. Diabatic and adiabatic populations calculated for initial excitation to pure diabatic and adiabatic states lead to a clear understanding of the mechanisms governing the non-adiabatic photodissociation process. The classical and quantum photodissociation cross-sections for absorption in two adiabatic states of the A’ symmetry are calculated. A remarkable agreement between quantum and classical results is obtained regarding the populations and the absorption cross-sections.

  15. Protected quantum computing: interleaving gate operations with dynamical decoupling sequences.

    PubMed

    Zhang, Jingfu; Souza, Alexandre M; Brandao, Frederico Dias; Suter, Dieter

    2014-02-07

    Implementing precise operations on quantum systems is one of the biggest challenges for building quantum devices in a noisy environment. Dynamical decoupling attenuates the destructive effect of the environmental noise, but so far, it has been used primarily in the context of quantum memories. Here, we experimentally demonstrate a general scheme for combining dynamical decoupling with quantum logical gate operations using the example of an electron-spin qubit of a single nitrogen-vacancy center in diamond. We achieve process fidelities >98% for gate times that are 2 orders of magnitude longer than the unprotected dephasing time T2.

  16. Efficient Quantum Private Communication Based on Dynamic Control Code Sequence

    NASA Astrophysics Data System (ADS)

    Cao, Zheng-Wen; Feng, Xiao-Yi; Peng, Jin-Ye; Zeng, Gui-Hua; Qi, Jin

    2017-04-01

    Based on chaos and quantum properties, we propose a quantum private communication scheme with dynamic control code sequence. The initial sequence is obtained via chaotic systems, and the control code sequence is derived by grouping, XOR and extracting. A shift cycle algorithm is designed to enable the dynamic change of control code sequence. Analysis shows that transmission efficiency could reach 100 % with high dynamics and security.

  17. Completely positive dynamical semigroups and quantum resonance theory

    NASA Astrophysics Data System (ADS)

    Könenberg, Martin; Merkli, Marco

    2017-07-01

    Starting from a microscopic system-environment model, we construct a quantum dynamical semigroup for the reduced evolution of the open system. The difference between the true system dynamics and its approximation by the semigroup has the following two properties: It is (linearly) small in the system-environment coupling constant for all times, and it vanishes exponentially quickly in the large time limit. Our approach is based on the quantum dynamical resonance theory.

  18. Efficient Quantum Private Communication Based on Dynamic Control Code Sequence

    NASA Astrophysics Data System (ADS)

    Cao, Zheng-Wen; Feng, Xiao-Yi; Peng, Jin-Ye; Zeng, Gui-Hua; Qi, Jin

    2016-12-01

    Based on chaos and quantum properties, we propose a quantum private communication scheme with dynamic control code sequence. The initial sequence is obtained via chaotic systems, and the control code sequence is derived by grouping, XOR and extracting. A shift cycle algorithm is designed to enable the dynamic change of control code sequence. Analysis shows that transmission efficiency could reach 100 % with high dynamics and security.

  19. Quantum Dynamical Behaviour in Complex Systems - A Semiclassical Approach

    SciTech Connect

    Ananth, Nandini

    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

  20. Density functional calculation of the structural and electronic properties of germanium quantum dots

    NASA Astrophysics Data System (ADS)

    Anas, M. M.; Gopir, G.

    2015-04-01

    We apply first principles density functional computational methods to study the structures, densities of states (DOS), and higher occupied molecular orbital (HOMO) - lowest unoccupied molecular orbital (LUMO) gaps of selected free-standing Ge semiconductor quantum dots up to 1.8nm. Our calculations are performed using numerical atomic orbital approach where linear combination of atomic orbital was applied. The surfaces of the quantum dots was passivized by hydrogen atoms. We find that surface passivation does affect the electronic properties associated with the changes of surface state, electron localization, and the energy gaps of germanium nanocrystals as well as the confinement of electrons inside the quantum dots (QDs). Our study shows that the energy gaps of germanium quantum dots decreases with the increasing dot diameter. The size-dependent variations of the computed HOMO-LUMO gaps in our quantum dots model were found to be consistent with the effects of quantum confinement reported in others theoretical and experimental calculation.

  1. Density functional calculation of the structural and electronic properties of germanium quantum dots

    SciTech Connect

    Anas, M. M.; Gopir, G.

    2015-04-24

    We apply first principles density functional computational methods to study the structures, densities of states (DOS), and higher occupied molecular orbital (HOMO) – lowest unoccupied molecular orbital (LUMO) gaps of selected free-standing Ge semiconductor quantum dots up to 1.8nm. Our calculations are performed using numerical atomic orbital approach where linear combination of atomic orbital was applied. The surfaces of the quantum dots was passivized by hydrogen atoms. We find that surface passivation does affect the electronic properties associated with the changes of surface state, electron localization, and the energy gaps of germanium nanocrystals as well as the confinement of electrons inside the quantum dots (QDs). Our study shows that the energy gaps of germanium quantum dots decreases with the increasing dot diameter. The size-dependent variations of the computed HOMO-LUMO gaps in our quantum dots model were found to be consistent with the effects of quantum confinement reported in others theoretical and experimental calculation.

  2. THE IONIC PATHWAYS OF LITHIUM CHEMISTRY IN THE EARLY UNIVERSE: QUANTUM CALCULATIONS FOR LiH{sup +} REACTING WITH H

    SciTech Connect

    Bovino, S.; Gianturco, F. A.; Stoecklin, T.

    2010-01-10

    To better understand the overall role of lithium chemistry in the early universe, reactive quantum calculations involving LiH{sup +} have been carried out and rate coefficients have been obtained. The reactive quantum calculations have been performed using a negative imaginary potential method. Infinite-order sudden approximation and the coupled state approximation have been used to simplify the angular coupling dynamics. Rate coefficients are obtained from the reactive cross sections by further integration over Boltzmann distribution of velocities. The results from the present calculations suggest that, at low redshifts (z), LiH{sup +} should be amenable to observation as imprinted on the cosmic background radiation, in contrast with its neutral counterpart. At higher z, the ionic species may disappear through both depletion reaction and three-body break-up processes.

  3. Dynamical collective calculation of supernova neutrino signals.

    PubMed

    Gava, Jérôme; Kneller, James; Volpe, Cristina; McLaughlin, G C

    2009-08-14

    We present the first calculations with three flavors of collective and shock wave effects for neutrino propagation in core-collapse supernovae using hydrodynamical density profiles and the S matrix formalism. We explore the interplay between the neutrino-neutrino interaction and the effects of multiple resonances upon the time signal of positrons in supernova observatories. A specific signature is found for the inverted hierarchy and a large third neutrino mixing angle and we predict, in this case, a dearth of lower energy positrons in Cherenkov detectors midway through the neutrino signal and the simultaneous revelation of valuable information about the original fluxes. We show that this feature is also observable with current generation neutrino detectors at the level of several sigmas.

  4. Quantum wavepacket ab initio molecular dynamics: an approach for computing dynamically averaged vibrational spectra including critical nuclear quantum effects.

    PubMed

    Sumner, Isaiah; Iyengar, Srinivasan S

    2007-10-18

    We have introduced a computational methodology to study vibrational spectroscopy in clusters inclusive of critical nuclear quantum effects. This approach is based on the recently developed quantum wavepacket ab initio molecular dynamics method that combines quantum wavepacket dynamics with ab initio molecular dynamics. The computational efficiency of the dynamical procedure is drastically improved (by several orders of magnitude) through the utilization of wavelet-based techniques combined with the previously introduced time-dependent deterministic sampling procedure measure to achieve stable, picosecond length, quantum-classical dynamics of electrons and nuclei in clusters. The dynamical information is employed to construct a novel cumulative flux/velocity correlation function, where the wavepacket flux from the quantized particle is combined with classical nuclear velocities to obtain the vibrational density of states. The approach is demonstrated by computing the vibrational density of states of [Cl-H-Cl]-, inclusive of critical quantum nuclear effects, and our results are in good agreement with experiment. A general hierarchical procedure is also provided, based on electronic structure harmonic frequencies, classical ab initio molecular dynamics, computation of nuclear quantum-mechanical eigenstates, and employing quantum wavepacket ab initio dynamics to understand vibrational spectroscopy in hydrogen-bonded clusters that display large degrees of anharmonicities.

  5. Dynamics and conductivity near quantum criticality

    NASA Astrophysics Data System (ADS)

    Gazit, Snir; Podolsky, Daniel; Auerbach, Assa; Arovas, Daniel P.

    2013-12-01

    Relativistic O(N) field theories are studied near the quantum-critical point in two space dimensions. We compute dynamical correlations by large-scale Monte Carlo simulations and numerical analytic continuation. In the ordered side, the scalar spectral function exhibits a universal peak at the Higgs mass. For N=3 and 4, we confirm its ω3 rise at low frequency. On the disordered side, the spectral function exhibits a sharp gap. For N=2, the dynamical conductivity rises above a threshold at the Higgs mass (density gap), in the superfluid (Mott insulator) phase. For charged bosons (Josephson arrays), the power-law rise above the Higgs mass increases from two to four. Approximate charge-vortex duality is reflected in the ratio of imaginary conductivities on either side of the transition. We determine the critical conductivity to be σc*=0.3(±0.1)×4e2/h and describe a generalization of the worm algorithm to N>2. We use a singular value decomposition error analysis for the numerical analytic continuation.

  6. Quantum mechanical wave packet and quasiclassical trajectory calculations for the Li + H2(+) reaction.

    PubMed

    Bulut, N; Castillo, J F; Bañares, L; Aoiz, F J

    2009-12-31

    The dynamics and kinetics of the Li + H2(+) reaction have been studied by means of quantum mechanical (QM) real wave packet, wave packet with flux operator, and quasiclassical trajectory (QCT) calculations on the ab initio potential energy surface of Martinazzo et al. [J. Chem. Phys., 2003, 119, 21]. Total initial state-selected reaction probabilities for the title reaction have been calculated for total angular momentum J = 0 at collision energies from threshold up to 1 eV. Wave packet reaction probabilities at selected values of the total angular momentum up to J = 60 are obtained using the centrifugal sudden approximation (CSA). Integral cross sections and rate constants have been calculated from the wave packet reactions probabilities by means of a refined J-shifting method and the separable rotation approximation in combination with the CSA for J > 0. The calculated rate constants as function of temperature show an Arrhenius type behavior. The QM results are found to be in overall good agreement with the corresponding QCT data.

  7. Surface Segregation Energies of BCC Binaries from Ab Initio and Quantum Approximate Calculations

    NASA Technical Reports Server (NTRS)

    Good, Brian S.

    2003-01-01

    We compare dilute-limit segregation energies for selected BCC transition metal binaries computed using ab initio and quantum approximate energy method. Ab initio calculations are carried out using the CASTEP plane-wave pseudopotential computer code, while quantum approximate results are computed using the Bozzolo-Ferrante-Smith (BFS) method with the most recent parameterization. Quantum approximate segregation energies are computed with and without atomistic relaxation. The ab initio calculations are performed without relaxation for the most part, but predicted relaxations from quantum approximate calculations are used in selected cases to compute approximate relaxed ab initio segregation energies. Results are discussed within the context of segregation models driven by strain and bond-breaking effects. We compare our results with other quantum approximate and ab initio theoretical work, and available experimental results.

  8. Quantum State Resolved Photodissociation Dynamics of the Formyl Radical.

    NASA Astrophysics Data System (ADS)

    Neyer, David William

    The photodissociation dynamics of the formyl (HCO) radical have been investigated both experimentally and theoretically. HCO molecules, produced in a molecular beam by the laser photolysis of acetaldehyde, were excited to metastable levels with quantum state resolution. The rotational and vibrational states of the CO products from the dissociation of these levels were probed by laser-induced fluorescence using a tunable vacuum ultraviolet laser. Measurement of detailed state-to-state dissociation cross sections and theoretical modeling of these dynamics have provided valuable information about the potential energy surface of the ground electronic state (X) of the HCO system. HCO was excited to predissociative levels of the first electronic state (A) characterized by their vibrational and K-rotational quantum numbers, and the rotational and vibrational populations of the CO products were measured. While the K-state excited in the HCO has little effect on the CO products, the vibrational character of the parent causes specific changes in the product state distributions. Addition of bending or C-H stretching quanta to the HCO parent leads to increased rotational excitation in the CO(nu =O) products. Adding C-O stretch to the parent state produces increased vibrational excitation in the CO products, The dynamics of this dissociation process, which involves Renner-Teller coupling between the X and A states, was modeled using classical trajectories calculated on a global X-state potential energy surface. Stimulated emission pumping (SEP) was used to prepare HCO in metastable resonances on the X state of HCO with vibrational and rotational resolution. The energies and linewidths of these resonances were measured, and the rotational and vibrational distributions of the CO products were determined. The linewidths and product state distributions show highly non-statistical behavior which depends on the vibrational character of the HCO resonance. The rotational distributions

  9. A measure of non-Markovianity for unital quantum dynamical maps

    NASA Astrophysics Data System (ADS)

    Haseli, S.; Salimi, S.; Khorashad, A. S.

    2015-09-01

    One of the most important topics in the study of the dynamics of open quantum systems is the information exchange between system and environment. Based on the features of back-flow information from an environment to a system, an approach is provided to detect non-Markovianity for unital dynamical maps. The method takes advantage of non-contraction property of the von Neumann entropy under completely positive and trace-preserving unital maps. Accordingly, for the dynamics of a single qubit as an open quantum system, the sign of the time derivative of the density matrix eigenvalues of the system determines the non-Markovianity of unital quantum dynamical maps. The main characteristics of the measure are to make the corresponding calculations and optimization procedure simpler.

  10. Quantum nonunital dynamics of spin-bath-assisted Fisher information

    SciTech Connect

    Hao, Xiang Wu, Yinzhong

    2016-04-15

    The nonunital non-Markovian dynamics of qubits immersed in a spin bath is studied without any Markovian approximation. The environmental effects on the precisions of quantum parameter estimation are taken into account. The time-dependent transfer matrix and inhomogeneity vector are obtained for the description of the open dynamical process. The dynamical behaviour of one qubit coupled to a spin bath is geometrically described by the Bloch vector. It is found out that the nonunital non-Markovian effects can engender the improvement of the precision of quantum parameter estimation. This result contributes to the environment-assisted quantum information theory.

  11. Exciton Relaxation and Electron Transfer Dynamics of Semiconductor Quantum Dots

    NASA Astrophysics Data System (ADS)

    Liu, Cunming

    Quantum dots (QDs), also referred to as colloidal semiconductor nanocrystals, exhibit unique electronic and optical properties arising from their three-dimensional confinement and strongly enhanced coulomb interactions. Developing a detailed understanding of the exciton relaxation dynamics within QDs is important not only for sake of exploring the fundamental physics of quantum confinement processes, but also for their applications. Ultrafast transient absorption (TA) spectroscopy, as a powerful tool to explore the relaxation dynamics of excitons, was employed to characterize the hot single/multiexciton relaxation dynamics at the first four exciton states of CdSe/CdZnS QDs. We observed for the first time that the hot hole can relax through two possible pathways: Intraband multiple phonon coupling and intrinsic defect trapping, with a lifetime of ˜7 ps. Additionally, an ultra-short component of ˜ 8 ps, directly associated with the Auger recombination of highly energetic exciton states, was discovered. After exploring the exciton relaxation inside QDs, ultrafast TA spectroscopy was further applied to study the electron transferring outside from QDs. By using a brand-new photocatalytic system consisting of CdSe QDs and Ni-dihydrolipoic acid (Ni-DHLA) catalyst, which has represented a robust photocatalysis of H2 from water, the photoinduced electron transfer (ET) dynamics between QD and the catalyst, one of most important steps during H2 generation, was studied. We found smaller bare CdSe QDs exhibit a better ET performance and CdS shelling on the bare QDs leads to worsen the ET. The calculations of effective mass approximation (EMA) and Marcus theory show the ET process is mainly dominated by driving force, electronic coupling strength and reorganization energy between QD and the catalyst.

  12. A perspective on quantum mechanics calculations in ADMET predictions.

    PubMed

    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.

  13. Conditional Born-Oppenheimer Dynamics: Quantum Dynamics Simulations for the Model Porphine.

    PubMed

    Albareda, Guillermo; Bofill, Josep Maria; Tavernelli, Ivano; Huarte-Larrañaga, Fermin; Illas, Francesc; Rubio, Angel

    2015-05-07

    We report a new theoretical approach to solve adiabatic quantum molecular dynamics halfway between wave function and trajectory-based methods. The evolution of a N-body nuclear wave function moving on a 3N-dimensional Born-Oppenheimer potential-energy hyper-surface is rewritten in terms of single-nuclei wave functions evolving nonunitarily on a 3-dimensional potential-energy surface that depends parametrically on the configuration of an ensemble of generally defined trajectories. The scheme is exact and, together with the use of trajectory-based statistical techniques, can be exploited to circumvent the calculation and storage of many-body quantities (e.g., wave function and potential-energy surface) whose size scales exponentially with the number of nuclear degrees of freedom. As a proof of concept, we present numerical simulations of a 2-dimensional model porphine where switching from concerted to sequential double proton transfer (and back) is induced quantum mechanically.

  14. Combining Dynamical Decoupling with Fault-Tolerant Quantum Computation

    DTIC Science & Technology

    2009-11-17

    ar X iv :0 91 1. 32 02 v1 [ qu an t- ph ] 1 7 N ov 2 00 9 Combining dynamical decoupling with fault-tolerant quantum computation Hui Khoon Ng,1...Daniel A. Lidar,2 and John Preskill1 1Institute for Quantum Information, California Institute of Technology, Pasadena, CA 91125, USA 2Departments...of Chemistry, Electrical Engineering, and Physics, and Center for Quantum Information Science & Technology, University of Southern California, Los

  15. Aging dynamics of quantum spin glasses of rotors

    NASA Astrophysics Data System (ADS)

    Kennett, Malcolm P.; Chamon, Claudio; Ye, Jinwu

    2001-12-01

    We study the long time dynamics of quantum spin glasses of rotors using the nonequilibrium Schwinger-Keldysh formalism. These models are known to have a quantum phase transition from a paramagnetic to a spin-glass phase, which we approach by looking at the divergence of the spin-relaxation rate at the transition point. In the aging regime, we determine the dynamical equations governing the time evolution of the spin response and correlation functions, and show that all terms in the equations that arise solely from quantum effects are irrelevant at long times under time reparametrization group (RPG) transformations. At long times, quantum effects enter only through the renormalization of the parameters in the dynamical equations for the classical counterpart of the rotor model. Consequently, quantum effects only modify the out-of-equilibrium fluctuation-dissipation relation (OEFDR), i.e. the ratio X between the temperature and the effective temperature, but not the form of the classical OEFDR.

  16. Post-Markovian dynamics of quantum correlations: entanglement versus discord

    NASA Astrophysics Data System (ADS)

    Mohammadi, Hamidreza

    2017-02-01

    Dynamics of an open two-qubit system is investigated in the post-Markovian regime, where the environments have a short-term memory. Each qubit is coupled to separate environment which is held in its own temperature. The inter-qubit interaction is modeled by XY-Heisenberg model in the presence of spin-orbit interaction and inhomogeneous magnetic field. The dynamical behavior of entanglement and discord has been considered. The results show that quantum discord is more robust than quantum entanglement, during the evolution. Also the asymmetric feature of quantum discord can be monitored by introducing the asymmetries due to inhomogeneity of magnetic field and temperature difference between the reservoirs. By employing proper parameters of the model, it is possible to maintain nonvanishing quantum correlation at high degree of temperature. The results can provide a useful recipe for studying dynamical behavior of two-qubit systems such as trapped spin electrons in coupled quantum dots.

  17. Hydration dynamics in water clusters via quantum molecular dynamics simulations

    SciTech Connect

    Turi, László

    2014-05-28

    We have investigated the hydration dynamics in size selected water clusters with n = 66, 104, 200, 500, and 1000 water molecules using molecular dynamics simulations. To study the most fundamental aspects of relaxation phenomena in clusters, we choose one of the simplest, still realistic, quantum mechanically treated test solute, an excess electron. The project focuses on the time evolution of the clusters following two processes, electron attachment to neutral equilibrated water clusters and electron detachment from an equilibrated water cluster anion. The relaxation dynamics is significantly different in the two processes, most notably restoring the equilibrium final state is less effective after electron attachment. Nevertheless, in both scenarios only minor cluster size dependence is observed. Significantly different relaxation patterns characterize electron detachment for interior and surface state clusters, interior state clusters relaxing significantly faster. This observation may indicate a potential way to distinguish surface state and interior state water cluster anion isomers experimentally. A comparison of equilibrium and non-equilibrium trajectories suggests that linear response theory breaks down for electron attachment at 200 K, but the results converge to reasonable agreement at higher temperatures. Relaxation following electron detachment clearly belongs to the linear regime. Cluster relaxation was also investigated using two different computational models, one preferring cavity type interior states for the excess electron in bulk water, while the other simulating non-cavity structure. While the cavity model predicts appearance of several different hydrated electron isomers in agreement with experiment, the non-cavity model locates only cluster anions with interior excess electron distribution. The present simulations show that surface isomers computed with the cavity predicting potential show similar dynamical behavior to the interior clusters of

  18. Quantum statistical effects on fusion dynamics of heavy ions

    SciTech Connect

    Ayik, S.; Yilmaz, B.; Gokalp, A.; Yilmaz, O.; Takigawa, N.

    2005-05-01

    To describe the fusion of two very heavy nuclei at near barrier energies, a generalized Langevin approach is proposed. The approach incorporates the quantum statistical fluctuations in accordance with the fluctuation and dissipation theorem. It is illustrated that the quantum statistical effects introduce an enhancement of the formation of a compound nucleus, though the quantum enhancement is somewhat less pronounced as indicated in the previous calculations.

  19. Direct calculation of (1)H(2)O T(1) NMRD profiles and EPR lineshapes for the electron spin quantum numbers S = 1, 3/2, 2, 5/2, 3, 7/2, based on the stochastic Liouville equation combined with Brownian dynamics simulation.

    PubMed

    Aman, Ken; Westlund, Per-Olof

    2007-02-14

    Direct calculation of electron spin relaxation and EPR lineshapes, based on Brownian dynamics simulation techniques and the stochastic Liouville equation approach (SLE-L) [Mol. Phys., 2004, 102, 1085-1093], is here generalized to high spin systems with spin quantum number S = 3/2, 2, 5/2, 3 and 7/2. A direct calculation method is demonstrated for electron spin-spin and spin-lattice relaxation, S-, X- and Q-band EPR-lineshapes and paramagnetic enhanced water proton T(1)- NMRD profiles. The main relaxation mechanism for the electron spin system is a stochastic second rank zero field splitting (ZFS). Brownian dynamics simulation techniques are used in describing a fluctuating ZFS interaction which comprises two parts namely the "permanent" part which is modulated by isotropic reorientation diffusion, and the transient part which is modulated by fast local distortion, which is also modelled by the isotropic rotation diffusion model. The SLE-L approach present is applicable both in the perturbation (Redfield) regime as well as outside the perturbation regime, in the so called slow motion regime.

  20. Dynamic homotopy and landscape dynamical set topology in quantum control

    SciTech Connect

    Dominy, Jason; Rabitz, Herschel

    2012-08-15

    We examine the topology of the subset of controls taking a given initial state to a given final state in quantum control, where 'state' may mean a pure state Double-Vertical-Line {psi}>, an ensemble density matrix {rho}, or a unitary propagator U(0, T). The analysis consists in showing that the endpoint map acting on control space is a Hurewicz fibration for a large class of affine control systems with vector controls. Exploiting the resulting fibration sequence and the long exact sequence of basepoint-preserving homotopy classes of maps, we show that the indicated subset of controls is homotopy equivalent to the loopspace of the state manifold. This not only allows us to understand the connectedness of 'dynamical sets' realized as preimages of subsets of the state space through this endpoint map, but also provides a wealth of additional topological information about such subsets of control space.

  1. Quantum and classical dynamics in adiabatic computation

    NASA Astrophysics Data System (ADS)

    Crowley, P. J. D.; Äńurić, T.; Vinci, W.; Warburton, P. A.; Green, A. G.

    2014-10-01

    Adiabatic transport provides a powerful way to manipulate quantum states. By preparing a system in a readily initialized state and then slowly changing its Hamiltonian, one may achieve quantum states that would otherwise be inaccessible. Moreover, a judicious choice of final Hamiltonian whose ground state encodes the solution to a problem allows adiabatic transport to be used for universal quantum computation. However, the dephasing effects of the environment limit the quantum correlations that an open system can support and degrade the power of such adiabatic computation. We quantify this effect by allowing the system to evolve over a restricted set of quantum states, providing a link between physically inspired classical optimization algorithms and quantum adiabatic optimization. This perspective allows us to develop benchmarks to bound the quantum correlations harnessed by an adiabatic computation. We apply these to the D-Wave Vesuvius machine with revealing—though inconclusive—results.

  2. Dynamic quantum tunneling in mesoscopic driven Duffing oscillators.

    PubMed

    Guo, Lingzhen; Zheng, Zhigang; Li, Xin-Qi; Yan, Yijing

    2011-07-01

    We investigate the dynamic quantum tunneling between two attractors of a mesoscopic driven Duffing oscillator. We find that, in addition to inducing a remarkable quantum shift of the bifurcation point, the mesoscopic nature also results in a perfect linear scaling behavior for the tunneling rate with the driving distance to the shifted bifurcation point.

  3. Quantum chemical calculation of the equilibrium structures of small metal atom clusters

    NASA Technical Reports Server (NTRS)

    Kahn, L. R.

    1982-01-01

    Metal atom clusters are studied based on the application of ab initio quantum mechanical approaches. Because these large 'molecular' systems pose special practical computational problems in the application of the quantum mechanical methods, there is a special need to find simplifying techniques that do not compromise the reliability of the calculations. Research is therefore directed towards various aspects of the implementation of the effective core potential technique for the removal of the metal atom core electrons from the calculations.

  4. On classical and quantum dynamics of tachyon-like fields and their cosmological implications

    NASA Astrophysics Data System (ADS)

    Dimitrijević, Dragoljub D.; Djordjević, Goran S.; Milošević, Milan; Vulcanov, Dumitru

    2014-11-01

    We consider a class of tachyon-like potentials, motivated by string theory, D-brane dynamics and inflation theory in the context of classical and quantum mechanics. A formalism for describing dynamics of tachyon fields in spatially homogenous and one-dimensional - classical and quantum mechanical limit is proposed. A few models with concrete potentials are considered. Additionally, possibilities for p-adic and adelic generalization of these models are discussed. Classical actions and corresponding quantum propagators, in the Feynman path integral approach, are calculated in a form invariant on a change of the background number fields, i.e. on both archimedean and nonarchimedean spaces. Looking for a quantum origin of inflation, relevance of p-adic and adelic generalizations are briefly discussed.

  5. On classical and quantum dynamics of tachyon-like fields and their cosmological implications

    SciTech Connect

    Dimitrijević, Dragoljub D. Djordjević, Goran S. Milošević, Milan; Vulcanov, Dumitru

    2014-11-24

    We consider a class of tachyon-like potentials, motivated by string theory, D-brane dynamics and inflation theory in the context of classical and quantum mechanics. A formalism for describing dynamics of tachyon fields in spatially homogenous and one-dimensional - classical and quantum mechanical limit is proposed. A few models with concrete potentials are considered. Additionally, possibilities for p-adic and adelic generalization of these models are discussed. Classical actions and corresponding quantum propagators, in the Feynman path integral approach, are calculated in a form invariant on a change of the background number fields, i.e. on both archimedean and nonarchimedean spaces. Looking for a quantum origin of inflation, relevance of p-adic and adelic generalizations are briefly discussed.

  6. Spin dynamics of an individual Cr atom in a semiconductor quantum dot under optical excitation

    SciTech Connect

    Lafuente-Sampietro, A.; Utsumi, H.; Kuroda, S.; Boukari, H.; Besombes, L.

    2016-08-01

    We studied the spin dynamics of a Cr atom incorporated in a II-VI semiconductor quantum dot using photon correlation techniques. We used recently developed singly Cr-doped CdTe/ZnTe quantum dots to access the spin of an individual magnetic atom. Auto-correlation of the photons emitted by the quantum dot under continuous wave optical excitation reveals fluctuations of the localized spin with a timescale in the 10 ns range. Cross-correlation gives quantitative transfer time between Cr spin states. A calculation of the time dependence of the spin levels population in Cr-doped quantum dots shows that the observed spin dynamics is dominated by the exciton-Cr interaction. These measurements also provide a lower bound in the 20 ns range for the intrinsic Cr spin relaxation time.

  7. A New Dynamical Reflection Algebra and Related Quantum Integrable Systems

    NASA Astrophysics Data System (ADS)

    Avan, Jean; Ragoucy, Eric

    2012-07-01

    We propose a new dynamical reflection algebra, distinct from the previous dynamical boundary algebra and semi-dynamical reflection algebra. The associated Yang-Baxter equations, coactions, fusions, and commuting traces are derived. Explicit examples are given and quantum integrable Hamiltonians are constructed. They exhibit features similar to the Ruijsenaars-Schneider Hamiltonians.

  8. Quantum Mechanical Calculations of Monoxides of Silicon Carbide Molecules

    DTIC Science & Technology

    2003-03-01

    discovery of quantum mechanics was finding an equation which gives t ),( trvψ . This was accomplished in 1926 by Erwin Schrödinger. The fundamental...permittivity of free space 16 Before we plug this potential into the Schrodinger equation and attempt to find a wavefunction, we also need to...the same is lifted. The first effect to consider is that the Schrödinger equation does not consider relativistic effects. When the Schrodinger

  9. Generalized dynamic scaling for quantum critical relaxation in imaginary time.

    PubMed

    Zhang, Shuyi; Yin, Shuai; Zhong, Fan

    2014-10-01

    We study the imaginary-time relaxation critical dynamics of a quantum system with a vanishing initial correlation length and an arbitrary initial order parameter M0. We find that in quantum critical dynamics, the behavior of M0 under scale transformations deviates from a simple power law, which was proposed for very small M0 previously. A universal characteristic function is then suggested to describe the rescaled initial magnetization, similar to classical critical dynamics. This characteristic function is shown to be able to describe the quantum critical dynamics in both short- and long-time stages of the evolution. The one-dimensional transverse-field Ising model is employed to numerically determine the specific form of the characteristic function. We demonstrate that it is applicable as long as the system is in the vicinity of the quantum critical point. The universality of the characteristic function is confirmed by numerical simulations of models belonging to the same universality class.

  10. Noether's theorem for dissipative quantum dynamical semi-groups

    NASA Astrophysics Data System (ADS)

    Gough, John E.; Ratiu, Tudor S.; Smolyanov, Oleg G.

    2015-02-01

    Noether's theorem on constants of the motion of dynamical systems has recently been extended to classical dissipative systems (Markovian semi-groups) by Baez and Fong [J. Math. Phys. 54, 013301 (2013)]. We show how to extend these results to the fully quantum setting of quantum Markov dynamics. For finite-dimensional Hilbert spaces, we construct a mapping from observables to completely positive maps that leads to the natural analogue of their criterion of commutativity with the infinitesimal generator of the Markov dynamics. Using standard results on the relaxation of states to equilibrium under quantum dynamical semi-groups, we are able to characterise the constants of the motion under quantum Markov evolutions in the infinite-dimensional setting under the usual assumption of existence of a stationary strictly positive density matrix. In particular, the Noether constants are identified with the fixed point of the Heisenberg picture semi-group.

  11. Modified quantum-speed-limit bounds for open quantum dynamics in quantum channels

    NASA Astrophysics Data System (ADS)

    Liu, Xin; Wu, Wei; Wang, Chao

    2017-05-01

    The minimal evolution time between two distinguishable states is of fundamental interest in quantum physics. Very recently Mirkin et al. [Phys. Rev. A 94, 052125 (2016), 10.1103/PhysRevA.94.052125] argued that some of the most common quantum-speed-limit (QSL) bounds which depend on the actual evolution time do not cleave to the essence of the QSL theory as they grow indefinitely but the final state is reached at a finite time in a damped Jaynes-Cummings model. In this paper, we thoroughly study this puzzling phenomenon. We find the inconsistent estimates will happen if and only if the limit of resolution of a calculation program is achieved, through which we propose that the nature of the inconsistency is not a violation of the essence of the QSL theory but an illusion caused by the finite precision in numerical simulations. We also present a generic method to overcome the inconsistent estimates and confirm its effectiveness in both amplitude-damping and phase-damping channels. Additionally, we show special cases which may restrict the QSL bound defined by "quantumness".

  12. First principles calculation of thermo-mechanical properties of thoria using Quantum ESPRESSO

    NASA Astrophysics Data System (ADS)

    Malakkal, Linu; Szpunar, Barbara; Zuniga, Juan Carlos; Siripurapu, Ravi Kiran; Szpunar, Jerzy A.

    2016-05-01

    In this work, we have used Quantum ESPRESSO (QE), an open source first principles code, based on density-functional theory, plane waves, and pseudopotentials, along with quasi-harmonic approximation (QHA) to calculate the thermo-mechanical properties of thorium dioxide (ThO2). Using Python programming language, our group developed qe-nipy-advanced, an interface to QE, which can evaluate the structural and thermo-mechanical properties of materials. We predicted the phonon contribution to thermal conductivity (kL) using the Slack model. We performed the calculations within local density approximation (LDA) and generalized gradient approximation (GGA) with the recently proposed version for solids (PBEsol). We employed a Monkhorst-Pack 5 × 5 × 5 k-points mesh in reciprocal space with a plane wave cut-off energy of 150 Ry to obtain the convergence of the structure. We calculated the dynamical matrices of the lattice on a 4 × 4 × 4 mesh. We have predicted the heat capacity, thermal expansion and the phonon contribution to thermal conductivity, as a function of temperature up to 1400K, and compared them with the previous work and known experimental results.

  13. Observing the nonequilibrium dynamics of the quantum transverse-field Ising chain in circuit QED.

    PubMed

    Viehmann, Oliver; von Delft, Jan; Marquardt, Florian

    2013-01-18

    We show how a quantum Ising spin chain in a time-dependent transverse magnetic field can be simulated and experimentally probed in the framework of circuit QED with current technology. The proposed setup provides a new platform for observing the nonequilibrium dynamics of interacting many-body systems. We calculate its spectrum to offer a guideline for its initial experimental characterization. We demonstrate that quench dynamics and the propagation of localized excitations can be observed with the proposed setup and discuss further possible applications and modifications of this circuit QED quantum simulator.

  14. First-principles calculations: half-metallic Au-V(Cr) quantum wires as spin filters.

    PubMed

    Min, Y; Yao, K L; Liu, Z L; Gao, G Y; Cheng, H G; Zhu, S C

    2009-03-04

    The half-metallic behavior of Au-V(Cr) quantum wires adsorbed on an armchair (5, 5) boron nitride nanotube is obtained by performing spin-polarized density functional calculations. The density of states shows a metallic property at the Fermi level for the majority spin channel and a semiconductor gap in the minority spin channel. The half-metallic behavior of the quantum wire/nanotube complex originates from the half-metallic behavior of the free-standing Au-V(Cr) quantum wires. The calculations of spin-polarized transport indicate that such a one-dimensional half-metallic magnet can be used as a spin filter.

  15. Communication: Relation of centroid molecular dynamics and ring-polymer molecular dynamics to exact quantum dynamics.

    PubMed

    Hele, Timothy J H; Willatt, Michael J; Muolo, Andrea; Althorpe, Stuart C

    2015-05-21

    We recently obtained a quantum-Boltzmann-conserving classical dynamics by making a single change to the derivation of the "Classical Wigner" approximation. Here, we show that the further approximation of this "Matsubara dynamics" gives rise to two popular heuristic methods for treating quantum Boltzmann time-correlation functions: centroid molecular dynamics (CMD) and ring-polymer molecular dynamics (RPMD). We show that CMD is a mean-field approximation to Matsubara dynamics, obtained by discarding (classical) fluctuations around the centroid, and that RPMD is the result of discarding a term in the Matsubara Liouvillian which shifts the frequencies of these fluctuations. These findings are consistent with previous numerical results and give explicit formulae for the terms that CMD and RPMD leave out.

  16. Dispersion dynamics of quantum cascade lasers

    DOE PAGES

    Burghoff, David; Yang, Yang; Reno, John L.; ...

    2016-12-20

    A key parameter underlying the efficacy of any nonlinear optical process is group velocity dispersion. In quantum cascade lasers (QCLs), there have been several recent demonstrations of devices exploiting nonlinearities in both the mid-infrared and the terahertz. Though the gain of QCLs has been well studied, the dispersion has been much less investigated, and several questions remain about its dynamics and precise origin. In this work, we use time-domain spectroscopy to investigate the dispersion of broadband terahertz QCLs, and demonstrate that contributions from both the material and the intersubband transitions are relevant. We show that in contrast to the lasermore » gain—which is clamped to a fixed value above lasing threshold—the dispersion changes with bias even above threshold, which is a consequence of shifting intersubband populations. In conclusion, we also examine the role of higher-order dispersion in QCLs and discuss the ramifications of our result for devices utilizing nonlinear effects, such as frequency combs.« less

  17. Quantum dynamical framework for Brownian heat engines

    NASA Astrophysics Data System (ADS)

    Agarwal, G. S.; Chaturvedi, S.

    2013-07-01

    We present a self-contained formalism modeled after the Brownian motion of a quantum harmonic oscillator for describing the performance of microscopic Brownian heat engines such as Carnot, Stirling, and Otto engines. Our theory, besides reproducing the standard thermodynamics results in the steady state, enables us to study the role dissipation plays in determining the efficiency of Brownian heat engines under actual laboratory conditions. In particular, we analyze in detail the dynamics associated with decoupling a system in equilibrium with one bath and recoupling it to another bath and obtain exact analytical results, which are shown to have significant ramifications on the efficiencies of engines involving such a step. We also develop a simple yet powerful technique for computing corrections to the steady state results arising from finite operation time and use it to arrive at the thermodynamic complementarity relations for various operating conditions and also to compute the efficiencies of the three engines cited above at maximum power. Some of the methods and exactly solvable models presented here are interesting in their own right and could find useful applications in other contexts as well.

  18. Time-Sliced Thawed Gaussian Propagation Method for Simulations of Quantum Dynamics.

    PubMed

    Kong, Xiangmeng; Markmann, Andreas; Batista, Victor S

    2016-05-19

    A rigorous method for simulations of quantum dynamics is introduced on the basis of concatenation of semiclassical thawed Gaussian propagation steps. The time-evolving state is represented as a linear superposition of closely overlapping Gaussians that evolve in time according to their characteristic equations of motion, integrated by fourth-order Runge-Kutta or velocity Verlet. The expansion coefficients of the initial superposition are updated after each semiclassical propagation period by implementing the Husimi Transform analytically in the basis of closely overlapping Gaussians. An advantage of the resulting time-sliced thawed Gaussian (TSTG) method is that it allows for full-quantum dynamics propagation without any kind of multidimensional integral calculation, or inversion of overlap matrices. The accuracy of the TSTG method is demonstrated as applied to simulations of quantum tunneling, showing quantitative agreement with benchmark calculations based on the split-operator Fourier transform method.

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

    NASA Technical Reports Server (NTRS)

    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.

  20. Quantum analysis applied to thermo field dynamics on dissipative systems

    SciTech Connect

    Hashizume, Yoichiro; Okamura, Soichiro; Suzuki, Masuo

    2015-03-10

    Thermo field dynamics is one of formulations useful to treat statistical mechanics in the scheme of field theory. In the present study, we discuss dissipative thermo field dynamics of quantum damped harmonic oscillators. To treat the effective renormalization of quantum dissipation, we use the Suzuki-Takano approximation. Finally, we derive a dissipative von Neumann equation in the Lindbrad form. In the present treatment, we can easily obtain the initial damping shown previously by Kubo.

  1. Effective quantum dynamics of interacting systems with inhomogeneous coupling

    SciTech Connect

    Lopez, C. E.; Retamal, J. C.; Christ, H.; Solano, E.

    2007-03-15

    We study the quantum dynamics of a single mode (particle) interacting inhomogeneously with a large number of particles and introduce an effective approach to find the accessible Hilbert space, where the dynamics takes place. Two relevant examples are given: the inhomogeneous Tavis-Cummings model (e.g., N atomic qubits coupled to a single cavity mode, or to a motional mode in trapped ions) and the inhomogeneous coupling of an electron spin to N nuclear spins in a quantum dot.

  2. Fractional Spin Fluctuations as a Precursor of Quantum Spin Liquids: Majorana Dynamical Mean-Field Study for the Kitaev Model.

    PubMed

    Yoshitake, Junki; Nasu, Joji; Motome, Yukitoshi

    2016-10-07

    Experimental identification of quantum spin liquids remains a challenge, as the pristine nature is to be seen in asymptotically low temperatures. We here theoretically show that the precursor of quantum spin liquids appears in the spin dynamics in the paramagnetic state over a wide temperature range. Using the cluster dynamical mean-field theory and the continuous-time quantum Monte Carlo method, which are newly developed in the Majorana fermion representation, we calculate the dynamical spin structure factor, relaxation rate in nuclear magnetic resonance, and magnetic susceptibility for the honeycomb Kitaev model whose ground state is a canonical example of the quantum spin liquid. We find that dynamical spin correlations show peculiar temperature and frequency dependence even below the temperature where static correlations saturate. The results provide the experimentally accessible symptoms of the fluctuating fractionalized spins evincing the quantum spin liquids.

  3. Fractional Spin Fluctuations as a Precursor of Quantum Spin Liquids: Majorana Dynamical Mean-Field Study for the Kitaev Model

    NASA Astrophysics Data System (ADS)

    Yoshitake, Junki; Nasu, Joji; Motome, Yukitoshi

    2016-10-01

    Experimental identification of quantum spin liquids remains a challenge, as the pristine nature is to be seen in asymptotically low temperatures. We here theoretically show that the precursor of quantum spin liquids appears in the spin dynamics in the paramagnetic state over a wide temperature range. Using the cluster dynamical mean-field theory and the continuous-time quantum Monte Carlo method, which are newly developed in the Majorana fermion representation, we calculate the dynamical spin structure factor, relaxation rate in nuclear magnetic resonance, and magnetic susceptibility for the honeycomb Kitaev model whose ground state is a canonical example of the quantum spin liquid. We find that dynamical spin correlations show peculiar temperature and frequency dependence even below the temperature where static correlations saturate. The results provide the experimentally accessible symptoms of the fluctuating fractionalized spins evincing the quantum spin liquids.

  4. Dynamic Load Balancing of Parallel Monte Carlo Transport Calculations

    SciTech Connect

    O'Brien, M; Taylor, J; Procassini, R

    2004-12-22

    The performance of parallel Monte Carlo transport calculations which use both spatial and particle parallelism is increased by dynamically assigning processors to the most worked domains. Since the particle work load varies over the course of the simulation, this algorithm determines each cycle if dynamic load balancing would speed up the calculation. If load balancing is required, a small number of particle communications are initiated in order to achieve load balance. This method has decreased the parallel run time by more than a factor of three for certain criticality calculations.

  5. Vibrational spectroscopic studies of Isoleucine by quantum chemical calculations.

    PubMed

    Moorthi, P P; Gunasekaran, S; Ramkumaar, G R

    2014-04-24

    In this work, we reported a combined experimental and theoretical study on molecular structure, vibrational spectra and NBO analysis of Isoleucine (2-Amino-3-methylpentanoic acid). The optimized molecular structure, vibrational frequencies, corresponding vibrational assignments, thermodynamics properties, NBO analyses, NMR chemical shifts and ultraviolet-visible spectral interpretation of Isoleucine have been studied by performing MP2 and DFT/cc-pVDZ level of theory. The FTIR, FT-Raman spectra were recorded in the region 4000-400 cm(-1) and 3500-50 cm(-1) respectively. The UV-visible absorption spectra of the compound were recorded in the range of 200-800 nm. Computational calculations at MP2 and B3LYP level with basis set of cc-pVDZ is employed in complete assignments of Isoleucine molecule on the basis of the potential energy distribution (PED) of the vibrational modes, calculated using VEDA-4 program. The calculated wavenumbers are compared with the experimental values. The difference between the observed and calculated wavenumber values of most of the fundamentals is very small. (13)C and (1)H nuclear magnetic resonance chemical shifts of the molecule were calculated using the gauge independent atomic orbital (GIAO) method and compared with experimental results. The formation of hydrogen bond was investigated in terms of the charge density by the NBO calculations. Based on the UV spectra and TD-DFT calculations, the electronic structure and the assignments of the absorption bands were carried out. Besides, molecular electrostatic potential (MEP) were investigated using theoretical calculations.

  6. Energetics and Dynamics of GaAs Epitaxial Growth via Quantum Wave Packet Studies

    NASA Technical Reports Server (NTRS)

    Dzegilenko, Fedor N.; Saini, Subhash (Technical Monitor)

    1998-01-01

    The dynamics of As(sub 2) molecule incorporation into the flat Ga-terminated GaAs(100) surface is studied computationally. The time-dependent Schrodinger equation is solved on a two-dimensional potential energy surface obtained using density functional theory calculations. The probabilities of trapping and subsequent dissociation of the molecular As(sub 2) bond are calculated as a function of beam translational energy and vibrational quantum number of As(sub 2).

  7. Communication: Quantum six-dimensional calculations of the coupled translation-rotation eigenstates of H2O@C60.

    PubMed

    Felker, Peter M; Bačić, Zlatko

    2016-05-28

    We report rigorous quantum calculations of the translation-rotation (TR) eigenstates of para- and ortho-H2O@C60. They provide a comprehensive description of the dynamical behavior of H2O inside the fullerene having icosahedral (Ih) symmetry. The TR eigenstates are assigned in terms of the irreducible representations of the proper symmetry group of H2O@C60, as well as the appropriate translational and rotational quantum numbers. The coupling between the orbital and the rotational angular momenta of the caged H2O gives rise to the total angular momentum λ, which additionally labels each TR level. The calculated TR levels allow tentative assignments of a number of transitions in the recent experimental INS spectra of H2O@C60 that have not been assigned previously.

  8. Quantum-classical Liouville dynamics of nonadiabatic proton transfer.

    PubMed

    Hanna, Gabriel; Kapral, Raymond

    2005-06-22

    A proton transfer reaction in a linear hydrogen-bonded complex dissolved in a polar solvent is studied using mixed quantum-classical Liouville dynamics. In this system, the proton is treated quantum mechanically and the remainder of the degrees of freedom is treated classically. The rates and mechanisms of the reaction are investigated using both adiabatic and nonadiabatic molecular dynamics. We use a nonadiabatic dynamics algorithm which allows the system to evolve on single adiabatic surfaces and on coherently coupled pairs of adiabatic surfaces. Reactive-flux correlation function expressions are used to compute the rate coefficients and the role of the dynamics on the coherently coupled surfaces is elucidated.

  9. Dynamic Quantum Tomography Model for Phase-Damping Channels

    NASA Astrophysics Data System (ADS)

    Czerwiński, Artur; Jamiołkowski, Andrzej

    In this paper we propose a dynamic quantum tomography model for open quantum systems with evolution given by phase-damping channels. Mathematically, these channels correspond to completely positive trace-preserving maps defined by the Hadamard product of the initial density matrix with a time-dependent matrix which carries the knowledge about the evolution. Physically, there is a strong motivation for considering this kind of evolution because such channels appear naturally in the theory of open quantum systems. The main idea behind a dynamic approach to quantum tomography claims that by performing the same kind of measurement at some time instants one can obtain new data for state reconstruction. Thus, this approach leads to a decrease in the number of distinct observables which are required for quantum tomography; however, the exact benefit for employing the dynamic approach depends strictly on how the quantum system evolves in time. Algebraic analysis of phase-damping channels allows one to determine criteria for quantum tomography of systems in question. General theorems and observations presented in the paper are accompanied by a specific example, which shows step by step how the theory works. The results introduced in this paper can potentially be applied in experiments where there is a tendency to look at quantum tomography from the point of view of economy of measurements, because each distinct kind of measurement requires, in general, preparing a separate setup.

  10. Quantum walk coherences on a dynamical percolation graph

    PubMed Central

    Elster, Fabian; Barkhofen, Sonja; Nitsche, Thomas; Novotný, Jaroslav; Gábris, Aurél; Jex, Igor; Silberhorn, Christine

    2015-01-01

    Coherent evolution governs the behaviour of all quantum systems, but in nature it is often subjected to influence of a classical environment. For analysing quantum transport phenomena quantum walks emerge as suitable model systems. In particular, quantum walks on percolation structures constitute an attractive platform for studying open system dynamics of random media. Here, we present an implementation of quantum walks differing from the previous experiments by achieving dynamical control of the underlying graph structure. We demonstrate the evolution of an optical time-multiplexed quantum walk over six double steps, revealing the intricate interplay between the internal and external degrees of freedom. The observation of clear non-Markovian signatures in the coin space testifies the high coherence of the implementation and the extraordinary degree of control of all system parameters. Our work is the proof-of-principle experiment of a quantum walk on a dynamical percolation graph, paving the way towards complex simulation of quantum transport in random media. PMID:26311434

  11. Non-equilibrium quantum phase transition via entanglement decoherence dynamics

    PubMed Central

    Lin, Yu-Chen; Yang, Pei-Yun; Zhang, Wei-Min

    2016-01-01

    We investigate the decoherence dynamics of continuous variable entanglement as the system-environment coupling strength varies from the weak-coupling to the strong-coupling regimes. Due to the existence of localized modes in the strong-coupling regime, the system cannot approach equilibrium with its environment, which induces a nonequilibrium quantum phase transition. We analytically solve the entanglement decoherence dynamics for an arbitrary spectral density. The nonequilibrium quantum phase transition is demonstrated as the system-environment coupling strength varies for all the Ohmic-type spectral densities. The 3-D entanglement quantum phase diagram is obtained. PMID:27713556

  12. Non-equilibrium quantum phase transition via entanglement decoherence dynamics.

    PubMed

    Lin, Yu-Chen; Yang, Pei-Yun; Zhang, Wei-Min

    2016-10-07

    We investigate the decoherence dynamics of continuous variable entanglement as the system-environment coupling strength varies from the weak-coupling to the strong-coupling regimes. Due to the existence of localized modes in the strong-coupling regime, the system cannot approach equilibrium with its environment, which induces a nonequilibrium quantum phase transition. We analytically solve the entanglement decoherence dynamics for an arbitrary spectral density. The nonequilibrium quantum phase transition is demonstrated as the system-environment coupling strength varies for all the Ohmic-type spectral densities. The 3-D entanglement quantum phase diagram is obtained.

  13. Dynamical algebra of observables in dissipative quantum systems

    NASA Astrophysics Data System (ADS)

    Alipour, Sahar; Chruściński, Dariusz; Facchi, Paolo; Marmo, Giuseppe; Pascazio, Saverio; Rezakhani, Ali T.

    2017-02-01

    Dynamics and features of quantum systems can be drastically different from classical systems. Dissipation is understood as a general mechanism through which quantum systems may lose part or all of their quantum aspects. Here we discuss a method to analyze behaviors of dissipative quantum systems in an algebraic sense. This method employs a time-dependent product between system’s observables which is induced by the underlying dissipative dynamics. We argue that the long-time limit of the algebra of observables defined with this product yields a contractive algebra which reflects the loss of some quantum features of the dissipative system, and it bears relevant information about irreversibility. We illustrate this result through several examples of dissipation in various Markovian and non-Markovian systems.

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

    SciTech Connect

    Gray, S.K.

    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.

  15. Quantum centipedes: collective dynamics of interacting quantum walkers

    NASA Astrophysics Data System (ADS)

    Krapivsky, P. L.; Luck, J. M.; Mallick, K.

    2016-08-01

    We consider the quantum centipede made of N fermionic quantum walkers on the one-dimensional lattice interacting by means of the simplest of all hard-bound constraints: the distance between two consecutive fermions is either one or two lattice spacings. This composite quantum walker spreads ballistically, just as the simple quantum walk. However, because of the interactions between the internal degrees of freedom, the distribution of its center-of-mass velocity displays numerous ballistic fronts in the long-time limit, corresponding to singularities in the empirical velocity distribution. The spectrum of the centipede and the corresponding group velocities are analyzed by direct means for the first few values of N. Some analytical results are obtained for arbitrary N by exploiting an exact mapping of the problem onto a free-fermion system. We thus derive the maximal velocity describing the ballistic spreading of the two extremal fronts of the centipede wavefunction, including its non-trivial value in the large-N limit.

  16. Frictionless quantum quenches in ultracold gases: A quantum-dynamical microscope

    SciTech Connect

    Campo, A. de

    2011-09-15

    In this Rapid Communication, a method is proposed to spatially scale up a trapped ultracold gas while conserving the quantum correlations of the initial many-body state. For systems supporting self-similar dynamics, this is achieved by implementing an engineered finite-time quench of the harmonic trap, which induces a frictionless expansion of the gas and acts as a quantum dynamical microscope.

  17. Quantum dynamics of the O + OH -> H + O2 reaction at low temperatures

    SciTech Connect

    Kendrick, Brian Kent; Quemener, Goulven; Balakrishnan, Naduvalath

    2008-01-01

    We report quantum dynamics calculations of rate coefficients for the O + OH {yields} H + O{sub 2} reaction on two potential energy surfaces (PESs) using a time-independent quantum formalism based on hyperspherical coordinates. Our calculations show that the rate coefficient remains largely constant in the temperature range 10--39 K, in agreement with the conclusions of a recent experimental study [Carty et al., J. Phys. Chem. A 110, 3101 (2006)]. This is in constrast with the quantum calculations of Xu et al. [J. Chem. Phys. 127, 024304 (2007)] which, using the same PES, predicted two orders of magnitude drop in the rate coefficient value from 39 K to 10 K. Implications of our findings to oxygen chemistry in the interstellar medium are discussed.

  18. Quantum chemical calculations for polymers and organic compounds

    NASA Technical Reports Server (NTRS)

    Lopez, J.; Yang, C.

    1982-01-01

    The relativistic effects of the orbiting electrons on a model compound were calculated. The computational method used was based on 'Modified Neglect of Differential Overlap' (MNDO). The compound tetracyanoplatinate was used since empirical measurement and calculations along "classical" lines had yielded many known properties. The purpose was to show that for large molecules relativity effects could not be ignored and that these effects could be calculated and yield data in closer agreement to empirical measurements. Both the energy band structure and molecular orbitals are depicted.

  19. Quenching a quantum critical state by the order parameter: Dynamical quantum phase transitions and quantum speed limits

    NASA Astrophysics Data System (ADS)

    Heyl, Markus

    2017-02-01

    Quantum critical states exhibit strong quantum fluctuations and are therefore highly susceptible to perturbations. In this Rapid Communication we study the dynamical stability against a sudden coupling to these strong fluctuations by quenching the order parameter of the underlying transition. Such a quench can generate superextensive energy fluctuations. This leads to a dynamical quantum phase transition (DQPT) with nonanalytic real-time behavior in the resulting decay of the initial state. By establishing a general connection between DQPTs and quantum speed limits, this allows us to obtain a quantum speed limit with unconventional system-size dependence. These findings are illustrated for the one-dimensional and the infinitely connected transverse-field Ising model. The main concepts, however, are general and can be applied also to other critical states. An outlook is given on the implications of superextensive energy fluctuations on potential restricted thermalization despite nonintegrability.

  20. Methane dissociation on Ni(111): A seven-dimensional to nine-dimensional quantum dynamics study

    NASA Astrophysics Data System (ADS)

    Shen, Xiangjian; Zhang, Zhaojun; Zhang, Dong H.

    2017-07-01

    As one benchmark system of CH4 dissociation on the Ni(111) surface, it is of great significance to explore the role of each degree of freedom (DOF) of reactant CH4 in its first C-H bond dissociation from quantum dynamics simulations. Here, the influence of the CH stretching DOF of methyl limited in C3v symmetry is quantitatively investigated as well as the important role of azimuth. We calculated the sticking probabilities, S0, of ground state (GS) CH4 dissociation on a rigid Ni(111) surface by performing some seven-dimensional to nine-dimensional (9D) quantum dynamics simulations based on one highly accurate and fifteen-dimensional (15D) ab initio potential energy surface which we recently developed. Our direct quantum dynamics results show that S0 of GS CH4 on four given surface impact sites are weakly enhanced by adding the CH stretching DOF of methyl but strongly weakened by the DOF of azimuth. Furthermore, using a 9D quantum dynamics model, we improve the post-treatment model for treating the influence of surface impact sites through a linear relationship between the effective potential barriers and the distances relative to that on the transition state site. These developed high-dimensional quantum dynamics models and improved post-treatments can be usefully extended for studying some complex polyatomic gas-surface reactions by other theoretical groups.

  1. Methane dissociation on Ni(111): A seven-dimensional to nine-dimensional quantum dynamics study.

    PubMed

    Shen, Xiangjian; Zhang, Zhaojun; Zhang, Dong H

    2017-07-14

    As one benchmark system of CH4 dissociation on the Ni(111) surface, it is of great significance to explore the role of each degree of freedom (DOF) of reactant CH4 in its first C-H bond dissociation from quantum dynamics simulations. Here, the influence of the CH stretching DOF of methyl limited in C3v symmetry is quantitatively investigated as well as the important role of azimuth. We calculated the sticking probabilities, S0, of ground state (GS) CH4 dissociation on a rigid Ni(111) surface by performing some seven-dimensional to nine-dimensional (9D) quantum dynamics simulations based on one highly accurate and fifteen-dimensional (15D) ab initio potential energy surface which we recently developed. Our direct quantum dynamics results show that S0 of GS CH4 on four given surface impact sites are weakly enhanced by adding the CH stretching DOF of methyl but strongly weakened by the DOF of azimuth. Furthermore, using a 9D quantum dynamics model, we improve the post-treatment model for treating the influence of surface impact sites through a linear relationship between the effective potential barriers and the distances relative to that on the transition state site. These developed high-dimensional quantum dynamics models and improved post-treatments can be usefully extended for studying some complex polyatomic gas-surface reactions by other theoretical groups.

  2. Ergodic dynamics and thermalization in an isolated quantum system

    NASA Astrophysics Data System (ADS)

    Neill, C.; Roushan, P.; Fang, M.; Chen, Y.; Kolodrubetz, M.; Chen, Z.; Megrant, A.; Barends, R.; Campbell, B.; Chiaro, B.; Dunsworth, A.; Jeffrey, E.; Kelly, J.; Mutus, J.; O'Malley, P. J. J.; Quintana, C.; Sank, D.; Vainsencher, A.; Wenner, J.; White, T. C.; Polkovnikov, A.; Martinis, J. M.

    2016-11-01

    Statistical mechanics is founded on the assumption that all accessible configurations of a system are equally likely. This requires dynamics that explore all states over time, known as ergodic dynamics. In isolated quantum systems, however, the occurrence of ergodic behaviour has remained an outstanding question. Here, we demonstrate ergodic dynamics in a small quantum system consisting of only three superconducting qubits. The qubits undergo a sequence of rotations and interactions and we measure the evolution of the density matrix. Maps of the entanglement entropy show that the full system can act like a reservoir for individual qubits, increasing their entropy through entanglement. Surprisingly, these maps bear a strong resemblance to the phase space dynamics in the classical limit; classically, chaotic motion coincides with higher entanglement entropy. We further show that in regions of high entropy the full multi-qubit system undergoes ergodic dynamics. Our work illustrates how controllable quantum systems can investigate fundamental questions in non-equilibrium thermodynamics.

  3. Principles and Dynamics of Quantum Mechanics

    NASA Astrophysics Data System (ADS)

    Efthimiades, Spyros

    2009-05-01

    Quantum mechanics can be founded on three principles: particle waves, concurrent states and averaged energy relations. The Schrodinger, time-evolution and Dirac equations are derived to be the conditions the wavefunction must satisfy in order to fulfill the corresponding averaged energy relations. Adopting a particle and wave balanced approach we attain a clear, consistent and justified quantum theory.

  4. Confidence and efficiency scaling in variational quantum Monte Carlo calculations

    NASA Astrophysics Data System (ADS)

    Delyon, F.; Bernu, B.; Holzmann, Markus

    2017-02-01

    Based on the central limit theorem, we discuss the problem of evaluation of the statistical error of Monte Carlo calculations using a time-discretized diffusion process. We present a robust and practical method to determine the effective variance of general observables and show how to verify the equilibrium hypothesis by the Kolmogorov-Smirnov test. We then derive scaling laws of the efficiency illustrated by variational Monte Carlo calculations on the two-dimensional electron gas.

  5. Hybrid approach for including electronic and nuclear quantum effects in molecular dynamics simulations of hydrogen transfer reactions in enzymes

    NASA Astrophysics Data System (ADS)

    Billeter, Salomon R.; Webb, Simon P.; Iordanov, Tzvetelin; Agarwal, Pratul K.; Hammes-Schiffer, Sharon

    2001-04-01

    A hybrid approach for simulating proton and hydride transfer reactions in enzymes is presented. The electronic quantum effects are incorporated with an empirical valence bond approach. The nuclear quantum effects of the transferring hydrogen are included with a mixed quantum/classical molecular dynamics method in which the hydrogen nucleus is described as a multidimensional vibrational wave function. The free energy profiles are obtained as functions of a collective reaction coordinate. A perturbation formula is derived to incorporate the vibrationally adiabatic nuclear quantum effects into the free energy profiles. The dynamical effects are studied with the molecular dynamics with quantum transitions (MDQT) surface hopping method, which incorporates nonadiabatic transitions among the adiabatic hydrogen vibrational states. The MDQT method is combined with a reactive flux approach to calculate the transmission coefficient and to investigate the real-time dynamics of reactive trajectories. This hybrid approach includes nuclear quantum effects such as zero point energy, hydrogen tunneling, and excited vibrational states, as well as the dynamics of the complete enzyme and solvent. The nuclear quantum effects are incorporated during the generation of the free energy profiles and dynamical trajectories rather than subsequently added as corrections. Moreover, this methodology provides detailed mechanistic information at the molecular level and allows the calculation of rates and kinetic isotope effects. An initial application of this approach to the enzyme liver alcohol dehydrogenase is also presented.

  6. Nonlinear dynamics and quantum entanglement in optomechanical systems.

    PubMed

    Wang, Guanglei; Huang, Liang; Lai, Ying-Cheng; Grebogi, Celso

    2014-03-21

    To search for and exploit quantum manifestations of classical nonlinear dynamics is one of the most fundamental problems in physics. Using optomechanical systems as a paradigm, we address this problem from the perspective of quantum entanglement. We uncover strong fingerprints in the quantum entanglement of two common types of classical nonlinear dynamical behaviors: periodic oscillations and quasiperiodic motion. There is a transition from the former to the latter as an experimentally adjustable parameter is changed through a critical value. Accompanying this process, except for a small region about the critical value, the degree of quantum entanglement shows a trend of continuous increase. The time evolution of the entanglement measure, e.g., logarithmic negativity, exhibits a strong dependence on the nature of classical nonlinear dynamics, constituting its signature.

  7. The classical and quantum dynamics of molecular spins on graphene

    NASA Astrophysics Data System (ADS)

    Cervetti, Christian; Rettori, Angelo; Pini, Maria Gloria; Cornia, Andrea; Repollés, Ana; Luis, Fernando; Dressel, Martin; Rauschenbach, Stephan; Kern, Klaus; Burghard, Marko; Bogani, Lapo

    2016-02-01

    Controlling the dynamics of spins on surfaces is pivotal to the design of spintronic and quantum computing devices. Proposed schemes involve the interaction of spins with graphene to enable surface-state spintronics and electrical spin manipulation. However, the influence of the graphene environment on the spin systems has yet to be unravelled. Here we explore the spin-graphene interaction by studying the classical and quantum dynamics of molecular magnets on graphene. Whereas the static spin response remains unaltered, the quantum spin dynamics and associated selection rules are profoundly modulated. The couplings to graphene phonons, to other spins, and to Dirac fermions are quantified using a newly developed model. Coupling to Dirac electrons introduces a dominant quantum relaxation channel that, by driving the spins over Villain’s threshold, gives rise to fully coherent, resonant spin tunnelling. Our findings provide fundamental insight into the interaction between spins and graphene, establishing the basis for electrical spin manipulation in graphene nanodevices.

  8. Communication: Relation of centroid molecular dynamics and ring-polymer molecular dynamics to exact quantum dynamics

    SciTech Connect

    Hele, Timothy J. H.; Willatt, Michael J.; Muolo, Andrea; Althorpe, Stuart C.

    2015-05-21

    We recently obtained a quantum-Boltzmann-conserving classical dynamics by making a single change to the derivation of the “Classical Wigner” approximation. Here, we show that the further approximation of this “Matsubara dynamics” gives rise to two popular heuristic methods for treating quantum Boltzmann time-correlation functions: centroid molecular dynamics (CMD) and ring-polymer molecular dynamics (RPMD). We show that CMD is a mean-field approximation to Matsubara dynamics, obtained by discarding (classical) fluctuations around the centroid, and that RPMD is the result of discarding a term in the Matsubara Liouvillian which shifts the frequencies of these fluctuations. These findings are consistent with previous numerical results and give explicit formulae for the terms that CMD and RPMD leave out.

  9. Quantum charge transport and conformational dynamics of macromolecules.

    PubMed

    Boninsegna, L; Faccioli, P

    2012-06-07

    We study the dynamics of quantum excitations inside macromolecules which can undergo conformational transitions. In the first part of the paper, we use the path integral formalism to rigorously derive a set of coupled equations of motion which simultaneously describe the molecular and quantum transport dynamics, and obey the fluctuation/dissipation relationship. We also introduce an algorithm which yields the most probable molecular and quantum transport pathways in rare, thermally activated reactions. In the second part of the paper, we apply this formalism to simulate the propagation of a quantum charge during the collapse of a polymer from an initial stretched conformation to a final globular state. We find that the charge dynamics is quenched when the chain reaches a molten globule state. Using random matrix theory we show that this transition is due to an increase of quantum localization driven by dynamical disorder. We argue that collapsing conducting polymers may represent a physical realization of quantum small-world networks with dynamical rewiring probability.

  10. Quantum dynamics of the avian compass

    NASA Astrophysics Data System (ADS)

    Walters, Zachary B.

    2014-10-01

    The ability of migratory birds to orient relative to the Earth's magnetic field is believed to involve a coherent superposition of two spin states of a radical electron pair. However, the mechanism by which this coherence can be maintained in the face of strong interactions with the cellular environment has remained unclear. This paper addresses the problem of decoherence between two electron spins due to hyperfine interaction with a bath of spin-1/2 nuclei. Dynamics of the radical pair density matrix are derived and shown to yield a simple mechanism for sensing magnetic field orientation. Rates of dephasing and decoherence are calculated ab initio and found to yield millisecond coherence times, consistent with behavioral experiments.

  11. Quantum grow--A quantum dynamics sampling approach for growing potential energy surfaces and nonadiabatic couplings

    SciTech Connect

    Godsi, Oded; Peskin, Uri; Collins, Michael A.

    2010-03-28

    A quantum sampling algorithm for the interpolation of diabatic potential energy matrices by the Grow method is introduced. The new procedure benefits from penetration of the wave packet into classically forbidden regions, and the accurate quantum mechanical description of nonadiabatic transitions. The increased complexity associated with running quantum dynamics is reduced by using approximate low order expansions of the nuclear wave function within a Multi-configuration time-dependent Hartree scheme during the Grow process. The sampling algorithm is formulated and applied for three representative test cases, demonstrating the recovery of analytic potentials by the interpolated ones, and the convergence of a dynamic observable.

  12. Nuclear-magnetic-resonance quantum calculations of the Jones polynomial

    PubMed Central

    Marx, Raimund; Fahmy, Amr; Kauffman, Louis; Lomonaco, Samuel; Spörl, Andreas; Pomplun, Nikolas; Schulte-Herbrüggen, Thomas; Myers, John M.; Glaser, Steffen J.

    2011-01-01

    The repertoire of problems theoretically solvable by a quantum computer recently expanded to include the approximate evaluation of knot invariants, specifically the Jones polynomial. The experimental implementation of this evaluation, however, involves many known experimental challenges. Here we present experimental results for small-scale approximate evaluation of the Jones polynomial by nuclear magnetic resonance (NMR); in addition, we show how to escape from the limitations of NMR approaches that employ pseudopure states. Specifically, we use two spin-1/2 nuclei of natural abundance chloroform and apply a sequence of unitary transforms representing the trefoil knot, the figure-eight knot, and the Borromean rings. After measuring the nuclear spin state of the molecule in each case, we are able to estimate the value of the Jones polynomial for each of the knots. PMID:21461143

  13. Efficient algorithms for large-scale quantum transport calculations

    NASA Astrophysics Data System (ADS)

    Brück, Sascha; Calderara, Mauro; Bani-Hashemian, Mohammad Hossein; VandeVondele, Joost; Luisier, Mathieu

    2017-08-01

    Massively parallel algorithms are presented in this paper to reduce the computational burden associated with quantum transport simulations from first-principles. The power of modern hybrid computer architectures is harvested in order to determine the open boundary conditions that connect the simulation domain with its environment and to solve the resulting Schrödinger equation. While the former operation takes the form of an eigenvalue problem that is solved by a contour integration technique on the available central processing units (CPUs), the latter can be cast into a linear system of equations that is simultaneously processed by SplitSolve, a two-step algorithm, on general-purpose graphics processing units (GPUs). A significant decrease of the computational time by up to two orders of magnitude is obtained as compared to standard solution methods.

  14. Linear scaling calculation of an n-type GaAs quantum dot.

    PubMed

    Nomura, Shintaro; Iitaka, Toshiaki

    2007-09-01

    A linear scale method for calculating electronic properties of large and complex systems is introduced within a local density approximation. The method is based on the Chebyshev polynomial expansion and the time-dependent method, which is tested on the calculation of the electronic structure of a model n-type GaAs quantum dot.

  15. Quantum Information Biology: From Theory of Open Quantum Systems to Adaptive Dynamics

    NASA Astrophysics Data System (ADS)

    Asano, Masanari; Basieva, Irina; Khrennikov, Andrei; Ohya, Masanori; Tanaka, Yoshiharu; Yamato, Ichiro

    This chapter reviews quantum(-like) information biology (QIB). Here biology is treated widely as even covering cognition and its derivatives: psychology and decision making, sociology, and behavioral economics and finances. QIB provides an integrative description of information processing by bio-systems at all scales of life: from proteins and cells to cognition, ecological and social systems. Mathematically QIB is based on the theory of adaptive quantum systems (which covers also open quantum systems). Ideologically QIB is based on the quantum-like (QL) paradigm: complex bio-systems process information in accordance with the laws of quantum information and probability. This paradigm is supported by plenty of statistical bio-data collected at all bio-scales. QIB re ects the two fundamental principles: a) adaptivity; and, b) openness (bio-systems are fundamentally open). In addition, quantum adaptive dynamics provides the most generally possible mathematical representation of these principles.

  16. Quantum Langevin approach for non-Markovian quantum dynamics of the spin-boson model

    NASA Astrophysics Data System (ADS)

    Zhou, Zheng-Yang; Chen, Mi; Yu, Ting; You, J. Q.

    2016-02-01

    One longstanding difficult problem in quantum dissipative dynamics is to solve the spin-boson model in a non-Markovian regime where a tractable systematic master equation does not exist. The spin-boson model is particularly important due to its crucial applications in quantum noise control and manipulation as well as its central role in developing quantum theories of open systems. Here we solve this important model by developing a non-Markovian quantum Langevin approach. By projecting the quantum Langevin equation onto the coherent states of the bath, we can derive a set of non-Markovian quantum Bloch equations containing no explicit noise variables. This special feature offers a tremendous advantage over the existing stochastic Schrödinger equations in numerical simulations. The physical significance and generality of our approach are briefly discussed.

  17. Fokker-Planck quantum master equation for mixed quantum-semiclassical dynamics.

    PubMed

    Ding, Jin-Jin; Wang, Yao; Zhang, Hou-Dao; Xu, Rui-Xue; Zheng, Xiao; Yan, YiJing

    2017-01-14

    We revisit Caldeira-Leggett's quantum master equation representing mixed quantum-classical theory, but with limited applications. Proposed is a Fokker-Planck quantum master equation theory, with a generic bi-exponential correlation function description on semiclassical Brownian oscillators' environments. The new theory has caustic terms that bridge between the quantum description on primary systems and the semiclassical or quasi-classical description on environments. Various parametrization schemes, both analytical and numerical, for the generic bi-exponential environment bath correlation functions are proposed and scrutinized. The Fokker-Planck quantum master equation theory is of the same numerical cost as the original Caldeira-Leggett's approach but acquires a significantly broadened validity and accuracy range, as illustrated against the exact dynamics on model systems in quantum Brownian oscillators' environments, at moderately low temperatures.

  18. Quantum Monte Carlo calculations of two neutrons in finite volume

    SciTech Connect

    Klos, P.; Lynn, J. E.; Tews, I.; Gandolfi, Stefano; Gezerlis, A.; Hammer, H. -W.; Hoferichter, M.; Schwenk, A.

    2016-11-18

    Ab initio calculations provide direct access to the properties of pure neutron systems that are challenging to study experimentally. In addition to their importance for fundamental physics, their properties are required as input for effective field theories of the strong interaction. In this work, we perform auxiliary-field diffusion Monte Carlo calculations of the ground state and first excited state of two neutrons in a finite box, considering a simple contact potential as well as chiral effective field theory interactions. We compare the results against exact diagonalizations and present a detailed analysis of the finite-volume effects, whose understanding is crucial for determining observables from the calculated energies. Finally, using the Lüscher formula, we extract the low-energy S-wave scattering parameters from ground- and excited-state energies for different box sizes.

  19. Quantum Monte Carlo calculations of two neutrons in finite volume

    DOE PAGES

    Klos, P.; Lynn, J. E.; Tews, I.; ...

    2016-11-18

    Ab initio calculations provide direct access to the properties of pure neutron systems that are challenging to study experimentally. In addition to their importance for fundamental physics, their properties are required as input for effective field theories of the strong interaction. In this work, we perform auxiliary-field diffusion Monte Carlo calculations of the ground state and first excited state of two neutrons in a finite box, considering a simple contact potential as well as chiral effective field theory interactions. We compare the results against exact diagonalizations and present a detailed analysis of the finite-volume effects, whose understanding is crucial formore » determining observables from the calculated energies. Finally, using the Lüscher formula, we extract the low-energy S-wave scattering parameters from ground- and excited-state energies for different box sizes.« less

  20. Lectures on dynamical models for quantum measurements

    NASA Astrophysics Data System (ADS)

    Nieuwenhuizen, Theo M.; Perarnau-Llobet, Marti; Balian, Roger

    2014-06-01

    In textbooks, ideal quantum measurements are described in terms of the tested system only by the collapse postulate and Born's rule. This level of description offers a rather flexible position for the interpretation of quantum mechanics. Here we analyse an ideal measurement as a process of interaction between the tested system S and an apparatus A, so as to derive the properties postulated in textbooks. We thus consider within standard quantum mechanics the measurement of a quantum spin component ŝz by an apparatus A, being a magnet coupled to a bath. We first consider the evolution of the density operator of S + A describing a large set of runs of the measurement process. The approach describes the disappearance of the off-diagonal terms ("truncation") of the density matrix as a physical effect due to A, while the registration of the outcome has classical features due to the large size of the pointer variable, the magnetization. A quantum ambiguity implies that the density matrix at the final time can be decomposed on many bases, not only the one of the measurement. This quantum oddity prevents to connect individual outcomes to measurements, a difficulty known as the "measurement problem". It is shown that it is circumvented by the apparatus as well, since the evolution in a small time interval erases all decompositions, except the one on the measurement basis. Once one can derive the outcome of individual events from quantum theory, the so-called collapse of the wavefunction or the reduction of the state appears as the result of a selection of runs among the original large set. Hence nothing more than standard quantum mechanics is needed to explain features of measurements. The employed statistical formulation is advocated for the teaching of quantum theory.

  1. Lectures on Dynamical Models for Quantum Measurements

    NASA Astrophysics Data System (ADS)

    Nieuwenhuizen, Theo M.; Perarnau-Llobet, Martí Balian, Roger

    2015-10-01

    In textbooks, ideal quantum measurements are described in terms of the tested system only by the collapse postulate and Born's rule. This level of description offers a rather flexible position for the interpretation of quantum mechanics. Here we analyse an ideal measurement as a process of interaction between the tested system S and an apparatus A, so as to derive the properties postulated in textbooks. We thus consider within standard quantum mechanics the measurement of a quantum spin component ŝz by an apparatus A, being a magnet coupled to a bath. We first consider the evolution of the density operator of S+A describing a large set of runs of the measurement process. The approach describes the disappearance of the off-diagonal terms ("truncation") of the density matrix as a physical effect due to A, while the registration of the outcome has classical features due to the large size of the pointer variable, the magnetisation. A quantum ambiguity implies that the density matrix at the final time can be decomposed on many bases, not only the one of the measurement. This quantum oddity prevents to connect individual outcomes to measurements, a difficulty known as the "measurement problem". It is shown that it is circumvented by the apparatus as well, since the evolution in a small time interval erases all decompositions, except the one on the measurement basis. Once one can derive the outcome of individual events from quantum theory, the so-called "collapse of the wave function" or the "reduction of the state" appears as the result of a selection of runs among the original large set. Hence nothing more than standard quantum mechanics is needed to explain features of measurements. The employed statistical formulation is advocated for the teaching of quantum theory.

  2. Progesterone and testosterone studies by neutron-scattering methods and quantum chemistry calculations

    NASA Astrophysics Data System (ADS)

    Holderna-Natkaniec, K.; Szyczewski, A.; Natkaniec, I.; Khavryutchenko, V. D.; Pawlukojc, A.

    Inelastic incoherent neutron scattering (IINS) and neutron diffraction spectra of progesterone and testosterone were measured simultaneously on the NERA spectrometer at the IBR-2 pulsed reactor in Dubna. Both studied samples do not indicate any phase transition in the temperature range from 20 to 290K. The IINS spectra have been transformed to the phonon density of states (PDS) in the one-phonon scattering approximation. The PDS spectra display well-resolved peaks of low-frequency internal vibration modes up to 600cm-1. The assignment of these modes was proposed taking into account the results of calculations of the structure and dynamics of isolated molecules of the investigated substances. The quantum chemistry calculations were performed by the semi-empirical PM3 method and at the restricted Hartree-Fock level with the 6-31* basis set. The lower internal modes assigned to torsional vibration of the androstane skeleton mix with the lattice vibrations. The intense bands in the PDS spectra in the frequency range from 150 to 300cm-1 are related to librations of structurally inequivalent methyl groups.

  3. A molecular dynamics study of nuclear quantum effect on diffusivity of hydrogen molecule

    NASA Astrophysics Data System (ADS)

    Nagashima, H.; Tsuda, S.; Tsuboi, N.; Hayashi, A. K.; Tokumasu, T.

    2017-07-01

    In this paper, the nuclear quantum effect of the hydrogen molecule on its diffusivity was analyzed using the molecular dynamics (MD) method. The centroid MD (CMD) method was applied to reproduce the time evolution of the molecules. The diffusion coefficient of hydrogen was calculated using the Green-Kubo method over a wide temperature region, and the temperature dependence of the quantum effect of the hydrogen molecule on its diffusivity was addressed. The calculated results were compared with classical MD results based on the principle of corresponding state (PCS). It was confirmed that the difference in the diffusion coefficient calculated in the CMD and classical MD methods was small, and the PCS appears to be satisfied on the temperature dependence of the diffusion coefficient, even though the quantum effect of the hydrogen molecules was taken into account. It was clarified that this result did not suggest that the quantum effect on the diffusivity of the hydrogen molecule was small but that the two changes in the intermolecular interaction of hydrogen due to the quantum effect offset each other. Moreover, it was found that this tendency was related to the temperature dependence of the ratio of the kinetic energy of the quantum fluctuational motion to the classical kinetic energy.

  4. Fractional quantum mechanics on networks: Long-range dynamics and quantum transport.

    PubMed

    Riascos, A P; Mateos, José L

    2015-11-01

    In this paper we study the quantum transport on networks with a temporal evolution governed by the fractional Schrödinger equation. We generalize the dynamics based on continuous-time quantum walks, with transitions to nearest neighbors on the network, to the fractional case that allows long-range displacements. By using the fractional Laplacian matrix of a network, we establish a formalism that combines a long-range dynamics with the quantum superposition of states; this general approach applies to any type of connected undirected networks, including regular, random, and complex networks, and can be implemented from the spectral properties of the Laplacian matrix. We study the fractional dynamics and its capacity to explore the network by means of the transition probability, the average probability of return, and global quantities that characterize the efficiency of this quantum process. As a particular case, we explore analytically these quantities for circulant networks such as rings, interacting cycles, and complete graphs.

  5. Fractional quantum mechanics on networks: Long-range dynamics and quantum transport

    NASA Astrophysics Data System (ADS)

    Riascos, A. P.; Mateos, José L.

    2015-11-01

    In this paper we study the quantum transport on networks with a temporal evolution governed by the fractional Schrödinger equation. We generalize the dynamics based on continuous-time quantum walks, with transitions to nearest neighbors on the network, to the fractional case that allows long-range displacements. By using the fractional Laplacian matrix of a network, we establish a formalism that combines a long-range dynamics with the quantum superposition of states; this general approach applies to any type of connected undirected networks, including regular, random, and complex networks, and can be implemented from the spectral properties of the Laplacian matrix. We study the fractional dynamics and its capacity to explore the network by means of the transition probability, the average probability of return, and global quantities that characterize the efficiency of this quantum process. As a particular case, we explore analytically these quantities for circulant networks such as rings, interacting cycles, and complete graphs.

  6. The quantum dynamics of electronically nonadiabatic chemical reactions

    NASA Technical Reports Server (NTRS)

    Truhlar, Donald G.

    1993-01-01

    Considerable progress was achieved on the quantum mechanical treatment of electronically nonadiabatic collisions involving energy transfer and chemical reaction in the collision of an electronically excited atom with a molecule. In the first step, a new diabatic representation for the coupled potential energy surfaces was created. A two-state diabatic representation was developed which was designed to realistically reproduce the two lowest adiabatic states of the valence bond model and also to have the following three desirable features: (1) it is more economical to evaluate; (2) it is more portable; and (3) all spline fits are replaced by analytic functions. The new representation consists of a set of two coupled diabatic potential energy surfaces plus a coupling surface. It is suitable for dynamics calculations on both the electronic quenching and reaction processes in collisions of Na(3p2p) with H2. The new two-state representation was obtained by a three-step process from a modified eight-state diatomics-in-molecules (DIM) representation of Blais. The second step required the development of new dynamical methods. A formalism was developed for treating reactions with very general basis functions including electronically excited states. Our formalism is based on the generalized Newton, scattered wave, and outgoing wave variational principles that were used previously for reactive collisions on a single potential energy surface, and it incorporates three new features: (1) the basis functions include electronic degrees of freedom, as required to treat reactions involving electronic excitation and two or more coupled potential energy surfaces; (2) the primitive electronic basis is assumed to be diabatic, and it is not assumed that it diagonalizes the electronic Hamiltonian even asymptotically; and (3) contracted basis functions for vibrational-rotational-orbital degrees of freedom are included in a very general way, similar to previous prescriptions for locally

  7. Quantum-like model of unconscious–conscious dynamics

    PubMed Central

    Khrennikov, Andrei

    2015-01-01

    We present a quantum-like model of sensation–perception dynamics (originated in Helmholtz theory of unconscious inference) based on the theory of quantum apparatuses and instruments. We illustrate our approach with the model of bistable perception of a particular ambiguous figure, the Schröder stair. This is a concrete model for unconscious and conscious processing of information and their interaction. The starting point of our quantum-like journey was the observation that perception dynamics is essentially contextual which implies impossibility of (straightforward) embedding of experimental statistical data in the classical (Kolmogorov, 1933) framework of probability theory. This motivates application of nonclassical probabilistic schemes. And the quantum formalism provides a variety of the well-approved and mathematically elegant probabilistic schemes to handle results of measurements. The theory of quantum apparatuses and instruments is the most general quantum scheme describing measurements and it is natural to explore it to model the sensation–perception dynamics. In particular, this theory provides the scheme of indirect quantum measurements which we apply to model unconscious inference leading to transition from sensations to perceptions. PMID:26283979

  8. Quantum-like model of unconscious-conscious dynamics.

    PubMed

    Khrennikov, Andrei

    2015-01-01

    We present a quantum-like model of sensation-perception dynamics (originated in Helmholtz theory of unconscious inference) based on the theory of quantum apparatuses and instruments. We illustrate our approach with the model of bistable perception of a particular ambiguous figure, the Schröder stair. This is a concrete model for unconscious and conscious processing of information and their interaction. The starting point of our quantum-like journey was the observation that perception dynamics is essentially contextual which implies impossibility of (straightforward) embedding of experimental statistical data in the classical (Kolmogorov, 1933) framework of probability theory. This motivates application of nonclassical probabilistic schemes. And the quantum formalism provides a variety of the well-approved and mathematically elegant probabilistic schemes to handle results of measurements. The theory of quantum apparatuses and instruments is the most general quantum scheme describing measurements and it is natural to explore it to model the sensation-perception dynamics. In particular, this theory provides the scheme of indirect quantum measurements which we apply to model unconscious inference leading to transition from sensations to perceptions.

  9. Mixed quantum-classical Liouville molecular dynamics without momentum jump

    NASA Astrophysics Data System (ADS)

    Ando, Koji; Santer, Mark

    2003-06-01

    An alternative Liouville formulation of mixed quantum-classical dynamics outlined recently [K. Ando, Chem. Phys. Lett. 360, 240 (2002)] is expanded in detail by taking an explicit account of the parametric dependence of the electronic (adiabatic) basis on the nuclear coordinates. As a consequence of the different operational order of the partial Wigner transformation for the nuclear coordinates and the calculation of the matrix elements in the adiabatic electronic basis, the present formula differs from the previously proposed one, slightly in the appearance but significantly in the treatment of nonadiabatic transitions in the trajectory implementation in that the former does not contain the "off-diagonal Hellmann-Feynman forces" representing the so-called "momentum-jump" associated with the nonadiabatic transitions. Because of this, the present formula is free from the numerical instability intrinsically coming from the momentum-jump operation at around the classical turning points of the nuclear motion. It is also shown that the density matrices from the two approaches coincide when the electronic basis is independent of the nuclear coordinates (R), and hence the momentum-jump approximation stems from the R-dependence of the adiabatic electronic basis. Improved stability and comparable to better reproduction of the quantum reference calculations are demonstrated by applications to one and three dimensional spin-boson models and a two-state three-mode model of the S2→S1 internal conversion of pyrazine. Also discussed is the importance of electronic coherence for the proper treatment of nonadiabatic transition rates which is naturally described by the Liouville methods compared to the conventional independent trajectory approaches.

  10. Quantum Calculations on Salt Bridges with Water: Potentials, Structure, and Properties

    SciTech Connect

    Liao, Sing; Green, Michael E.

    2011-01-01

    Salt bridges are electrostatic links between acidic and basic amino acids in a protein; quantum calculations are used here to determine the energetics and other properties of one form of these species, in the presence of water molecules. The acidic groups are carboxylic acids (aspartic and glutamic acids); proteins have two bases with pK above physiological pH: one, arginine, with a guanidinium basic group, the other lysine, which is a primary amine. Only arginine is modeled here, by ethyl guanidinium, while propionic acid is used as a model for either carboxylic acid. The salt bridges are accompanied by 0-12 water molecules; for each of the 13 systems, the energy-bond distance relation, natural bond orbitals (NBO), frequency calculations allowing thermodynamic corrections to room temperature, and dielectric constant dependence, were all calculated. The water molecules were found to arrange themselves in hydrogen bonded rings anchored to the oxygens of the salt bridge components. This was not surprising in itself, but it was found that the rings lead to a periodicity in the energy, and to a 'water addition' rule. The latter shows that the initial rings, with four oxygen atoms, become five member rings when an additional water molecule becomes available, with the additional water filling in at the bond with the lowest Wiberg index, as calculated using NBO. The dielectric constant dependence is the expected hyperbola, and the fit of the energy to the inverse dielectric constant is determined. There is an energy periodicity related to ring formation upon addition of water molecules. When 10 water molecules have been added, all spaces near the salt bridge are filled, completing the first hydration shell, and a second shell starts to form. The potentials associated with salt bridges depend on their hydration, and potentials assigned without regard to local hydration are likely to cause errors as large as or larger than kBT, thus suggesting a serious problem if these

  11. Symmetry-projected wave functions in quantum Monte Carlo calculations

    NASA Astrophysics Data System (ADS)

    Shi, Hao; Jiménez-Hoyos, Carlos A.; Rodríguez-Guzmán, R.; Scuseria, Gustavo E.; Zhang, Shiwei

    2014-03-01

    We consider symmetry-projected Hartree-Fock trial wave functions in constrained-path Monte Carlo (CPMC) calculations. Previous CPMC calculations have mostly employed Hartree-Fock (HF) trial wave functions, restricted or unrestricted. The symmetry-projected HF approach results in a hierarchy of wave functions with increasing quality: the more symmetries that are broken and restored in a self-consistent manner, the higher the quality of the trial wave function. This hierarchy is approximately maintained in CPMC calculations: the accuracy in the energy increases and the statistical variance decreases when further symmetries are broken and restored. Significant improvement is achieved in CPMC with the best symmetry-projected trial wave functions over those from simple HF. We analyze and quantify the behavior using the two-dimensional repulsive Hubbard model as an example. In the sign-problem-free region, where CPMC can be made exact but a constraint is deliberately imposed here, spin-projected wave functions remove the constraint bias. Away from half filling, spatial symmetry restoration in addition to that of the spin leads to highly accurate results from CPMC. Since the computational cost of symmetry-projected HF trial wave functions in CPMC can be made to scale algebraically with system size, this provides a potentially general approach for accurate calculations in many-fermion systems.

  12. Investigating non-Markovian dynamics of quantum open systems

    NASA Astrophysics Data System (ADS)

    Chen, Yusui

    Quantum open system coupled to a non-Markovian environment has recently attracted widespread interest for its important applications in quantum information processing and quantum dissipative systems. New phenomena induced by the non-Markovian environment have been discovered in variety of research areas ranging from quantum optics, quantum decoherence to condensed matter physics. However, the study of the non-Markovian quantum open system is known a difficult problem due to its technical complexity in deriving the fundamental equation of motion and elusive conceptual issues involving non-equilibrium dynamics for a strong coupled environment. The main purpose of this thesis is to introduce several new techniques of solving the quantum open systems including a systematic approach to dealing with non-Markovian master equations from a generic quantum-state diffusion (QSD) equation. In the first part of this thesis, we briefly introduce the non-Markovian quantum-state diffusion approach, and illustrate some pronounced non-Markovian quantum effects through numerical investigation on a cavity-QED model. Then we extend the non-Markovian QSD theory to an interesting model where the environment has a hierarchical structure, and find out the exact non-Markovian QSD equation of this model system. We observe the generation of quantum entanglement due to the interplay between the non-Markovian environment and the cavity. In the second part, we show an innovative method to obtain the exact non-Markovian master equations for a set of generic quantum open systems based on the corresponding non-Markovian QSD equations. Multiple-qubit systems and multilevel systems are discussed in details as two typical examples. Particularly, we derive the exact master equation for a model consisting of a three-level atom coupled to an optical cavity and controlled by an external laser field. Additionally, we discuss in more general context the mathematical similarity between the multiple

  13. Divisible quantum dynamics satisfies temporal Tsirelson’s bound

    NASA Astrophysics Data System (ADS)

    Le, Thao; Pollock, Felix A.; Paterek, Tomasz; Paternostro, Mauro; Modi, Kavan

    2017-02-01

    We give strong evidence that divisibility of qubit quantum processes implies temporal Tsirelson’s bound. We also give strong evidence that the classical bound of the temporal Bell’s inequality holds for dynamics that can be described by entanglement-breaking channels—a more general class of dynamics than that allowed by classical physics.

  14. Mixed quantum classical calculation of proton transfer reaction rates: From deep tunneling to over the barrier regimes

    SciTech Connect

    Xie, Weiwei; Xu, Yang; Zhu, Lili; Shi, Qiang

    2014-05-07

    We present mixed quantum classical calculations of the proton transfer (PT) reaction rates represented by a double well system coupled to a dissipative bath. The rate constants are calculated within the so called nontraditional view of the PT reaction, where the proton motion is quantized and the solvent polarization is used as the reaction coordinate. Quantization of the proton degree of freedom results in a problem of non-adiabatic dynamics. By employing the reactive flux formulation of the rate constant, the initial sampling starts from the transition state defined using the collective reaction coordinate. Dynamics of the collective reaction coordinate is treated classically as over damped diffusive motion, for which the equation of motion can be derived using the path integral, or the mixed quantum classical Liouville equation methods. The calculated mixed quantum classical rate constants agree well with the results from the numerically exact hierarchical equation of motion approach for a broad range of model parameters. Moreover, we are able to obtain contributions from each vibrational state to the total reaction rate, which helps to understand the reaction mechanism from the deep tunneling to over the barrier regimes. The numerical results are also compared with those from existing approximate theories based on calculations of the non-adiabatic transmission coefficients. It is found that the two-surface Landau-Zener formula works well in calculating the transmission coefficients in the deep tunneling regime, where the crossing point between the two lowest vibrational states dominates the total reaction rate. When multiple vibrational levels are involved, including additional crossing points on the free energy surfaces is important to obtain the correct reaction rate using the Landau-Zener formula.

  15. Mixed quantum classical calculation of proton transfer reaction rates: from deep tunneling to over the barrier regimes.

    PubMed

    Xie, Weiwei; Xu, Yang; Zhu, Lili; Shi, Qiang

    2014-05-07

    We present mixed quantum classical calculations of the proton transfer (PT) reaction rates represented by a double well system coupled to a dissipative bath. The rate constants are calculated within the so called nontraditional view of the PT reaction, where the proton motion is quantized and the solvent polarization is used as the reaction coordinate. Quantization of the proton degree of freedom results in a problem of non-adiabatic dynamics. By employing the reactive flux formulation of the rate constant, the initial sampling starts from the transition state defined using the collective reaction coordinate. Dynamics of the collective reaction coordinate is treated classically as over damped diffusive motion, for which the equation of motion can be derived using the path integral, or the mixed quantum classical Liouville equation methods. The calculated mixed quantum classical rate constants agree well with the results from the numerically exact hierarchical equation of motion approach for a broad range of model parameters. Moreover, we are able to obtain contributions from each vibrational state to the total reaction rate, which helps to understand the reaction mechanism from the deep tunneling to over the barrier regimes. The numerical results are also compared with those from existing approximate theories based on calculations of the non-adiabatic transmission coefficients. It is found that the two-surface Landau-Zener formula works well in calculating the transmission coefficients in the deep tunneling regime, where the crossing point between the two lowest vibrational states dominates the total reaction rate. When multiple vibrational levels are involved, including additional crossing points on the free energy surfaces is important to obtain the correct reaction rate using the Landau-Zener formula.

  16. Recent Advances in Quantum Dynamics of Bimolecular Reactions

    NASA Astrophysics Data System (ADS)

    Zhang, Dong H.; Guo, Hua

    2016-05-01

    In this review, we survey the latest advances in theoretical understanding of bimolecular reaction dynamics in the past decade. The remarkable recent progress in this field has been driven by more accurate and efficient ab initio electronic structure theory, effective potential-energy surface fitting techniques, and novel quantum scattering algorithms. Quantum mechanical characterization of bimolecular reactions continues to uncover interesting dynamical phenomena in atom-diatom reactions and beyond, reaching an unprecedented level of sophistication. In tandem with experimental explorations, these theoretical developments have greatly advanced our understanding of key issues in reaction dynamics, such as microscopic reaction mechanisms, mode specificity, product energy disposal, influence of reactive resonances, and nonadiabatic effects.

  17. Advancements in dynamic kill calculations for blowout wells

    SciTech Connect

    Kouba, G.E. . Production Fluids Div.); MacDougall, G.R. ); Schumacher, B.W. . Information Technology Dept.)

    1993-09-01

    This paper addresses the development, interpretation, and use of dynamic kill equations. To this end, three simple calculation techniques are developed for determining the minimum dynamic kill rate. Two techniques contain only single-phase calculations and are independent of reservoir inflow performance. Despite these limitations, these two methods are useful for bracketing the minimum flow rates necessary to kill a blowing well. For the third technique, a simplified mechanistic multiphase-flow model is used to determine a most-probable minimum kill rate.

  18. Stochastic Approximation of Dynamical Exponent at Quantum Critical Point

    NASA Astrophysics Data System (ADS)

    Suwa, Hidemaro; Yasuda, Shinya; Todo, Synge

    We have developed a unified finite-size scaling method for quantum phase transitions that requires no prior knowledge of the dynamical exponent z. During a quantum Monte Carlo simulation, the temperature is automatically tuned by the Robbins-Monro stochastic approximation method, being proportional to the lowest gap of the finite-size system. The dynamical exponent is estimated in a straightforward way from the system-size dependence of the temperature. As a demonstration of our novel method, the two-dimensional S = 1 / 2 quantum XY model, or equivalently the hard-core boson system, in uniform and staggered magnetic fields is investigated in the combination of the world-line quantum Monte Carlo worm algorithm. In the absence of a uniform magnetic field, we obtain the fully consistent result with the Lorentz invariance at the quantum critical point, z = 1 . Under a finite uniform magnetic field, on the other hand, the dynamical exponent becomes two, and the mean-field universality with effective dimension (2+2) governs the quantum phase transition. We will discuss also the system with random magnetic fields, or the dirty boson system, bearing a non-trivial dynamical exponent.Reference: S. Yasuda, H. Suwa, and S. Todo Phys. Rev. B 92, 104411 (2015); arXiv:1506.04837

  19. Acceleration of adiabatic quantum dynamics in electromagnetic fields

    SciTech Connect

    Masuda, Shumpei; Nakamura, Katsuhiro

    2011-10-15

    We show a method to accelerate quantum adiabatic dynamics of wave functions under electromagnetic field (EMF) by developing the preceding theory [Masuda and Nakamura, Proc. R. Soc. London Ser. A 466, 1135 (2010)]. Treating the orbital dynamics of a charged particle in EMF, we derive the driving field which accelerates quantum adiabatic dynamics in order to obtain the final adiabatic states in any desired short time. The scheme is consolidated by describing a way to overcome possible singularities in both the additional phase and driving potential due to nodes proper to wave functions under EMF. As explicit examples, we exhibit the fast forward of adiabatic squeezing and transport of excited Landau states with nonzero angular momentum, obtaining the result consistent with the transitionless quantum driving applied to the orbital dynamics in EMF.

  20. Quantum correlations at infinite temperature: The dynamical Nagaoka effect

    NASA Astrophysics Data System (ADS)

    Kanász-Nagy, Márton; Lovas, Izabella; Grusdt, Fabian; Greif, Daniel; Greiner, Markus; Demler, Eugene A.

    2017-07-01

    Do quantum correlations play a role in high-temperature dynamics of many-body systems? A common expectation is that thermal fluctuations lead to fast decoherence and make dynamics classical. In this paper we provide a striking example that a single particle created in a featureless, infinite temperature spin bath not only exhibits nonclassical dynamics but it also induces strong long-lived correlations between the surrounding spins. We study the nonequilibrium dynamics of a hole created in a Mott insulator in the atomic limit, which corresponds to a degenerate spin system. In the absence of interactions, the spin correlations arise purely from quantum interference. Furthermore, these correlations are both antiferromagnetic and ferromagnetic, in striking contrast to the equilibrium Nagaoka effect. These results are relevant for a number of condensed matter spin systems and should be observable using state of the art bosonic or fermionic quantum gas microscopes.

  1. Calculating Conductance of Ion Channels - Linking Molecular Dynamics and Electrophysiology

    NASA Astrophysics Data System (ADS)

    Wilson, Michael A.; Pohorille, Andrew

    2015-01-01

    Molecular dynamics computer simulations were combined with an electrodiffusion model to compute conduction of simple ion channels. The main assumptions of the model, and the consistency, efficiency and accuracy of the ion current calculations were tested and found satisfactory. The calculated current-voltage dependence for a synthetic peptide channel is in agreement with experiments and correctly captures the asymmetry of current with respect to applied field.

  2. Gravitation Field Calculations on a Dynamic Lattice by Distributed Computing

    NASA Astrophysics Data System (ADS)

    Mähönen, Petri; Punkka, Veikko

    A new method of calculating numerically time evolution of a gravitational field in General Relatity is introduced. Vierbein (tetrad) formalism, dynamic lattice and massively parallelized computation are suggested as they are expected to speed up the calculations considerably and facilitate the solution of problems previously considered too hard to be solved, such as the time evolution of a system consisting of two or more black holes or the structure of worm holes.

  3. Gravitational field calculations on a dynamic lattice by distributed computing.

    NASA Astrophysics Data System (ADS)

    Mähönen, P.; Punkka, V.

    A new method of calculating numerically time evolution of a gravitational field in general relativity is introduced. Vierbein (tetrad) formalism, dynamic lattice and massively parallelized computation are suggested as they are expected to speed up the calculations considerably and facilitate the solution of problems previously considered too hard to be solved, such as the time evolution of a system consisting of two or more black holes or the structure of worm holes.

  4. Machine Learning of Parameters for Accurate Semiempirical Quantum Chemical Calculations

    PubMed Central

    2015-01-01

    We investigate possible improvements in the accuracy of semiempirical quantum chemistry (SQC) methods through the use of machine learning (ML) models for the parameters. For a given class of compounds, ML techniques require sufficiently large training sets to develop ML models that can be used for adapting SQC parameters to reflect changes in molecular composition and geometry. The ML-SQC approach allows the automatic tuning of SQC parameters for individual molecules, thereby improving the accuracy without deteriorating transferability to molecules with molecular descriptors very different from those in the training set. The performance of this approach is demonstrated for the semiempirical OM2 method using a set of 6095 constitutional isomers C7H10O2, for which accurate ab initio atomization enthalpies are available. The ML-OM2 results show improved average accuracy and a much reduced error range compared with those of standard OM2 results, with mean absolute errors in atomization enthalpies dropping from 6.3 to 1.7 kcal/mol. They are also found to be superior to the results from specific OM2 reparameterizations (rOM2) for the same set of isomers. The ML-SQC approach thus holds promise for fast and reasonably accurate high-throughput screening of materials and molecules. PMID:26146493

  5. Quantum Monte Carlo Calculations of Transition Metal Oxides

    NASA Astrophysics Data System (ADS)

    Wagner, Lucas

    2006-03-01

    Quantum Monte Carlo is a powerful computational tool to study correlated systems, allowing us to explicitly treat many-body interactions with favorable scaling in the number of particles. It has been regarded as a benchmark tool for first and second row condensed matter systems, although its accuracy has not been thoroughly investigated in strongly correlated transition metal oxides. QMC has also historically suffered from the mixed estimator error in operators that do not commute with the Hamiltonian and from stochastic uncertainty, which make small energy differences unattainable. Using the Reptation Monte Carlo algorithm of Moroni and Baroni(along with contributions from others), we have developed a QMC framework that makes these previously unavailable quantities computationally feasible for systems of hundreds of electrons in a controlled and consistent way, and apply this framework to transition metal oxides. We compare these results with traditional mean-field results like the LDA and with experiment where available, focusing in particular on the polarization and lattice constants in a few interesting ferroelectric materials. This work was performed in collaboration with Lubos Mitas and Jeffrey Grossman.

  6. Machine learning of parameters for accurate semiempirical quantum chemical calculations

    SciTech Connect

    Dral, Pavlo O.; von Lilienfeld, O. Anatole; Thiel, Walter

    2015-04-14

    We investigate possible improvements in the accuracy of semiempirical quantum chemistry (SQC) methods through the use of machine learning (ML) models for the parameters. For a given class of compounds, ML techniques require sufficiently large training sets to develop ML models that can be used for adapting SQC parameters to reflect changes in molecular composition and geometry. The ML-SQC approach allows the automatic tuning of SQC parameters for individual molecules, thereby improving the accuracy without deteriorating transferability to molecules with molecular descriptors very different from those in the training set. The performance of this approach is demonstrated for the semiempirical OM2 method using a set of 6095 constitutional isomers C7H10O2, for which accurate ab initio atomization enthalpies are available. The ML-OM2 results show improved average accuracy and a much reduced error range compared with those of standard OM2 results, with mean absolute errors in atomization enthalpies dropping from 6.3 to 1.7 kcal/mol. They are also found to be superior to the results from specific OM2 reparameterizations (rOM2) for the same set of isomers. The ML-SQC approach thus holds promise for fast and reasonably accurate high-throughput screening of materials and molecules.

  7. Machine Learning of Parameters for Accurate Semiempirical Quantum Chemical Calculations

    SciTech Connect

    Dral, Pavlo O.; von Lilienfeld, O. Anatole; Thiel, Walter

    2015-05-01

    We investigate possible improvements in the accuracy of semiempirical quantum chemistry (SQC) methods through the use of machine learning (ML) models for the parameters. For a given class of compounds, ML techniques require sufficiently large training sets to develop ML models that can be used for adapting SQC parameters to reflect changes in molecular composition and geometry. The ML-SQC approach allows the automatic tuning of SQC parameters for individual molecules, thereby improving the accuracy without deteriorating transferability to molecules with molecular descriptors very different from those in the training set. The performance of this approach is demonstrated for the semiempirical OM2 method using a set of 6095 constitutional isomers C7H10O2, for which accurate ab initio atomization enthalpies are available. The ML-OM2 results show improved average accuracy and a much reduced error range compared with those of standard OM2 results, with mean absolute errors in atomization enthalpies dropping from 6.3 to 1.7 kcal/mol. They are also found to be superior to the results from specific OM2 reparameterizations (rOM2) for the same set of isomers. The ML-SQC approach thus holds promise for fast and reasonably accurate high-throughput screening of materials and molecules.

  8. Machine Learning of Parameters for Accurate Semiempirical Quantum Chemical Calculations.

    PubMed

    Dral, Pavlo O; von Lilienfeld, O Anatole; Thiel, Walter

    2015-05-12

    We investigate possible improvements in the accuracy of semiempirical quantum chemistry (SQC) methods through the use of machine learning (ML) models for the parameters. For a given class of compounds, ML techniques require sufficiently large training sets to develop ML models that can be used for adapting SQC parameters to reflect changes in molecular composition and geometry. The ML-SQC approach allows the automatic tuning of SQC parameters for individual molecules, thereby improving the accuracy without deteriorating transferability to molecules with molecular descriptors very different from those in the training set. The performance of this approach is demonstrated for the semiempirical OM2 method using a set of 6095 constitutional isomers C7H10O2, for which accurate ab initio atomization enthalpies are available. The ML-OM2 results show improved average accuracy and a much reduced error range compared with those of standard OM2 results, with mean absolute errors in atomization enthalpies dropping from 6.3 to 1.7 kcal/mol. They are also found to be superior to the results from specific OM2 reparameterizations (rOM2) for the same set of isomers. The ML-SQC approach thus holds promise for fast and reasonably accurate high-throughput screening of materials and molecules.

  9. Machine learning of parameters for accurate semiempirical quantum chemical calculations

    DOE PAGES

    Dral, Pavlo O.; von Lilienfeld, O. Anatole; Thiel, Walter

    2015-04-14

    We investigate possible improvements in the accuracy of semiempirical quantum chemistry (SQC) methods through the use of machine learning (ML) models for the parameters. For a given class of compounds, ML techniques require sufficiently large training sets to develop ML models that can be used for adapting SQC parameters to reflect changes in molecular composition and geometry. The ML-SQC approach allows the automatic tuning of SQC parameters for individual molecules, thereby improving the accuracy without deteriorating transferability to molecules with molecular descriptors very different from those in the training set. The performance of this approach is demonstrated for the semiempiricalmore » OM2 method using a set of 6095 constitutional isomers C7H10O2, for which accurate ab initio atomization enthalpies are available. The ML-OM2 results show improved average accuracy and a much reduced error range compared with those of standard OM2 results, with mean absolute errors in atomization enthalpies dropping from 6.3 to 1.7 kcal/mol. They are also found to be superior to the results from specific OM2 reparameterizations (rOM2) for the same set of isomers. The ML-SQC approach thus holds promise for fast and reasonably accurate high-throughput screening of materials and molecules.« less

  10. Comparisons of classical chemical dynamics simulations of the unimolecular decomposition of classical and quantum microcanonical ensembles.

    PubMed

    Manikandan, Paranjothy; Hase, William L

    2012-05-14

    Previous studies have shown that classical trajectory simulations often give accurate results for short-time intramolecular and unimolecular dynamics, particularly for initial non-random energy distributions. To obtain such agreement between experiment and simulation, the appropriate distributions must be sampled to choose initial coordinates and momenta for the ensemble of trajectories. If a molecule's classical phase space is sampled randomly, its initial decomposition will give the classical anharmonic microcanonical (RRKM) unimolecular rate constant for its decomposition. For the work presented here, classical trajectory simulations of the unimolecular decomposition of quantum and classical microcanonical ensembles, at the same fixed total energy, are compared. In contrast to the classical microcanonical ensemble, the quantum microcanonical ensemble does not sample the phase space randomly. The simulations were performed for CH(4), C(2)H(5), and Cl(-)---CH(3)Br using both analytic potential energy surfaces and direct dynamics methods. Previous studies identified intrinsic RRKM dynamics for CH(4) and C(2)H(5), but intrinsic non-RRKM dynamics for Cl(-)---CH(3)Br. Rate constants calculated from trajectories obtained by the time propagation of the classical and quantum microcanonical ensembles are compared with the corresponding harmonic RRKM estimates to obtain anharmonic corrections to the RRKM rate constants. The relevance and accuracy of the classical trajectory simulation of the quantum microcanonical ensemble, for obtaining the quantum anharmonic RRKM rate constant, is discussed.

  11. Calculating two-dimensional spectra with the mixed quantum-classical Ehrenfest method.

    PubMed

    van der Vegte, C P; Dijkstra, A G; Knoester, J; Jansen, T L C

    2013-07-25

    We present a mixed quantum-classical simulation approach to calculate two-dimensional spectra of coupled two-level electronic model systems. We include the change in potential energy of the classical system due to transitions in the quantum system using the Ehrenfest method. We study how this feedback of the quantum system on the classical system influences the shape of two-dimensional spectra. We show that the feedback leads to the expected Stokes shift of the energy levels in the quantum system. This subsequently leads to changes in the population transfer between quantum sites, which in turn influence the intensities of the peaks in two-dimensional spectra. The obtained spectra are compared with spectra calculated using the Hierarchical Equations of Motion method which is exact. While the spectra match perfectly for short waiting times, clear differences are found for longer waiting times. This is attributed to a violation of detailed balance between the quantum states in the Ehrenfest method. The energy of the total quantum-classical system however does obey a Boltzmann distribution, when coupled to a stochastic heat bath.

  12. Relativistic quantum metrology in open system dynamics.

    PubMed

    Tian, Zehua; Wang, Jieci; Fan, Heng; Jing, Jiliang

    2015-01-22

    Quantum metrology studies the ultimate limit of precision in estimating a physical quantity if quantum strategies are exploited. Here we investigate the evolution of a two-level atom as a detector which interacts with a massless scalar field using the master equation approach for open quantum system. We employ local quantum estimation theory to estimate the Unruh temperature when probed by a uniformly accelerated detector in the Minkowski vacuum. In particular, we evaluate the Fisher information (FI) for population measurement, maximize its value over all possible detector preparations and evolution times, and compare its behavior with that of the quantum Fisher information (QFI). We find that the optimal precision of estimation is achieved when the detector evolves for a long enough time. Furthermore, we find that in this case the FI for population measurement is independent of initial preparations of the detector and is exactly equal to the QFI, which means that population measurement is optimal. This result demonstrates that the achievement of the ultimate bound of precision imposed by quantum mechanics is possible. Finally, we note that the same configuration is also available to the maximum of the QFI itself.

  13. Relativistic Quantum Metrology in Open System Dynamics

    PubMed Central

    Tian, Zehua; Wang, Jieci; Fan, Heng; Jing, Jiliang

    2015-01-01

    Quantum metrology studies the ultimate limit of precision in estimating a physical quantity if quantum strategies are exploited. Here we investigate the evolution of a two-level atom as a detector which interacts with a massless scalar field using the master equation approach for open quantum system. We employ local quantum estimation theory to estimate the Unruh temperature when probed by a uniformly accelerated detector in the Minkowski vacuum. In particular, we evaluate the Fisher information (FI) for population measurement, maximize its value over all possible detector preparations and evolution times, and compare its behavior with that of the quantum Fisher information (QFI). We find that the optimal precision of estimation is achieved when the detector evolves for a long enough time. Furthermore, we find that in this case the FI for population measurement is independent of initial preparations of the detector and is exactly equal to the QFI, which means that population measurement is optimal. This result demonstrates that the achievement of the ultimate bound of precision imposed by quantum mechanics is possible. Finally, we note that the same configuration is also available to the maximum of the QFI itself. PMID:25609187

  14. Quantum chemistry calculation of resveratrol and related stilbenes

    NASA Astrophysics Data System (ADS)

    Del Nero, J.; de Melo, C. P.

    2003-01-01

    We report a semiempirical investigation of the first excited states and of the spectroscopic properties of resveratrol, a phytoalexin with well-known antioxidative properties, and of structurally related stilbenes. The analysis of the calculated bond length and charge rearrangements resulting from the photoexcitation and of the corresponding theoretical spectra gives us some insight of how chemical modifications of these molecules could affect the possible physiological properties of resveratrol.

  15. Comparison of Oxygen Gauche Effects in Poly(Oxyethylene) and Poly(ethylene terephtylene) Based on Quantum Chemistry Calculations

    NASA Technical Reports Server (NTRS)

    Jaffe, Richard; Han, Jie; Yoon, Do; Langhoff, Stephen R. (Technical Monitor)

    1997-01-01

    The so-called oxygen gauche effect in poly(oxyethylene) (POE) and its model molecules such as 1,2-dimethoxyethane (DME) and diglyme (CH3OC2H4OC2H4OCH3) is manifested in the preference for gauche C-C bond conformations over trans. This has also been observed for poly(ethylene terephthalate) (PET). Our previous quantum chemistry calculations demonstrated that the large C-C gauche population in DME is due, in part, to a low-lying tg +/- g+ conformer that exhibits a substantial 1,5 CH ... O attraction. New calculations will be described that demonstrate the accuracy of the original quantum chemistry calculations. In addition, an extension of this work to model molecules for PET will be presented. It is seen that the C-C gauche preference is much stronger in 1,2 diacetoxyethane than in DME. In addition, there exist low-lying tg +/- g+/- and g+/-g+/-g+/- conformers that exhibit 1,5 CH ... O attractions involving the carbonyl oxygens. It is expected that the -O-C-C-O- torsional properties will be quite different in these two polymers. The quantum chemistry results are used to parameterize rotational isomeric states models (RIS) and force fields for molecular dynamics simulations of these polymers.

  16. Comparison of Oxygen Gauche Effects in Poly(Oxyethylene) and Poly(ethylene terephtylene) Based on Quantum Chemistry Calculations

    NASA Technical Reports Server (NTRS)

    Jaffe, Richard; Han, Jie; Yoon, Do; Langhoff, Stephen R. (Technical Monitor)

    1997-01-01

    The so-called oxygen gauche effect in poly(oxyethylene) (POE) and its model molecules such as 1,2-dimethoxyethane (DME) and diglyme (CH3OC2H4OC2H4OCH3) is manifested in the preference for gauche C-C bond conformations over trans. This has also been observed for poly(ethylene terephthalate) (PET). Our previous quantum chemistry calculations demonstrated that the large C-C gauche population in DME is due, in part, to a low-lying tg +/- g+ conformer that exhibits a substantial 1,5 CH ... O attraction. New calculations will be described that demonstrate the accuracy of the original quantum chemistry calculations. In addition, an extension of this work to model molecules for PET will be presented. It is seen that the C-C gauche preference is much stronger in 1,2 diacetoxyethane than in DME. In addition, there exist low-lying tg +/- g+/- and g+/-g+/-g+/- conformers that exhibit 1,5 CH ... O attractions involving the carbonyl oxygens. It is expected that the -O-C-C-O- torsional properties will be quite different in these two polymers. The quantum chemistry results are used to parameterize rotational isomeric states models (RIS) and force fields for molecular dynamics simulations of these polymers.

  17. Quantum-chemistry calculations of hydrogen adsorption in MOF-5.

    PubMed

    Gomez, Diego A; Combariza, Aldo F; Sastre, German

    2009-10-28

    High concentrations of molecular hydrogen adsorption on MOF-5 were evaluated at the semiempirical PM6 (periodic and cluster) and ab initio MP2 (cluster) theoretical levels. From the semiempirical calculations, an uptake of 3.9% weight on the inorganic building unit of MOF-5 was estimated, in good agreement with a recent accurate estimation of 4.5-5.2%. Although PM6 allows a correct estimation of the maximum uptake, the adsorption energy was overestimated and hence ab initio calculations, including a correlation treatment at the MP2 level as well as corrections for basis set superposition error, were performed with full optimisation, including the 6-31G basis set, which rendered an adsorption energy (per hydrogen molecule) of -0.14 kcal mol(-1). The crucial role of the quality of the basis set, as well as the importance of simulating high hydrogen loading (resembling experimental measurements), are remarked. Single point calculations (using the 6-31G geometry) with improved basis sets 6-31G(d,p) and 6-31++G(d,p) yielded adsorption energies of -0.33 and -0.57 kcal mol(-1), the latter in reasonable agreement with a recent experimental estimation of -1.0 kcal mol(-1). The role of the intermolecular hydrogen interactions is highlighted in this study, since many previous computational studies were performed at low hydrogen loadings, far from the experimental uptake conditions.

  18. Efficient method for calculating electronic bound states in arbitrary one-dimensional quantum wells

    NASA Astrophysics Data System (ADS)

    de Aquino, V. M.; Iwamoto, H.; Dias, I. F. L.; Laureto, E.; da Silva, M. A. T.; da Silva, E. C. F.; Quivy, A. A.

    2017-01-01

    In the present paper it is demonstrated that the bound electronic states of multiple quantum wells structures may be calculated very efficiently by expanding their eigenstates in terms of the eigenfunctions of a particle in a box. The bound states of single and multiple symmetric or nonsymmetric wells are calculated within the single-band effective mass approximation. A comparison is then made between the results obtained for simple cases with exact calculations. We also apply our approach to a GaAs/AlGaAs multiple quantum well structure composed of forty periods each one with seven quantum wells. The method may be very useful to design narrow band quantum cascade photodetectors to work without applied bias in a photovoltaic mode. With the presented method the effects of a electric field may also be easily included which is very important if one desires study quantum well structures for application to the development of quantum cascade lasers. The advantages of the method are also presented.

  19. Communications: Evaluation of the nondiabaticity of quantum molecular dynamics with the dephasing representation of quantum fidelity.

    PubMed

    Zimmermann, Tomás; Vanícek, Jirí

    2010-06-28

    We propose an approximate method for evaluating the importance of non-Born-Oppenheimer effects on the quantum dynamics of nuclei. The method uses a generalization of the dephasing representation (DR) of quantum fidelity to several diabatic potential energy surfaces and its computational cost is the cost of dynamics of a classical phase space distribution. It can be implemented easily into any molecular dynamics program and also can utilize on-the-fly ab initio electronic structure information. We test the methodology on three model problems introduced by Tully and on the photodissociation of NaI. The results show that for dynamics close to the diabatic limit, the decay of fidelity due to nondiabatic effects is described accurately by the DR. In this regime, unlike the mixed quantum-classical methods such as surface hopping or Ehrenfest dynamics, the DR can capture more subtle quantum effects than the population transfer between potential energy surfaces. Hence we propose using the DR to estimate the dynamical importance of diabatic, spin-orbit, or other couplings between potential energy surfaces. The acquired information can help reduce the complexity of a studied system without affecting the accuracy of the quantum simulation.

  20. Role of Core Electrons in Quantum Dynamics Using TDDFT.

    PubMed

    Foglia, Nicolás O; Morzan, Uriel N; Estrin, Dario A; Scherlis, Damian A; Gonzalez Lebrero, Mariano C

    2017-01-10

    The explicit simulation of time dependent electronic processes requires computationally onerous routes involving the temporal integration of motion equations for the charge density. Efficiency optimization of these methods typically relies on increasing the integration time-step and on the reduction of the computational cost per step. The implicit representation of inner electrons by effective core potentials-or pseudopotentials-is a standard practice in localized-basis quantum-chemistry implementations to improve the efficiency of ground-state calculations, still preserving the quality of the output. This article presents an investigation on the impact that effective core potentials have on the overall efficiency of real time electron dynamics with TDDFT. Interestingly, the speedups achieved with the use of pseudopotentials in this kind of simulation are on average much more significant than in ground-state calculations, reaching in some cases a factor as large as 600×. This boost in performance originates from two contributions: on the one hand, the size of the density matrix, which is considerably reduced, and, on the other, the elimination of high-frequency electronic modes, responsible for limiting the maximum time-step, which vanish when the core electrons are not propagated explicitly. The latter circumstance allows for significant increases in time-step, that in certain cases may reach up to 3 orders of magnitude, without losing any relevant chemical or spectroscopic information.

  1. Optimal approach to quantum communication using dynamic programming

    PubMed Central

    Jiang, Liang; Taylor, Jacob M.; Khaneja, Navin; Lukin, Mikhail D.

    2007-01-01

    Reliable preparation of entanglement between distant systems is an outstanding problem in quantum information science and quantum communication. In practice, this has to be accomplished by noisy channels (such as optical fibers) that generally result in exponential attenuation of quantum signals at large distances. A special class of quantum error correction protocols, quantum repeater protocols, can be used to overcome such losses. In this work, we introduce a method for systematically optimizing existing protocols and developing more efficient protocols. Our approach makes use of a dynamic programming-based searching algorithm, the complexity of which scales only polynomially with the communication distance, letting us efficiently determine near-optimal solutions. We find significant improvements in both the speed and the final-state fidelity for preparing long-distance entangled states. PMID:17959783

  2. Linear Optics Simulation of Quantum Non-Markovian Dynamics

    PubMed Central

    Chiuri, Andrea; Greganti, Chiara; Mazzola, Laura; Paternostro, Mauro; Mataloni, Paolo

    2012-01-01

    The simulation of open quantum dynamics has recently allowed the direct investigation of the features of system-environment interaction and of their consequences on the evolution of a quantum system. Such interaction threatens the quantum properties of the system, spoiling them and causing the phenomenon of decoherence. Sometimes however a coherent exchange of information takes place between system and environment, memory effects arise and the dynamics of the system becomes non-Markovian. Here we report the experimental realisation of a non-Markovian process where system and environment are coupled through a simulated transverse Ising model. By engineering the evolution in a photonic quantum simulator, we demonstrate the role played by system-environment correlations in the emergence of memory effects. PMID:23236588

  3. Linear Optics Simulation of Quantum Non-Markovian Dynamics

    NASA Astrophysics Data System (ADS)

    Chiuri, Andrea; Greganti, Chiara; Mazzola, Laura; Paternostro, Mauro; Mataloni, Paolo

    2012-12-01

    The simulation of open quantum dynamics has recently allowed the direct investigation of the features of system-environment interaction and of their consequences on the evolution of a quantum system. Such interaction threatens the quantum properties of the system, spoiling them and causing the phenomenon of decoherence. Sometimes however a coherent exchange of information takes place between system and environment, memory effects arise and the dynamics of the system becomes non-Markovian. Here we report the experimental realisation of a non-Markovian process where system and environment are coupled through a simulated transverse Ising model. By engineering the evolution in a photonic quantum simulator, we demonstrate the role played by system-environment correlations in the emergence of memory effects.

  4. Geometric origin of dynamically induced freezing of quantum evolution

    SciTech Connect

    Matos-Abiague, A.; Berakdar, J.

    2006-02-15

    The phenomenon of dynamical, field-induced freezing of quantum evolution is discussed. It occurs when a time-dependent state is dynamically driven in such a way that the evolution of the corresponding wave function is effectively localized within a small region in the projective Hilbert space. As a consequence, the dynamics of the system is frozen and the expectation values of all physical observables hardly change with time. Necessary and sufficient conditions for inducing dynamical freezing are inferred from a general analysis of the geometry of quantum evolution. The relevance of the dynamical freezing for a sustainable in time, dynamical control is discussed and exemplified by a study of the coherent control of the kicked rotor motion.

  5. Ring-Polymer Molecular Dynamics Rate Coefficient Calculations for Insertion Reactions: X + H2 → HX + H (X = N, O).

    PubMed

    Li, Yongle; Suleimanov, Yury V; Guo, Hua

    2014-02-20

    The thermal rate constants of two prototypical insertion-type reactions, namely, N/O + H2 → NH/OH + H, are investigated with ring polymer molecular dynamics (RPMD) on full-dimensional potential energy surfaces using recently developed RPMDrate code. It is shown that the unique ability of the RPMD approach among the existing theoretical methods to capture the quantum effects, e.g., tunneling and zero-point energy, as well as recrossing dynamics quantum mechanically with ring-polymer trajectories leads to excellent agreement with rigorous quantum dynamics calculations. The present result is encouraging for future applications of the RPMD method and the RPMDrate code to complex-forming chemical reactions involving polyatomic reactants.

  6. Quantum chemistry calculations for molecules coupled to reservoirs: Formalism, implementation, and application to benzenedithiol

    NASA Astrophysics Data System (ADS)

    Arnold, A.; Weigend, F.; Evers, F.

    2007-05-01

    Modern quantum chemistry calculations are usually implemented for isolated systems—big molecules or atom clusters; total energy and particle number are fixed. However, in many situations, like quantum transport calculations or molecules in a electrochemical environment, the molecule can exchange particles (and energy) with a reservoir. Calculations for such cases require to switch from the canonical to a grand canonical description, where one fixes the chemical potential rather than particle number. To achieve this goal, the authors propose an implementation in standard quantum chemistry packages. An application to the nonlinear charge transport through 1,4-benzenedithiol will be presented. They explain the leading finite bias effect on the transmission as a consequence of a nonequilibrium Stark effect and discuss the relation to earlier work.

  7. Yoshimori-Kasai Model Phase Diagram and Naniwa Series for Quantum Dynamics

    NASA Astrophysics Data System (ADS)

    Arguelles, Elvis; Shimizu, Koji; Nakanishi, Hiroshi; Kasai, Hideaki

    We present the phase diagram of heavy fermions system (HFS) and muon adsorption calculations on Pd (111) surface. HFS undergoes phase transitions from Fermi liquid (FL) to non-Fermi liquid (NFL). Furthermore, antiferromagnetic (AF), spin-density wave (SDW)and superconductivity can be realized by changing electron densities and temperature. It is shown that at upper Hubbard band filling, HFS changes phase from antiferromagnetic to superconducting at low temperatures. Furthermore, in an attempt to elucidate muon dynamics on surfaces and subsurfaces, we show thatmuon exhibits tunneling effects independent of surface vibrations from quantum dynamical calculations. The results shown herein may have important implications on future ultra-slow muon experiments.

  8. Quantum modeling of nonlinear dynamics of stock prices: Bohmian approach

    NASA Astrophysics Data System (ADS)

    Choustova, O.

    2007-08-01

    We use quantum mechanical methods to model the price dynamics in the financial market mathematically. We propose describing behavioral financial factors using the pilot-wave (Bohmian) model of quantum mechanics. The real price trajectories are determined (via the financial analogue of the second Newton law) by two financial potentials: the classical-like potential V (q) (“hard” market conditions) and the quantumlike potential U(q) (behavioral market conditions).

  9. Dynamics of quantum correlation and coherence in de Sitter universe

    NASA Astrophysics Data System (ADS)

    Huang, Zhiming

    2017-09-01

    In this article, we investigate the dynamics of quantum correlation and coherence for two atoms interacting with massless scalar field in the background de Sitter spacetime. We firstly analyze the solving process of master equation that describes the system evolution with initial Werner state. Then, we discuss the degradation, generation, revival and enhancement of quantum correlation and coherence for three cases of different initial states: zero correlation state, nonzero correlation separable state and maximally entangled state.

  10. Information dynamics and new geometric foundations of quantum theory

    NASA Astrophysics Data System (ADS)

    Kostecki, Ryszard Paweł

    2012-03-01

    We discuss new approach to mathematical foundations of quantum theory, which is completely independent of Hilbert spaces and measure spaces. New kinematics is defined by nonlinear geometry of spaces of integrals on abstract non-commutative algebras. New dynamics is defined by constrained maximisation of quantum relative entropy. We recover Hilbert space based approach (including unitary evolution and the von Neumann-Lüders rule) and measure theoretic approach to probability theory (including Bayes' rule) as special cases of our approach.

  11. Dynamical localization in molecular alignment of kicked quantum rotors

    SciTech Connect

    Kamalov, A.; Broege, D. W.; Bucksbaum, P. H.

    2015-07-13

    The periodically δ -kicked quantum linear rotor is known to experience nonclassical bounded energy growth due to quantum dynamical localization in angular momentum space. We study the effect of random deviations of the kick period in simulations and experiments. This breaks the energy and angular momentum localization and increases the rotational alignment, which is the analog of the onset of Anderson localization in one-dimensional chains.

  12. Partial dynamical symmetry at critical points of quantum phase transitions.

    PubMed

    Leviatan, A

    2007-06-15

    We show that partial dynamical symmetries can occur at critical points of quantum phase transitions, in which case underlying competing symmetries are conserved exactly by a subset of states, and mix strongly in other states. Several types of partial dynamical symmetries are demonstrated with the example of critical-point Hamiltonians for first- and second-order transitions in the framework of the interacting boson model, whose dynamical symmetries correspond to different shape phases in nuclei.

  13. Complex scattering dynamics and the quantum Hall effects

    SciTech Connect

    Trugman, S.A.

    1994-12-16

    We review both classical and quantum potential scattering in two dimensions in a magnetic field, with applications to the quantum Hall effect. Classical scattering is complex, due to the approach of scattering states to an infinite number of dynamically bound states. Quantum scattering follows the classical behavior rather closely, exhibiting sharp resonances in place of the classical bound states. Extended scatterers provide a quantitative explanation for the breakdown of the QHE at a comparatively small Hall voltage as seen by Kawaji et al., and possibly for noise effects.

  14. Computer studies of multiple-quantum spin dynamics

    SciTech Connect

    Murdoch, J.B.

    1982-11-01

    The excitation and detection of multiple-quantum (MQ) transitions in Fourier transform NMR spectroscopy is an interesting problem in the quantum mechanical dynamics of spin systems as well as an important new technique for investigation of molecular structure. In particular, multiple-quantum spectroscopy can be used to simplify overly complex spectra or to separate the various interactions between a nucleus and its environment. The emphasis of this work is on computer simulation of spin-system evolution to better relate theory and experiment.

  15. Bohmian dynamics on subspaces using linearized quantum force.

    PubMed

    Rassolov, Vitaly A; Garashchuk, Sophya

    2004-04-15

    In the de Broglie-Bohm formulation of quantum mechanics the time-dependent Schrodinger equation is solved in terms of quantum trajectories evolving under the influence of quantum and classical potentials. For a practical implementation that scales favorably with system size and is accurate for semiclassical systems, we use approximate quantum potentials. Recently, we have shown that optimization of the nonclassical component of the momentum operator in terms of fitting functions leads to the energy-conserving approximate quantum potential. In particular, linear fitting functions give the exact time evolution of a Gaussian wave packet in a locally quadratic potential and can describe the dominant quantum-mechanical effects in the semiclassical scattering problems of nuclear dynamics. In this paper we formulate the Bohmian dynamics on subspaces and define the energy-conserving approximate quantum potential in terms of optimized nonclassical momentum, extended to include the domain boundary functions. This generalization allows a better description of the non-Gaussian wave packets and general potentials in terms of simple fitting functions. The optimization is performed independently for each domain and each dimension. For linear fitting functions optimal parameters are expressed in terms of the first and second moments of the trajectory distribution. Examples are given for one-dimensional anharmonic systems and for the collinear hydrogen exchange reaction.

  16. Quantum Calculations of Electron Tunneling in Respiratory Complex III.

    PubMed

    Hagras, Muhammad A; Hayashi, Tomoyuki; Stuchebrukhov, Alexei A

    2015-11-19

    The most detailed and comprehensive to date study of electron transfer reactions in the respiratory complex III of aerobic cells, also known as bc1 complex, is reported. In the framework of the tunneling current theory, electron tunneling rates and atomistic tunneling pathways between different redox centers were investigated for all electron transfer reactions comprising different stages of the proton-motive Q-cycle. The calculations reveal that complex III is a smart nanomachine, which under certain conditions undergoes conformational changes gating electron transfer, or channeling electrons to specific pathways. One-electron tunneling approximation was adopted in the tunneling calculations, which were performed using hybrid Broken-Symmetry (BS) unrestricted DFT/ZINDO levels of theory. The tunneling orbitals were determined using an exact biorthogonalization scheme that uniquely separates pairs of tunneling orbitals with small overlaps out of the remaining Franck-Condon orbitals with significant overlap. Electron transfer rates in different redox pairs show exponential distance dependence, in agreement with the reported experimental data; some reactions involve coupled proton transfer. Proper treatment of a concerted two-electron bifurcated tunneling reaction at the Q(o) site is given.

  17. Equation of state of dense plasmas: Orbital-free molecular dynamics as the limit of quantum molecular dynamics for high-Z elements

    SciTech Connect

    Danel, J.-F.; Blottiau, P.; Kazandjian, L.; Piron, R.; Torrent, M.

    2014-10-15

    The applicability of quantum molecular dynamics to the calculation of the equation of state of a dense plasma is limited at high temperature by computational cost. Orbital-free molecular dynamics, based on a semiclassical approximation and possibly on a gradient correction, is a simulation method available at high temperature. For a high-Z element such as lutetium, we examine how orbital-free molecular dynamics applied to the equation of state of a dense plasma can be regarded as the limit of quantum molecular dynamics at high temperature. For the normal mass density and twice the normal mass density, we show that the pressures calculated with the quantum approach converge monotonically towards those calculated with the orbital-free approach; we observe a faster convergence when the orbital-free approach includes the gradient correction. We propose a method to obtain an equation of state reproducing quantum molecular dynamics results up to high temperatures where this approach cannot be directly implemented. With the results already obtained for low-Z plasmas, the present study opens the way for reproducing the quantum molecular dynamics pressure for all elements up to high temperatures.

  18. Operators versus functions: from quantum dynamical semigroups to tomographic semigroups

    NASA Astrophysics Data System (ADS)

    Aniello, Paolo

    2013-11-01

    Quantum mechanics can be formulated in terms of phase-space functions, according to Wigner's approach. A generalization of this approach consists in replacing the density operators of the standard formulation with suitable functions, the so-called generalized Wigner functions or (group-covariant) tomograms, obtained by means of group-theoretical methods. A typical problem arising in this context is to express the evolution of a quantum system in terms of tomograms. In the case of a (suitable) open quantum system, the dynamics can be described by means of a quantum dynamical semigroup 'in disguise', namely, by a semigroup of operators acting on tomograms rather than on density operators. We focus on a special class of quantum dynamical semigroups, the twirling semigroups, that have interesting applications, e.g., in quantum information science. The 'disguised counterparts' of the twirling semigroups, i.e., the corresponding semigroups acting on tomograms, form a class of semigroups of operators that we call tomographic semigroups. We show that the twirling semigroups and the tomographic semigroups can be encompassed in a unique theoretical framework, a class of semigroups of operators including also the probability semigroups of classical probability theory, so achieving a deeper insight into both the mathematical and the physical aspects of the problem.

  19. Stochastic approximation of dynamical exponent at quantum critical point

    NASA Astrophysics Data System (ADS)

    Yasuda, Shinya; Suwa, Hidemaro; Todo, Synge

    2015-09-01

    We have developed a unified finite-size scaling method for quantum phase transitions that requires no prior knowledge of the dynamical exponent z . During a quantum Monte Carlo simulation, the temperature is automatically tuned by the Robbins-Monro stochastic approximation method, being proportional to the lowest gap of the finite-size system. The dynamical exponent is estimated in a straightforward way from the system-size dependence of the temperature. As a demonstration of our novel method, the two-dimensional S =1 /2 quantum X Y model in uniform and staggered magnetic fields is investigated in the combination of the world-line quantum Monte Carlo worm algorithm. In the absence of a uniform magnetic field, we obtain the fully consistent result with the Lorentz invariance at the quantum critical point, z =1 , i.e., the three-dimensional classical X Y universality class. Under a finite uniform magnetic field, on the other hand, the dynamical exponent becomes two, and the mean-field universality with effective dimension (2 +2 ) governs the quantum phase transition.

  20. Computational Issues in the Control of Quantum Dynamics

    NASA Astrophysics Data System (ADS)

    Rabitz, Herschel

    2003-03-01

    Computational Issues in the Control of Quantum Dynamics Phenomena Herschel Rabitz Department of Chemistry Princeton University The control of quantum phenomena embraces a variety of applications, with the most common implementation involving tailored laser pulses to steer the dynamics of a quantum system towards some specified observable outcome. The theoretical and computational aspects of this subject are intimately tied to the growing experimental capabilities, especially the ability to perform massive numbers of high throughput experiments. Computational studies in this context have special roles. Especially important is the use of computational techniques to develop new control algorithms, which ultimately would be implemented in the laboratory to guide the control of complex quantum systems. Beyond control alone, many of the same concepts can be exploited for the performance of experiments optimally tuned for inversion, to extract Hamiltonian information. The latter scenario poses very high demands on the efficiency of solving the quantum dynamics equations to extract the information content from the experimental data. The concept of exploiting a computational quantum control tool kit will be introduced as a means for addressing many of these challenges.

  1. Dynamical quantum phase transitions in presence of a spin bath

    NASA Astrophysics Data System (ADS)

    Gómez-León, Á.; Stamp, P. C. E.

    2017-02-01

    We derive an effective time independent Hamiltonian for the transverse Ising model coupled to a spin bath, in the presence of a high frequency AC magnetic field. The spin blocking mechanism that removes the quantum phase transition can be suppressed by the AC field, allowing tunability of the quantum critical point. We calculate the phase diagram, including the nuclear spins, and apply the results to quantum Ising systems with long-range dipolar interactions; the example of LiHoF4 is discussed in detail.

  2. Nonanalyticity, Valley Quantum Phases, and Lightlike Exciton Dispersion in Monolayer Transition Metal Dichalcogenides: Theory and First-Principles Calculations.

    PubMed

    Qiu, Diana Y; Cao, Ting; Louie, Steven G

    2015-10-23

    Exciton dispersion as a function of center-of-mass momentum Q is essential to the understanding of exciton dynamics. We use the ab initio GW-Bethe-Salpeter equation method to calculate the dispersion of excitons in monolayer MoS(2) and find a nonanalytic lightlike dispersion. This behavior arises from an unusual |Q|-term in both the intra- and intervalley exchange of the electron-hole interaction, which concurrently gives rise to a valley quantum phase of winding number two. A simple effective Hamiltonian to Q(2) order with analytic solutions is derived to describe quantitatively these behaviors.

  3. Nonanalyticity, Valley Quantum Phases, and Lightlike Exciton Dispersion in Monolayer Transition Metal Dichalcogenides: Theory and First-Principles Calculations

    NASA Astrophysics Data System (ADS)

    Qiu, Diana Y.; Cao, Ting; Louie, Steven G.

    2015-10-01

    Exciton dispersion as a function of center-of-mass momentum Q is essential to the understanding of exciton dynamics. We use the ab initio G W -Bethe-Salpeter equation method to calculate the dispersion of excitons in monolayer MoS2 and find a nonanalytic lightlike dispersion. This behavior arises from an unusual |Q |-term in both the intra- and intervalley exchange of the electron-hole interaction, which concurrently gives rise to a valley quantum phase of winding number two. A simple effective Hamiltonian to Q2 order with analytic solutions is derived to describe quantitatively these behaviors.

  4. Multi channel quantum defect theory calculations of the Rydberg spectra of HCO

    NASA Astrophysics Data System (ADS)

    Douguet, Nicolas; Orel, Ann

    2014-05-01

    We present a first-principles theoretical study of the photoionization spectra of vibrationally autoionizing Rydberg states converging to excited states of HCO+. The clamped-nuclei scattering matrix, quantum defects parameters and transition dipole moments are explicitly calculated using the complex variational Kohn technique. The multi-channel quantum defect theory and vibrational frame transformation are then used to calculate the absorption spectrum. The results are compared with experimental data on double-resonance spectroscopy of the high Rydberg states of formyl radical. This work is supported by the DOE Office of Basic Energy Science and the National Science Foundation, Grant No's PHY-10-68785 and PHY-11-60611.

  5. PDB ligand conformational energies calculated quantum-mechanically.

    PubMed

    Sitzmann, Markus; Weidlich, Iwona E; Filippov, Igor V; Liao, Chenzhong; Peach, Megan L; Ihlenfeldt, Wolf-Dietrich; Karki, Rajeshri G; Borodina, Yulia V; Cachau, Raul E; Nicklaus, Marc C

    2012-03-26

    We present here a greatly updated version of an earlier study on the conformational energies of protein-ligand complexes in the Protein Data Bank (PDB) [Nicklaus et al. Bioorg. Med. Chem. 1995, 3, 411-428], with the goal of improving on all possible aspects such as number and selection of ligand instances, energy calculations performed, and additional analyses conducted. Starting from about 357,000 ligand instances deposited in the 2008 version of the Ligand Expo database of the experimental 3D coordinates of all small-molecule instances in the PDB, we created a "high-quality" subset of ligand instances by various filtering steps including application of crystallographic quality criteria and structural unambiguousness. Submission of 640 Gaussian 03 jobs yielded a set of about 415 successfully concluded runs. We used a stepwise optimization of internal degrees of freedom at the DFT level of theory with the B3LYP/6-31G(d) basis set and a single-point energy calculation at B3LYP/6-311++G(3df,2p) after each round of (partial) optimization to separate energy changes due to bond length stretches vs bond angle changes vs torsion changes. Even for the most "conservative" choice of all the possible conformational energies-the energy difference between the conformation in which all internal degrees of freedom except torsions have been optimized and the fully optimized conformer-significant energy values were found. The range of 0 to ~25 kcal/mol was populated quite evenly and independently of the crystallographic resolution. A smaller number of "outliers" of yet higher energies were seen only at resolutions above 1.3 Å. The energies showed some correlation with molecular size and flexibility but not with crystallographic quality metrics such as the Cruickshank diffraction-component precision index (DPI) and R(free)-R, or with the ligand instance-specific metrics such as occupancy-weighted B-factor (OWAB), real-space R factor (RSR), and real-space correlation coefficient

  6. Sensing of molecules using quantum dynamics

    DOE PAGES

    Migliore, Agostino; Naaman, Ron; Beratan, David N.

    2015-04-24

    In this study, we design sensors where information is transferred between the sensing event and the actuator via quantum relaxation processes, through distances of a few nanometers. We thus explore the possibility of sensing using intrinsically quantum mechanical phenomena that are also at play in photobiology, bioenergetics, and information processing. Specifically, we analyze schemes for sensing based on charge transfer and polarization (electronic relaxation) processes. These devices can have surprising properties. Their sensitivity can increase with increasing separation between the sites of sensing (the receptor) and the actuator (often a solid-state substrate). This counterintuitive response and other quantum features givemore » these devices favorable characteristics, such as enhanced sensitivity and selectivity. Finally, using coherent phenomena at the core of molecular sensing presents technical challenges but also suggests appealing schemes for molecular sensing and information transfer in supramolecular structures.« less

  7. Ab initio quantum direct dynamics simulations of ultrafast photochemistry with Multiconfigurational Ehrenfest approach

    NASA Astrophysics Data System (ADS)

    Makhov, Dmitry V.; Symonds, Christopher; Fernandez-Alberti, Sebastian; Shalashilin, Dmitrii V.

    2017-08-01

    The Multiconfigurational Ehrenfest (MCE) method is a quantum dynamics technique which allows treatment of a large number of quantum nuclear degrees of freedom. This paper presents a review of MCE and its recent applications, providing a summary of the formalisms, including its ab initio direct dynamics versions and also giving a summary of recent results. Firstly, we describe the Multiconfigurational Ehrenfest version 2 (MCEv2) method and its applicability to direct dynamics and report new calculations which show that the approach converges to the exact result in model systems with tens of degrees of freedom. Secondly, we review previous ;on the fly; ab initio Multiple Cloning (AIMC-MCE) MCE dynamics results obtained for systems of a similar size, in which the calculations treat every electron and every nucleus of a polyatomic molecule on a fully quantum basis. We also review the Time Dependent Diabatic Basis (TDDB) version of the technique and give an example of its application. We summarise the details of the sampling techniques and interpolations used for calculation of the matrix elements, which make our approach efficient. Future directions of work are outlined.

  8. Scaling and Universality at Dynamical Quantum Phase Transitions.

    PubMed

    Heyl, Markus

    2015-10-02

    Dynamical quantum phase transitions (DQPTs) at critical times appear as nonanalyticities during nonequilibrium quantum real-time evolution. Although there is evidence for a close relationship between DQPTs and equilibrium phase transitions, a major challenge is still to connect to fundamental concepts such as scaling and universality. In this work, renormalization group transformations in complex parameter space are formulated for quantum quenches in Ising models showing that the DQPTs are critical points associated with unstable fixed points of equilibrium Ising models. Therefore, these DQPTs obey scaling and universality. On the basis of numerical simulations, signatures of these DQPTs in the dynamical buildup of spin correlations are found with an associated power-law scaling determined solely by the fixed point's universality class. An outlook is given on how to explore this dynamical scaling experimentally in systems of trapped ions.

  9. Heideggerian dynamics and the monadological role of the 'between': A crossing with quantum brain dynamics.

    PubMed

    Globus, Gordon

    2015-12-01

    Heideggerian theory is retrieved as a dynamics, the "Godly event" of das Ereignis ("enowning"), which is unexpectedly compatible with a version of quantum brain dynamics. In both the "between" (das Zwischen) has the fundamental role of the dis-closure that is Existenz. Heidegger's harsh critique of technology and science does not apply to revolutionary quantum brain dynamics. The crossing between Heidegger and quantum brain dynamics, as well as one fundamental ontological difference, illuminates both. To our surprise this difference turns out, contra Heidegger, to be monadological. The monadological conception is applied to long-standing problematics of measurement in quantum physics and consciousness in philosophy. Heideggerian Existenz is affirmed as fundamentally non-computational but is reformulated as a dynamical process of monadological dis-closure that radically deconstructs transcendent world. Copyright © 2015. Published by Elsevier Ltd.

  10. Discrete scale invariant quantum dynamics and universal quantum beats in Bose gases

    NASA Astrophysics Data System (ADS)

    Maki, J.; Jiang, S. J.; Zhou, F.

    2017-06-01

    We study the signature of classical scale invariance in the far-from-equilibrium quantum dynamics of two-dimensional Bose gases. We show that the density profile displays a scale invariant logarithmic singularity near the center. In addition, the density oscillates due to quantum beats with universal structures. Namely, the frequencies of the beats can be connected with one another by a universal discrete scale transformation induced by the classical scale invariance. The experimental applicability of these results is then discussed.

  11. Cosmological dynamics in spin-foam loop quantum cosmology: challenges and prospects

    NASA Astrophysics Data System (ADS)

    Craig, David A.; Singh, Parampreet

    2017-04-01

    We explore the structure of the spin foam-like vertex expansion in loop quantum cosmology and discuss properties of the corresponding amplitudes, with the aim of elucidating some of the expansion’s useful properties and features. We find that the expansion is best suited for consideration of conceptual questions and for investigating short-time, highly quantum behavior. In order to study dynamics at cosmological scales, the expansion must be carried to very high order, limiting its direct utility as a calculational tool for such questions. Conversely, it is unclear that the expansion can be truncated at finite order in a controlled manner.

  12. Four-dimensional quantum oscillator and magnetic monopole with U(1) dynamical group

    NASA Astrophysics Data System (ADS)

    Bakhshi, Z.; Panahi, H.; Golchehre, S. G.

    2017-09-01

    By using an appropriate transformation, it was shown that the quantum system of four-dimensional (4D) simple harmonic oscillator can describe the motion of a charged particle in the presence of a magnetic monopole field. It was shown that the Dirac magnetic monopole has the hidden algebra of U(1) symmetry and by reducing the dimensions of space, the U(1) × U(1) dynamical group for 4D harmonic oscillator quantum system was obtained. Using the group representation and based on explicit solution of the obtained differential equation, the spectrum of system was calculated.

  13. Noise-resilient quantum evolution steered by dynamical decoupling

    PubMed Central

    Liu, Gang-Qin; Po, Hoi Chun; Du, Jiangfeng; Liu, Ren-Bao; Pan, Xin-Yu

    2013-01-01

    Realistic quantum computing is subject to noise. Therefore, an important frontier in quantum computing is to implement noise-resilient quantum control over qubits. At the same time, dynamical decoupling can protect the coherence of qubits. Here we demonstrate non-trivial quantum evolution steered by dynamical decoupling control, which simultaneously suppresses noise effects. We design and implement a self-protected controlled-NOT gate on the electron spin of a nitrogen-vacancy centre and a nearby carbon-13 nuclear spin in diamond at room temperature, by employing an engineered dynamical decoupling control on the electron spin. Final state fidelity of 0.91(1) is observed in preparation of a Bell state using the gate. At the same time, the qubit coherence time is elongated at least 30 fold. The design scheme does not require the dynamical decoupling control to commute with the qubit interaction and therefore works for general qubit systems. This work marks a step towards implementing realistic quantum computing systems. PMID:23912335

  14. Quantum superchemistry: dynamical quantum effects in coupled atomic and molecular Bose-Einstein condensates.

    PubMed

    Hope, J J; Olsen, M K

    2001-04-09

    We show that in certain parameter regimes there is a macroscopic dynamical breakdown of the Gross-Pitaevskii equation. Stochastic field equations for coupled atomic and molecular condensates are derived using the functional positive- P representation. These equations describe the full quantum state of the coupled condensates and include the commonly used Gross-Pitaevskii equation as the noiseless limit. The full quantum theory includes the spontaneous processes which will become significant when the atomic population is low. The experimental signature of the quantum effects will be the time scale of the revival of the atomic population after a near total conversion to the molecular condensate.

  15. Simulation of Quantum Dynamics Based on the Quantum Stochastic Differential Equation

    PubMed Central

    2013-01-01

    The quantum stochastic differential equation derived from the Lindblad form quantum master equation is investigated. The general formulation in terms of environment operators representing the quantum state diffusion is given. The numerical simulation algorithm of stochastic process of direct photodetection of a driven two-level system for the predictions of the dynamical behavior is proposed. The effectiveness and superiority of the algorithm are verified by the performance analysis of the accuracy and the computational cost in comparison with the classical Runge-Kutta algorithm. PMID:23781156

  16. Simulation of quantum dynamics based on the quantum stochastic differential equation.

    PubMed

    Li, Ming

    2013-01-01

    The quantum stochastic differential equation derived from the Lindblad form quantum master equation is investigated. The general formulation in terms of environment operators representing the quantum state diffusion is given. The numerical simulation algorithm of stochastic process of direct photodetection of a driven two-level system for the predictions of the dynamical behavior is proposed. The effectiveness and superiority of the algorithm are verified by the performance analysis of the accuracy and the computational cost in comparison with the classical Runge-Kutta algorithm.

  17. Thermalization dynamics close to a quantum phase transition.

    PubMed

    Patanè, Dario; Silva, Alessandro; Sols, Fernando; Amico, Luigi

    2009-06-19

    We investigate the dissipative dynamics of a quantum critical system in contact with a thermal bath, focusing on the response of the system to a sudden change of the bath temperature, in analogy to studies of aging. The specific example of the XY model in a transverse magnetic field whose spins are locally coupled to a set of bosonic baths is considered. We analyze the spin-spin correlations and block correlations and identify some universal features in the out-of-equilibrium dynamics. Two distinct regimes, characterized by different time and length scales, emerge. The initial transient dynamics is characterized by the same critical exponents as those of the equilibrium quantum phase transition and resembles the dynamics of thermal phase transitions. At long times equilibrium is reached through the propagation along the chain of a thermal front in a manner similar to the classical Glauber dynamics.

  18. Quantum Monte Carlo calculations of the dimerization energy of borane.

    PubMed

    Fracchia, Francesco; Bressanini, Dario; Morosi, Gabriele

    2011-09-07

    Accurate thermodynamic data are required to improve the performance of chemical hydrides that are potential hydrogen storage materials. Boron compounds are among the most interesting candidates. However, different experimental measurements of the borane dimerization energy resulted in a rather wide range (-34.3 to -39.1) ± 2 kcal/mol. Diffusion Monte Carlo (DMC) simulations usually recover more than 95% of the correlation energy, so energy differences rely less on error cancellation than other methods. DMC energies of BH(3), B(2)H(6), BH(3)CO, CO, and BH(2)(+) allowed us to predict the borane dimerization energy, both via the direct process and indirect processes such as the dissociation of BH(3)CO. Our D(e) = -43.12(8) kcal/mol, corrected for the zero point energy evaluated by considering the anharmonic contributions, results in a borane dimerization energy of -36.59(8) kcal/mol. The process via the dissociation of BH(3)CO gives -34.5(2) kcal/mol. Overall, our values suggest a slightly less D(e) than the most recent W4 estimate D(e) = -44.47 kcal/mol [A. Karton and J. M. L. Martin, J. Phys. Chem. A 111, 5936 (2007)]. Our results show that reliable thermochemical data for boranes can be predicted by fixed node (FN)-DMC calculations.

  19. Molecular docking, spectroscopic studies and quantum calculations on nootropic drug.

    PubMed

    Uma Maheswari, J; Muthu, S; Sundius, Tom

    2014-04-05

    A systematic vibrational spectroscopic assignment and analysis of piracetam [(2-oxo-1-pyrrolidineacetamide)] have been carried out using FT-IR and FT-Raman spectral data. The vibrational analysis was aided by an electronic structure calculation based on the hybrid density functional method B3LYP using a 6-311G++(d,p) basis set. Molecular equilibrium geometries, electronic energies, IR and Raman intensities, and harmonic vibrational frequencies have been computed. The assignments are based on the experimental IR and Raman spectra, and a complete assignment of the observed spectra has been proposed. The UV-visible spectrum of the compound was recorded and the electronic properties, such as HOMO and LUMO energies and the maximum absorption wavelengths λmax were determined by the time-dependent DFT (TD-DFT) method. The geometrical parameters, vibrational frequencies and absorption wavelengths were compared with the experimental data. The complete vibrational assignments are performed on the basis of the potential energy distributions (PED) of the vibrational modes in terms of natural internal coordinates. The simulated FT-IR, FT-Raman, and UV spectra of the title compound have been constructed. Molecular docking studies have been carried out in the active site of piracetam by using Argus Lab. In addition, the potential energy surface, HOMO and LUMO energies, first-order hyperpolarizability and the molecular electrostatic potential have been computed.

  20. Hyperon puzzle: hints from quantum Monte Carlo calculations.

    PubMed

    Lonardoni, Diego; Lovato, Alessandro; Gandolfi, Stefano; Pederiva, Francesco

    2015-03-06

    The onset of hyperons in the core of neutron stars and the consequent softening of the equation of state have been questioned for a long time. Controversial theoretical predictions and recent astrophysical observations of neutron stars are the grounds for the so-called hyperon puzzle. We calculate the equation of state and the neutron star mass-radius relation of an infinite systems of neutrons and Λ particles by using the auxiliary field diffusion Monte Carlo algorithm. We find that the three-body hyperon-nucleon interaction plays a fundamental role in the softening of the equation of state and for the consequent reduction of the predicted maximum mass. We have considered two different models of three-body force that successfully describe the binding energy of medium mass hypernuclei. Our results indicate that they give dramatically different results on the maximum mass of neutron stars, not necessarily incompatible with the recent observation of very massive neutron stars. We conclude that stronger constraints on the hyperon-neutron force are necessary in order to properly assess the role of hyperons in neutron stars.