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

PubMed

Yilmazer, Nusret Duygu; Korth, Martin

2016-05-16

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

Density functional theory and an experimentally-designed energy functional of electron density.

PubMed

Miranda, David A; Bueno, Paulo R

2016-09-21

We herein demonstrate that capacitance spectroscopy (CS) experimentally allows access to the energy associated with the quantum mechanical ground state of many-electron systems. Priorly, electrochemical capacitance, C [small mu, Greek, macron] [ρ], was previously understood from conceptual and computational density functional theory (DFT) calculations. Thus, we herein propose a quantum mechanical experiment-based variational method for electron charging processes based on an experimentally-designed functional of the ground state electron density. In this methodology, the electron state density, ρ, and an energy functional of the electron density, E [small mu, Greek, macron] [ρ], can be obtained from CS data. CS allows the derivative of the electrochemical potential with respect to the electron density, (δ[small mu, Greek, macron][ρ]/δρ), to be obtained as a unique functional of the energetically minimised system, i.e., β/C [small mu, Greek, macron] [ρ], where β is a constant (associated with the size of the system) and C [small mu, Greek, macron] [ρ] is an experimentally observable quantity. Thus the ground state energy (at a given fixed external potential) can be obtained simply as E [small mu, Greek, macron] [ρ], from the experimental measurement of C [small mu, Greek, macron] [ρ]. An experimental data-set was interpreted to demonstrate the potential of this quantum mechanical experiment-based variational principle.

Dielectric properties of classical and quantized ionic fluids.

PubMed

Høye, Johan S

2010-06-01

We study time-dependent correlation functions of classical and quantum gases using methods of equilibrium statistical mechanics for systems of uniform as well as nonuniform densities. The basis for our approach is the path integral formalism of quantum mechanical systems. With this approach the statistical mechanics of a quantum mechanical system becomes the equivalent of a classical polymer problem in four dimensions where imaginary time is the fourth dimension. Several nontrivial results for quantum systems have been obtained earlier by this analogy. Here, we will focus upon the presence of a time-dependent electromagnetic pair interaction where the electromagnetic vector potential that depends upon currents, will be present. Thus both density and current correlations are needed to evaluate the influence of this interaction. Then we utilize that densities and currents can be expressed by polarizations by which the ionic fluid can be regarded as a dielectric one for which a nonlocal susceptibility is found. This nonlocality has as a consequence that we find no contribution from a possible transverse electric zero-frequency mode for the Casimir force between metallic plates. Further, we establish expressions for a leading correction to ab initio calculations for the energies of the quantized electrons of molecules where now retardation effects also are taken into account.

Multicomponent Time-Dependent Density Functional Theory: Proton and Electron Excitation Energies.

PubMed

Yang, Yang; Culpitt, Tanner; Hammes-Schiffer, Sharon

2018-04-05

The quantum mechanical treatment of both electrons and protons in the calculation of excited state properties is critical for describing nonadiabatic processes such as photoinduced proton-coupled electron transfer. Multicomponent density functional theory enables the consistent quantum mechanical treatment of more than one type of particle and has been implemented previously for studying ground state molecular properties within the nuclear-electronic orbital (NEO) framework, where all electrons and specified protons are treated quantum mechanically. To enable the study of excited state molecular properties, herein the linear response multicomponent time-dependent density functional theory (TDDFT) is derived and implemented within the NEO framework. Initial applications to FHF - and HCN illustrate that NEO-TDDFT provides accurate proton and electron excitation energies within a single calculation. As its computational cost is similar to that of conventional electronic TDDFT, the NEO-TDDFT approach is promising for diverse applications, particularly nonadiabatic proton transfer reactions, which may exhibit mixed electron-proton vibronic excitations.

Formation of uniform high-density and small-size Ge/Si quantum dots by scanning pulsed laser annealing of pre-deposited Ge/Si film

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

Qayyum, Hamza; Chen, Szu-yuan, E-mail: sychen@ltl.iams.sinica.edu.tw; Department of Physics, National Central University, Zhongli, Taoyuan 320, Taiwan

2016-05-15

The capability to fabricate Ge/Si quantum dots with small dot size and high dot density uniformly over a large area is crucial for many applications. In this work, we demonstrate that this can be achieved by scanning a pre-deposited Ge thin layer on Si substrate with a line-focused pulsed laser beam to induce formation of quantum dots. With suitable setting, Ge/Si quantum dots with a mean height of 2.9 nm, a mean diameter of 25 nm, and a dot density of 6×10{sup 10} cm{sup −2} could be formed over an area larger than 4 mm{sup 2}. The average size ofmore » the laser-induced quantum dots is smaller while their density is higher than that of quantum dots grown by using Stranski-Krastanov growth mode. Based on the dependence of the characteristics of quantum dots on the laser parameters, a model consisting of laser-induced strain, surface diffusion, and Ostwald ripening is proposed for the mechanism underlying the formation of the Ge/Si quantum dots. The technique demonstrated could be applicable to other materials besides Ge/Si.« less

Quantum dynamics of a two-atom-qubit system

NASA Astrophysics Data System (ADS)

Van Hieu, Nguyen; Bich Ha, Nguyen; Linh, Le Thi Ha

2009-09-01

A physical model of the quantum information exchange between two qubits is studied theoretically. The qubits are two identical two-level atoms, the physical mechanism of the quantum information exchange is the mutual dependence of the reduced density matrices of two qubits generated by their couplings with a multimode radiation field. The Lehmberg-Agarwal master equation is exactly solved. The explicit form of the mutual dependence of two reduced density matrices is established. The application to study the entanglement of two qubits is discussed.

Density matrix Monte Carlo modeling of quantum cascade lasers

NASA Astrophysics Data System (ADS)

Jirauschek, Christian

2017-10-01

By including elements of the density matrix formalism, the semiclassical ensemble Monte Carlo method for carrier transport is extended to incorporate incoherent tunneling, known to play an important role in quantum cascade lasers (QCLs). In particular, this effect dominates electron transport across thick injection barriers, which are frequently used in terahertz QCL designs. A self-consistent model for quantum mechanical dephasing is implemented, eliminating the need for empirical simulation parameters. Our modeling approach is validated against available experimental data for different types of terahertz QCL designs.

Theoretical Characterization of the Spectral Density of the Water-Soluble Chlorophyll-Binding Protein from Combined Quantum Mechanics/Molecular Mechanics Molecular Dynamics Simulations.

PubMed

Rosnik, Andreana M; Curutchet, Carles

2015-12-08

Over the past decade, both experimentalists and theorists have worked to develop methods to describe pigment-protein coupling in photosynthetic light-harvesting complexes in order to understand the molecular basis of quantum coherence effects observed in photosynthesis. Here we present an improved strategy based on the combination of quantum mechanics/molecular mechanics (QM/MM) molecular dynamics (MD) simulations and excited-state calculations to predict the spectral density of electronic-vibrational coupling. We study the water-soluble chlorophyll-binding protein (WSCP) reconstituted with Chl a or Chl b pigments as the system of interest and compare our work with data obtained by Pieper and co-workers from differential fluorescence line-narrowing spectra (Pieper et al. J. Phys. Chem. B 2011, 115 (14), 4042-4052). Our results demonstrate that the use of QM/MM MD simulations where the nuclear positions are still propagated at the classical level leads to a striking improvement of the predicted spectral densities in the middle- and high-frequency regions, where they nearly reach quantitative accuracy. This demonstrates that the so-called "geometry mismatch" problem related to the use of low-quality structures in QM calculations, not the quantum features of pigments high-frequency motions, causes the failure of previous studies relying on similar protocols. Thus, this work paves the way toward quantitative predictions of pigment-protein coupling and the comprehension of quantum coherence effects in photosynthesis.

Quantum measurement-induced antiferromagnetic order and density modulations in ultracold Fermi gases in optical lattices

NASA Astrophysics Data System (ADS)

Mazzucchi, Gabriel; Caballero-Benitez, Santiago F.; Mekhov, Igor B.

2016-08-01

Ultracold atomic systems offer a unique tool for understanding behavior of matter in the quantum degenerate regime, promising studies of a vast range of phenomena covering many disciplines from condensed matter to quantum information and particle physics. Coupling these systems to quantized light fields opens further possibilities of observing delicate effects typical of quantum optics in the context of strongly correlated systems. Measurement backaction is one of the most funda- mental manifestations of quantum mechanics and it is at the core of many famous quantum optics experiments. Here we show that quantum backaction of weak measurement can be used for tailoring long-range correlations of ultracold fermions, realizing quantum states with spatial modulations of the density and magnetization, thus overcoming usual requirement for a strong interatomic interactions. We propose detection schemes for implementing antiferromagnetic states and density waves. We demonstrate that such long-range correlations cannot be realized with local addressing, and they are a consequence of the competition between global but spatially structured backaction of weak quantum measurement and unitary dynamics of fermions.

Scattering mechanisms in shallow undoped Si/SiGe quantum wells

DOE PAGES

Laroche, Dominique; Huang, S. -H.; Nielsen, Erik; ...

2015-10-07

We report the magneto-transport study and scattering mechanism analysis of a series of increasingly shallow Si/SiGe quantum wells with depth ranging from ~ 100 nm to ~ 10 nm away from the heterostructure surface. The peak mobility increases with depth, suggesting that charge centers near the oxide/semiconductor interface are the dominant scattering source. The power-law exponent of the electron mobility versus density curve, μ ∝ n α, is extracted as a function of the depth of the Si quantum well. At intermediate densities, the power-law dependence is characterized by α ~ 2.3. At the highest achievable densities in the quantummore » wells buried at intermediate depth, an exponent α ~ 5 is observed. Lastly, we propose and show by simulations that this increase in the mobility dependence on the density can be explained by a non-equilibrium model where trapped electrons smooth out the potential landscape seen by the two-dimensional electron gas.« less

Nine formulations of quantum mechanics

NASA Astrophysics Data System (ADS)

Styer, Daniel F.; Balkin, Miranda S.; Becker, Kathryn M.; Burns, Matthew R.; Dudley, Christopher E.; Forth, Scott T.; Gaumer, Jeremy S.; Kramer, Mark A.; Oertel, David C.; Park, Leonard H.; Rinkoski, Marie T.; Smith, Clait T.; Wotherspoon, Timothy D.

2002-03-01

Nine formulations of nonrelativistic quantum mechanics are reviewed. These are the wavefunction, matrix, path integral, phase space, density matrix, second quantization, variational, pilot wave, and Hamilton-Jacobi formulations. Also mentioned are the many-worlds and transactional interpretations. The various formulations differ dramatically in mathematical and conceptual overview, yet each one makes identical predictions for all experimental results.

Spiers Memorial Lecture. Quantum chemistry: the first seventy years.

PubMed

McWeeny, Roy

2007-01-01

Present-day theoretical chemistry is rooted in Quantum Mechanics. The aim of the opening lecture is to trace the evolution of Quantum Chemistry from the Heitler-London paper of 1927 up to the end of the last century, emphasizing concepts rather than calculations. The importance of symmetry concepts became evident in the early years: one thinks of the necessary anti-symmetry of the wave function under electron permutations, the Pauli principle, the aufbau scheme, and the classification of spectroscopic states. But for chemists perhaps the key concept is embodied in the Hellmann-Feynman theorem, which provides a pictorial interpretation of chemical bonding in terms of classical electrostatic forces exerted on the nuclei by the electron distribution. Much of the lecture is concerned with various electron distribution functions--the electron density, the current density, the spin density, and other 'property densities'--and with their use in interpreting both molecular structure and molecular properties. Other topics touched upon include Response theory and propagators; Chemical groups in molecules and the group function approach; Atoms in molecules and Bader's theory; Electron correlation and the 'pair function'. Finally, some long-standing controversies, in particular the EPR paradox, are re-examined in the context of molecular dissociation. By admitting the concept of symmetry breaking, along with the use of the von Neumann-Dirac statistical ensemble, orthodox quantum mechanics can lead to a convincing picture of the dissociation mechanism.

Quantum formalism for classical statistics

NASA Astrophysics Data System (ADS)

Wetterich, C.

2018-06-01

In static classical statistical systems the problem of information transport from a boundary to the bulk finds a simple description in terms of wave functions or density matrices. While the transfer matrix formalism is a type of Heisenberg picture for this problem, we develop here the associated Schrödinger picture that keeps track of the local probabilistic information. The transport of the probabilistic information between neighboring hypersurfaces obeys a linear evolution equation, and therefore the superposition principle for the possible solutions. Operators are associated to local observables, with rules for the computation of expectation values similar to quantum mechanics. We discuss how non-commutativity naturally arises in this setting. Also other features characteristic of quantum mechanics, such as complex structure, change of basis or symmetry transformations, can be found in classical statistics once formulated in terms of wave functions or density matrices. We construct for every quantum system an equivalent classical statistical system, such that time in quantum mechanics corresponds to the location of hypersurfaces in the classical probabilistic ensemble. For suitable choices of local observables in the classical statistical system one can, in principle, compute all expectation values and correlations of observables in the quantum system from the local probabilistic information of the associated classical statistical system. Realizing a static memory material as a quantum simulator for a given quantum system is not a matter of principle, but rather of practical simplicity.

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

PubMed

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

2017-08-03

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

Quantum mechanical probability current as electromagnetic 4-current from topological EM fields

NASA Astrophysics Data System (ADS)

van der Mark, Martin B.

2015-09-01

Starting from a complex 4-potential A = αdβ we show that the 4-current density in electromagnetism and the probability current density in relativistic quantum mechanics are of identical form. With the Dirac-Clifford algebra Cl1,3 as mathematical basis, the given 4-potential allows topological solutions of the fields, quite similar to Bateman's construction, but with a double field solution that was overlooked previously. A more general nullvector condition is found and wave-functions of charged and neutral particles appear as topological configurations of the electromagnetic fields.

Spin-polarization dependent carrier recombination dynamics and spin relaxation mechanism in asymmetrically doped (110) n-GaAs quantum wells

NASA Astrophysics Data System (ADS)

Teng, Lihua; Jiang, Tianran; Wang, Xia; Lai, Tianshu

2018-05-01

Carrier recombination and electron spin relaxation dynamics in asymmetric n-doped (110) GaAs/AlGaAs quantum wells are investigated with time-resolved pump-probe spectroscopy. The experiment results reveal that the measured carrier recombination time depends strongly on the polarization of pump pulse. With the same pump photon flux densities, the recombination time of spin-polarized carriers is always longer than that of the spin-balanced carriers except at low pump photon flux densities, this anomaly originates from the polarization-sensitive nonlinear absorption effect. Differing from the traditional views, in the low carrier density regime, the D'yakonov-Perel' (DP) mechanism can be more important than the Bir-Aronov-Pikus (BAP) mechanism, since the DP mechanism takes effect, the spin relaxation time in (110) GaAs QWs is shortened obviously via asymmetric doping.

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

NASA Astrophysics Data System (ADS)

Soirat, Arnaud J. A.

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

Transport in semiconductor nanowire superlattices described by coupled quantum mechanical and kinetic models.

PubMed

Alvaro, M; Bonilla, L L; Carretero, M; Melnik, R V N; Prabhakar, S

2013-08-21

In this paper we develop a kinetic model for the analysis of semiconductor superlattices, accounting for quantum effects. The model consists of a Boltzmann-Poisson type system of equations with simplified Bhatnagar-Gross-Krook collisions, obtained from the general time-dependent Schrödinger-Poisson model using Wigner functions. This system for superlattice transport is supplemented by the quantum mechanical part of the model based on the Ben-Daniel-Duke form of the Schrödinger equation for a cylindrical superlattice of finite radius. The resulting energy spectrum is used to characterize the Fermi-Dirac distribution that appears in the Bhatnagar-Gross-Krook collision, thereby coupling the quantum mechanical and kinetic parts of the model. The kinetic model uses the dispersion relation obtained by the generalized Kronig-Penney method, and allows us to estimate radii of quantum wire superlattices that have the same miniband widths as in experiments. It also allows us to determine more accurately the time-dependent characteristics of superlattices, in particular their current density. Results, for several experimentally grown superlattices, are discussed in the context of self-sustained coherent oscillations of the current density which are important in an increasing range of current and potential applications.

Sampling Molecular Conformers in Solution with Quantum Mechanical Accuracy at a Nearly Molecular-Mechanics Cost.

PubMed

Rosa, Marta; Micciarelli, Marco; Laio, Alessandro; Baroni, Stefano

2016-09-13

We introduce a method to evaluate the relative populations of different conformers of molecular species in solution, aiming at quantum mechanical accuracy, while keeping the computational cost at a nearly molecular-mechanics level. This goal is achieved by combining long classical molecular-dynamics simulations to sample the free-energy landscape of the system, advanced clustering techniques to identify the most relevant conformers, and thermodynamic perturbation theory to correct the resulting populations, using quantum-mechanical energies from density functional theory. A quantitative criterion for assessing the accuracy thus achieved is proposed. The resulting methodology is demonstrated in the specific case of cyanin (cyanidin-3-glucoside) in water solution.

Quantum-mechanical transport equation for atomic systems.

NASA Technical Reports Server (NTRS)

Berman, P. R.

1972-01-01

A quantum-mechanical transport equation (QMTE) is derived which should be applicable to a wide range of problems involving the interaction of radiation with atoms or molecules which are also subject to collisions with perturber atoms. The equation follows the time evolution of the macroscopic atomic density matrix elements of atoms located at classical position R and moving with classical velocity v. It is quantum mechanical in the sense that all collision kernels or rates which appear have been obtained from a quantum-mechanical theory and, as such, properly take into account the energy-level variations and velocity changes of the active (emitting or absorbing) atom produced in collisions with perturber atoms. The present formulation is better suited to problems involving high-intensity external fields, such as those encountered in laser physics.

Quantum plasmonics: optical properties of a nanomatryushka.

PubMed

Kulkarni, Vikram; Prodan, Emil; Nordlander, Peter

2013-01-01

Quantum mechanical effects can significantly reduce the plasmon-induced field enhancements around nanoparticles. Here we present a quantum mechanical investigation of the plasmon resonances in a nanomatryushka, which is a concentric core-shell nanoparticle consisting of a solid metallic core encapsulated in a thin metallic shell. We compute the optical response using the time-dependent density functional theory and compare the results with predictions based on the classical electromagnetic theory. We find strong quantum mechanical effects for core-shell spacings below 5 Å, a regime where both the absorption cross section and the local field enhancements differ significantly from the classical predictions. We also show that the workfunction of the metal is a crucial parameter determining the onset and magnitude of quantum effects. For metals with lower workfunctions such as aluminum, the quantum effects are found to be significantly more pronounced than for a noble metal such as gold.

Quantum Corrections to the 'Atomistic' MOSFET Simulations

NASA Technical Reports Server (NTRS)

Asenov, Asen; Slavcheva, G.; Kaya, S.; Balasubramaniam, R.

2000-01-01

We have introduced in a simple and efficient manner quantum mechanical corrections in our 3D 'atomistic' MOSFET simulator using the density gradient formalism. We have studied in comparison with classical simulations the effect of the quantum mechanical corrections on the simulation of random dopant induced threshold voltage fluctuations, the effect of the single charge trapping on interface states and the effect of the oxide thickness fluctuations in decanano MOSFETs with ultrathin gate oxides. The introduction of quantum corrections enhances the threshold voltage fluctuations but does not affect significantly the amplitude of the random telegraph noise associated with single carrier trapping. The importance of the quantum corrections for proper simulation of oxide thickness fluctuation effects has also been demonstrated.

Influence of Force Fields and Quantum Chemistry Approach on Spectral Densities of BChl a in Solution and in FMO Proteins

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

Chandrasekaran, Suryanarayanan; Aghtar, Mortaza; Valleau, Stéphanie

2015-08-06

Studies on light-harvesting (LH) systems have attracted much attention after the finding of long-lived quantum coherences in the exciton dynamics of the Fenna–Matthews–Olson (FMO) complex. In this complex, excitation energy transfer occurs between the bacteriochlorophyll a (BChl a) pigments. Two quantum mechanics/molecular mechanics (QM/MM) studies, each with a different force-field and quantum chemistry approach, reported different excitation energy distributions for the FMO complex. To understand the reasons for these differences in the predicted excitation energies, we have carried out a comparative study between the simulations using the CHARMM and AMBER force field and the Zerner intermediate neglect of differential orbitalmore » (ZINDO)/S and time-dependent density functional theory (TDDFT) quantum chemistry methods. The calculations using the CHARMM force field together with ZINDO/S or TDDFT always show a wider spread in the energy distribution compared to those using the AMBER force field. High- or low-energy tails in these energy distributions result in larger values for the spectral density at low frequencies. A detailed study on individual BChl a molecules in solution shows that without the environment, the density of states is the same for both force field sets. Including the environmental point charges, however, the excitation energy distribution gets broader and, depending on the applied methods, also asymmetric. The excitation energy distribution predicted using TDDFT together with the AMBER force field shows a symmetric, Gaussian-like distribution.« less

Molecular dynamics simulations of dense plasmas

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

Collins, L.A.; Kress, J.D.; Kwon, I.

1993-12-31

We have performed quantum molecular dynamics simulations of hot, dense plasmas of hydrogen over a range of temperatures(0.1-5eV) and densities(0.0625-5g/cc). We determine the forces quantum mechanically from density functional, extended Huckel, and tight binding techniques and move the nuclei according to the classical equations of motion. We determine pair-correlation functions, diffusion coefficients, and electrical conductivities. We find that many-body effects predominate in this regime. We begin to obtain agreement with the OCP and Thomas-Fermi models only at the higher temperatures and densities.

Recombination dynamics in In{sub x}Ga{sub 1−x}N quantum wells—Contribution of excited subband recombination to carrier leakage

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

Schulz, T.; Markurt, T.; Albrecht, M.

2014-11-03

The recombination dynamics of In{sub x}Ga{sub 1−x}N single quantum wells are investigated. By comparing the photoluminescence (PL) decay spectra with simulated emission spectra obtained by a Schrödinger-Poisson approach, we give evidence that recombination from higher subbands contributes the emission of the quantum well at high excitation densities. This recombination path appears as a shoulder on the high energy side of the spectrum at high charge carrier densities and exhibits decay in the range of ps. Due to the lower confinement of the excited subband states, a distinct proportion of the probability density function lies outside the quantum well, thus contributingmore » to charge carrier loss. By estimating the current density in our time resolved PL experiments, we show that the onset of this loss mechanism occurs in the droop relevant regime above 20 A/cm{sup 2}.« less

Density-Dependent Formulation of Dispersion-Repulsion Interactions in Hybrid Multiscale Quantum/Molecular Mechanics (QM/MM) Models.

PubMed

Curutchet, Carles; Cupellini, Lorenzo; Kongsted, Jacob; Corni, Stefano; Frediani, Luca; Steindal, Arnfinn Hykkerud; Guido, Ciro A; Scalmani, Giovanni; Mennucci, Benedetta

2018-03-13

Mixed multiscale quantum/molecular mechanics (QM/MM) models are widely used to explore the structure, reactivity, and electronic properties of complex chemical systems. Whereas such models typically include electrostatics and potentially polarization in so-called electrostatic and polarizable embedding approaches, respectively, nonelectrostatic dispersion and repulsion interactions are instead commonly described through classical potentials despite their quantum mechanical origin. Here we present an extension of the Tkatchenko-Scheffler semiempirical van der Waals (vdW TS ) scheme aimed at describing dispersion and repulsion interactions between quantum and classical regions within a QM/MM polarizable embedding framework. Starting from the vdW TS expression, we define a dispersion and a repulsion term, both of them density-dependent and consistently based on a Lennard-Jones-like potential. We explore transferable atom type-based parametrization strategies for the MM parameters, based on either vdW TS calculations performed on isolated fragments or on a direct estimation of the parameters from atomic polarizabilities taken from a polarizable force field. We investigate the performance of the implementation by computing self-consistent interaction energies for the S22 benchmark set, designed to represent typical noncovalent interactions in biological systems, in both equilibrium and out-of-equilibrium geometries. Overall, our results suggest that the present implementation is a promising strategy to include dispersion and repulsion in multiscale QM/MM models incorporating their explicit dependence on the electronic density.

A Note on the Propagation of Quantized Vortex Rings Through a Quantum Turbulence Tangle: Energy Transport or Energy Dissipation?

NASA Astrophysics Data System (ADS)

Laurie, Jason; Baggaley, Andrew W.

2015-07-01

We investigate quantum vortex ring dynamics at scales smaller than the inter-vortex spacing in quantum turbulence. Through geometrical arguments and high-resolution numerical simulations, we examine the validity of simple estimates for the mean free path and the structure of vortex rings post-reconnection. We find that a large proportion of vortex rings remain coherent objects where approximately of their energy is preserved. This leads us to consider the effectiveness of energy transport in turbulent tangles. Moreover, we show that in low density tangles, appropriate for the ultra-quantum regime, ring emission cannot be ruled out as an important mechanism for energy dissipation. However at higher vortex line densities, typically associated with the quasi-classical regime, loop emission is expected to make a negligible contribution to energy dissipation, even allowing for the fact that our work shows rings can survive multiple reconnection events. Hence the Kelvin wave cascade seems the most plausible mechanism leading to energy dissipation.

On the Conformable Fractional Quantum Mechanics

NASA Astrophysics Data System (ADS)

Mozaffari, F. S.; Hassanabadi, H.; Sobhani, H.; Chung, W. S.

2018-05-01

In this paper, a conformable fractional quantum mechanic has been introduced using three postulates. Then in such a formalism, Schr¨odinger equation, probability density, probability flux and continuity equation have been derived. As an application of considered formalism, a fractional-radial harmonic oscillator has been considered. After obtaining its wave function and energy spectrum, effects of the conformable fractional parameter on some quantities have been investigated and plotted for different excited states.

Classical-Quantum Correspondence by Means of Probability Densities

NASA Technical Reports Server (NTRS)

Vegas, Gabino Torres; Morales-Guzman, J. D.

1996-01-01

Within the frame of the recently introduced phase space representation of non relativistic quantum mechanics, we propose a Lagrangian from which the phase space Schrodinger equation can be derived. From that Lagrangian, the associated conservation equations, according to Noether's theorem, are obtained. This shows that one can analyze quantum systems completely in phase space as it is done in coordinate space, without additional complications.

Quantum Mechanical Enhancement of the Random Dopant Induced Threshold Voltage Fluctuations and Lowering in Sub 0.1 Micron MOSFETs

NASA Technical Reports Server (NTRS)

Asenov, Asen; Slavcheva, G.; Brown, A. R.; Davies, J. H.; Saini, Subhash

1999-01-01

A detailed study of the influence of quantum effects in the inversion layer on the random dopant induced threshold voltage fluctuations and lowering in sub 0.1 micron MOSFETs has been performed. This has been achieved using a full 3D implementation of the density gradient (DG) formalism incorporated in our previously published 3D 'atomistic' simulation approach. This results in a consistent, fully 3D, quantum mechanical picture which implies not only the vertical inversion layer quantisation but also the lateral confinement effects manifested by current filamentation in the 'valleys' of the random potential fluctuations. We have shown that the net result of including quantum mechanical effects, while considering statistical fluctuations, is an increase in both threshold voltage fluctuations and lowering.

Cosmological implications of the transition from the false vacuum to the true vacuum state

NASA Astrophysics Data System (ADS)

Stachowski, Aleksander; Szydłowski, Marek; Urbanowski, Krzysztof

2017-06-01

We study cosmology with running dark energy. The energy density of dark energy is obtained from the quantum process of transition from the false vacuum state to the true vacuum state. We use the Breit-Wigner energy distribution function to model the quantum unstable systems and obtain the energy density of the dark energy parametrization ρ _ {de}(t). We also use Krauss and Dent's idea linking properties of the quantum mechanical decay of unstable states with the properties of the observed Universe. In the cosmological model with this parametrization there is an energy transfer between dark matter and dark energy. The intensity of this process, measured by a parameter α , distinguishes two scenarios. As the Universe starts from the false vacuum state, for the small value of α (0<α <0.4) it goes through an intermediate oscillatory (quantum) regime of the density of dark energy, while for α > 0.4 the density of the dark energy jumps down. In both cases the present value of the density of dark energy is reached. From a statistical analysis we find this model to be in good agreement with the astronomical data and practically indistinguishable from the Λ CDM model.

Stochastic mechanics of reciprocal diffusions

NASA Astrophysics Data System (ADS)

Levy, Bernard C.; Krener, Arthur J.

1996-02-01

The dynamics and kinematics of reciprocal diffusions were examined in a previous paper [J. Math. Phys. 34, 1846 (1993)], where it was shown that reciprocal diffusions admit a chain of conservation laws, which close after the first two laws for two disjoint subclasses of reciprocal diffusions, the Markov and quantum diffusions. For the case of quantum diffusions, the conservation laws are equivalent to Schrödinger's equation. The Markov diffusions were employed by Schrödinger [Sitzungsber. Preuss. Akad. Wiss. Phys. Math Kl. 144 (1931); Ann. Inst. H. Poincaré 2, 269 (1932)], Nelson [Dynamical Theories of Brownian Motion (Princeton University, Princeton, NJ, 1967); Quantum Fluctuations (Princeton University, Princeton, NJ, 1985)], and other researchers to develop stochastic formulations of quantum mechanics, called stochastic mechanics. We propose here an alternative version of stochastic mechanics based on quantum diffusions. A procedure is presented for constructing the quantum diffusion associated to a given wave function. It is shown that quantum diffusions satisfy the uncertainty principle, and have a locality property, whereby given two dynamically uncoupled but statistically correlated particles, the marginal statistics of each particle depend only on the local fields to which the particle is subjected. However, like Wigner's joint probability distribution for the position and momentum of a particle, the finite joint probability densities of quantum diffusions may take negative values.

On the possibility of many-body localization in a doped Mott insulator

PubMed Central

He, Rong-Qiang; Weng, Zheng-Yu

2016-01-01

Many-body localization (MBL) is currently a hot issue of interacting systems, in which quantum mechanics overcomes thermalization of statistical mechanics. Like Anderson localization of non-interacting electrons, disorders are usually crucial in engineering the quantum interference in MBL. For translation invariant systems, however, the breakdown of eigenstate thermalization hypothesis due to a pure many-body quantum effect is still unclear. Here we demonstrate a possible MBL phenomenon without disorder, which emerges in a lightly doped Hubbard model with very strong interaction. By means of density matrix renormalization group numerical calculation on a two-leg ladder, we show that whereas a single hole can induce a very heavy Nagaoka polaron, two or more holes will form bound pair/droplets which are all localized excitations with flat bands at low energy densities. Consequently, MBL eigenstates of finite energy density can be constructed as composed of these localized droplets spatially separated. We further identify the underlying mechanism for this MBL as due to a novel ‘Berry phase’ of the doped Mott insulator, and show that by turning off this Berry phase either by increasing the anisotropy of the model or by hand, an eigenstate transition from the MBL to a conventional quasiparticle phase can be realized. PMID:27752064

Atom Tunneling in the Hydroxylation Process of Taurine/α-Ketoglutarate Dioxygenase Identified by Quantum Mechanics/Molecular Mechanics Simulations.

PubMed

Álvarez-Barcia, Sonia; Kästner, Johannes

2017-06-01

Taurine/α-ketoglutarate dioxygenase is one of the most studied α-ketoglutarate-dependent dioxygenases (αKGDs), involved in several biotechnological applications. We investigated the key step in the catalytic cycle of the αKGDs, the hydrogen transfer process, by a quantum mechanics/molecular mechanics approach (B3LYP/CHARMM22). Analysis of the charge and spin densities during the reaction demonstrates that a concerted mechanism takes place, where the H atom transfer happens simultaneously with the electron transfer from taurine to the Fe═O cofactor. We found the quantum tunneling of the hydrogen atom to increase the rate constant by a factor of 40 at 5 °C. As a consequence, a quite high kinetic isotope effect close to 60 is obtained, which is consistent with the experimental value.

Entangled quantum electronic wavefunctions of the Mn₄CaO₅ cluster in photosystem II.

PubMed

Kurashige, Yuki; Chan, Garnet Kin-Lic; Yanai, Takeshi

2013-08-01

It is a long-standing goal to understand the reaction mechanisms of catalytic metalloenzymes at an entangled many-electron level, but this is hampered by the exponential complexity of quantum mechanics. Here, by exploiting the special structure of physical quantum states and using the density matrix renormalization group, we compute near-exact many-electron wavefunctions of the Mn4CaO5 cluster of photosystem II, with more than 1 × 10(18) quantum degrees of freedom. This is the first treatment of photosystem II beyond the single-electron picture of density functional theory. Our calculations support recent modifications to the structure determined by X-ray crystallography. We further identify multiple low-lying energy surfaces associated with the structural distortion seen using X-ray crystallography, highlighting multistate reactivity in the chemistry of the cluster. Direct determination of Mn spin-projections from our wavefunctions suggests that current candidates that have been recently distinguished using parameterized spin models should be reassessed. Through entanglement maps, we reveal rich information contained in the wavefunctions on bonding changes in the cycle.

Nonrelativistic Quantum Mechanics with Fundamental Environment

NASA Astrophysics Data System (ADS)

Gevorkyan, Ashot S.

2011-03-01

Spontaneous transitions between bound states of an atomic system, "Lamb Shift" of energy levels and many other phenomena in real nonrelativistic quantum systems are connected within the influence of the quantum vacuum fluctuations ( fundamental environment (FE)) which are impossible to consider in the limits of standard quantum-mechanical approaches. The joint system "quantum system (QS) + FE" is described in the framework of the stochastic differential equation (SDE) of Langevin-Schrödinger (L-Sch) type, and is defined on the extended space R 3 ⊗ R { ξ}, where R 3 and R { ξ} are the Euclidean and functional spaces, respectively. The density matrix for single QS in FE is defined. The entropy of QS entangled with FE is defined and investigated in detail. It is proved that as a result of interaction of QS with environment there arise structures of various topologies which are a new quantum property of the system.

Quantum Dynamics in Biological Systems

NASA Astrophysics Data System (ADS)

Shim, Sangwoo

In the first part of this dissertation, recent efforts to understand quantum mechanical effects in biological systems are discussed. Especially, long-lived quantum coherences observed during the electronic energy transfer process in the Fenna-Matthews-Olson complex at physiological condition are studied extensively using theories of open quantum systems. In addition to the usual master equation based approaches, the effect of the protein structure is investigated in atomistic detail through the combined application of quantum chemistry and molecular dynamics simulations. To evaluate the thermalized reduced density matrix, a path-integral Monte Carlo method with a novel importance sampling approach is developed for excitons coupled to an arbitrary phonon bath at a finite temperature. In the second part of the thesis, simulations of molecular systems and applications to vibrational spectra are discussed. First, the quantum dynamics of a molecule is simulated by combining semiclassical initial value representation and density funcitonal theory with analytic derivatives. A computationally-tractable approximation to the sum-of-states formalism of Raman spectra is subsequently discussed.

Electroluminescence from ZnCuInS/ZnS quantum dots/poly(9-vinylcarbazole) multilayer films with different thicknesses of quantum dot layer

NASA Astrophysics Data System (ADS)

Dong, Xiaofei; Xu, Jianping; Shi, Shaobo; Zhang, Xiaosong; Li, Lan; Yin, Shougen

2017-05-01

We report tunable electroluminescence (EL) from solution-processed ZnCuInS/ZnS (ZCIS/ZnS) quantum dots (QDs)/poly(9-vinlycarbazole) multilayer films. The EL spectra exhibit a red shift as the QD layer thickness increases. By analyzing the dependence of the applied voltage and the ZCIS/ZnS QD layer thickness on the EL spectra, the origin of the red shift is associated with the increased trap density of QDs that induces the injected electrons to be trapped in the deep donor level. The current conduction mechanism based on the current density-voltage curves at different voltage regions was discussed.

Density effects on electronic configurations in dense plasmas

NASA Astrophysics Data System (ADS)

Faussurier, Gérald; Blancard, Christophe

2018-02-01

We present a quantum mechanical model to describe the density effects on electronic configurations inside a plasma environment. Two different approaches are given by starting from a quantum average-atom model. Illustrations are shown for an aluminum plasma in local thermodynamic equilibrium at solid density and at a temperature of 100 eV and in the thermodynamic conditions of a recent experiment designed to characterize the effects of the ionization potential depression treatment. Our approach compares well with experiment and is consistent in that case with the approach of Stewart and Pyatt to describe the ionization potential depression rather than with the method of Ecker and Kröll.

Solvation of fluoro-acetonitrile in water by 2D-IR spectroscopy: A combined experimental-computational study

NASA Astrophysics Data System (ADS)

Cazade, Pierre-André; Tran, Halina; Bereau, Tristan; Das, Akshaya K.; Kläsi, Felix; Hamm, Peter; Meuwly, Markus

2015-06-01

The solvent dynamics around fluorinated acetonitrile is characterized by 2-dimensional infrared spectroscopy and atomistic simulations. The lineshape of the linear infrared spectrum is better captured by semiempirical (density functional tight binding) mixed quantum mechanical/molecular mechanics simulations, whereas force field simulations with multipolar interactions yield lineshapes that are significantly too narrow. For the solvent dynamics, a relatively slow time scale of 2 ps is found from the experiments and supported by the mixed quantum mechanical/molecular mechanics simulations. With multipolar force fields fitted to the available thermodynamical data, the time scale is considerably faster—on the 0.5 ps time scale. The simulations provide evidence for a well established CF-HOH hydrogen bond (population of 25%) which is found from the radial distribution function g(r) from both, force field and quantum mechanics/molecular mechanics simulations.

Diffuse Surface Scattering in the Plasmonic Resonances of Ultralow Electron Density Nanospheres.

PubMed

Monreal, R Carmina; Antosiewicz, Tomasz J; Apell, S Peter

2015-05-21

Localized surface plasmon resonances (LSPRs) have recently been identified in extremely diluted electron systems obtained by doping semiconductor quantum dots. Here, we investigate the role that different surface effects, namely, electronic spill-out and diffuse surface scattering, play in the optical properties of these ultralow electron density nanosystems. Diffuse scattering originates from imperfections or roughness at a microscopic scale on the surface. Using an electromagnetic theory that describes this mechanism in conjunction with a dielectric function including the quantum size effect, we find that the LSPRs show an oscillatory behavior in both position and width for large particles and a strong blue shift in energy and an increased width for smaller radii, consistent with recent experimental results for photodoped ZnO nanocrystals. We thus show that the commonly ignored process of diffuse surface scattering is a more important mechanism affecting the plasmonic properties of ultralow electron density nanoparticles than the spill-out effect.

Ab initio quantum chemistry: methodology and applications.

PubMed

Friesner, Richard A

2005-05-10

This Perspective provides an overview of state-of-the-art ab initio quantum chemical methodology and applications. The methods that are discussed include coupled cluster theory, localized second-order Moller-Plesset perturbation theory, multireference perturbation approaches, and density functional theory. The accuracy of each approach for key chemical properties is summarized, and the computational performance is analyzed, emphasizing significant advances in algorithms and implementation over the past decade. Incorporation of a condensed-phase environment by means of mixed quantum mechanical/molecular mechanics or self-consistent reaction field techniques, is presented. A wide range of illustrative applications, focusing on materials science and biology, are discussed briefly.

Quantum Stochastic Trajectories: The Fokker-Planck-Bohm Equation Driven by the Reduced Density Matrix.

PubMed

Avanzini, Francesco; Moro, Giorgio J

2018-03-15

The quantum molecular trajectory is the deterministic trajectory, arising from the Bohm theory, that describes the instantaneous positions of the nuclei of molecules by assuring the agreement with the predictions of quantum mechanics. Therefore, it provides the suitable framework for representing the geometry and the motions of molecules without neglecting their quantum nature. However, the quantum molecular trajectory is extremely demanding from the computational point of view, and this strongly limits its applications. To overcome such a drawback, we derive a stochastic representation of the quantum molecular trajectory, through projection operator techniques, for the degrees of freedom of an open quantum system. The resulting Fokker-Planck operator is parametrically dependent upon the reduced density matrix of the open system. Because of the pilot role played by the reduced density matrix, this stochastic approach is able to represent accurately the main features of the open system motions both at equilibrium and out of equilibrium with the environment. To verify this procedure, the predictions of the stochastic and deterministic representation are compared for a model system of six interacting harmonic oscillators, where one oscillator is taken as the open quantum system of interest. The undeniable advantage of the stochastic approach is that of providing a simplified and self-contained representation of the dynamics of the open system coordinates. Furthermore, it can be employed to study the out of equilibrium dynamics and the relaxation of quantum molecular motions during photoinduced processes, like photoinduced conformational changes and proton transfers.

Quantum States and Generalized Observables: A Simple Proof of Gleason's Theorem

NASA Astrophysics Data System (ADS)

Busch, P.

2003-09-01

A quantum state can be understood in a loose sense as a map that assigns a value to every observable. Formalizing this characterization of states in terms of generalized probability distributions on the set of effects, we obtain a simple proof of the result, analogous to Gleason’s theorem, that any quantum state is given by a density operator. As a corollary we obtain a vonNeumann type argument against noncontextual hidden variables. It follows that on an individual interpretation of quantum mechanics the values of effects are appropriately understood as propensities.

An investigation of student understanding of classical ideas related to quantum mechanics: Potential energy diagrams and spatial probability density

NASA Astrophysics Data System (ADS)

Stephanik, Brian Michael

This dissertation describes the results of two related investigations into introductory student understanding of ideas from classical physics that are key elements of quantum mechanics. One investigation probes the extent to which students are able to interpret and apply potential energy diagrams (i.e., graphs of potential energy versus position). The other probes the extent to which students are able to reason classically about probability and spatial probability density. The results of these investigations revealed significant conceptual and reasoning difficulties that students encounter with these topics. The findings guided the design of instructional materials to address the major problems. Results from post-instructional assessments are presented that illustrate the impact of the curricula on student learning.

Computational applications of the many-interacting-worlds interpretation of quantum mechanics.

PubMed

Sturniolo, Simone

2018-05-01

While historically many quantum-mechanical simulations of molecular dynamics have relied on the Born-Oppenheimer approximation to separate electronic and nuclear behavior, recently a great deal of interest has arisen in quantum effects in nuclear dynamics as well. Due to the computational difficulty of solving the Schrödinger equation in full, these effects are often treated with approximate methods. In this paper, we present an algorithm to tackle these problems using an extension to the many-interacting-worlds approach to quantum mechanics. This technique uses a kernel function to rebuild the probability density, and therefore, in contrast with the approximation presented in the original paper, it can be naturally extended to n-dimensional systems. This opens up the possibility of performing quantum ground-state searches with steepest-descent methods, and it could potentially lead to real-time quantum molecular-dynamics simulations. The behavior of the algorithm is studied in different potentials and numbers of dimensions and compared both to the original approach and to exact Schrödinger equation solutions whenever possible.

Teaching Chemistry with Electron Density Models.

ERIC Educational Resources Information Center

Shusterman, Gwendolyn P.; Shusterman, Alan J.

1997-01-01

Describes a method for teaching electronic structure and its relevance to chemical phenomena that relies on computer-generated three-dimensional models of electron density distributions. Discusses the quantum mechanical background needed and presents ways of using models of electronic ground states to teach electronic structure, bonding concepts,…

About Schrödinger Equation on Fractals Curves Imbedding in R 3

NASA Astrophysics Data System (ADS)

Golmankhaneh, Alireza Khalili; Golmankhaneh, Ali Khalili; Baleanu, Dumitru

2015-04-01

In this paper we introduced the quantum mechanics on fractal time-space. In a suggested formalism the time and space vary on Cantor-set and Von-Koch curve, respectively. Using Feynman path method in quantum mechanics and F α -calculus we find Schrëdinger equation on on fractal time-space. The Hamiltonian and momentum fractal operator has been indicated. More, the continuity equation and the probability density is given in view of F α -calculus.

Experimental Evidence for Quantum Interference and Vibrationally Induced Decoherence in Single-Molecule Junctions

NASA Astrophysics Data System (ADS)

Ballmann, Stefan; Härtle, Rainer; Coto, Pedro B.; Elbing, Mark; Mayor, Marcel; Bryce, Martin R.; Thoss, Michael; Weber, Heiko B.

2012-08-01

We analyze quantum interference and decoherence effects in single-molecule junctions both experimentally and theoretically by means of the mechanically controlled break junction technique and density-functional theory. We consider the case where interference is provided by overlapping quasidegenerate states. Decoherence mechanisms arising from electronic-vibrational coupling strongly affect the electrical current flowing through a single-molecule contact and can be controlled by temperature variation. Our findings underline the universal relevance of vibrations for understanding charge transport through molecular junctions.

Experimental evidence for quantum interference and vibrationally induced decoherence in single-molecule junctions.

PubMed

Ballmann, Stefan; Härtle, Rainer; Coto, Pedro B; Elbing, Mark; Mayor, Marcel; Bryce, Martin R; Thoss, Michael; Weber, Heiko B

2012-08-03

We analyze quantum interference and decoherence effects in single-molecule junctions both experimentally and theoretically by means of the mechanically controlled break junction technique and density-functional theory. We consider the case where interference is provided by overlapping quasidegenerate states. Decoherence mechanisms arising from electronic-vibrational coupling strongly affect the electrical current flowing through a single-molecule contact and can be controlled by temperature variation. Our findings underline the universal relevance of vibrations for understanding charge transport through molecular junctions.

Benchmarking Quantum Mechanics/Molecular Mechanics (QM/MM) Methods on the Thymidylate Synthase-Catalyzed Hydride Transfer.

PubMed

Świderek, Katarzyna; Arafet, Kemel; Kohen, Amnon; Moliner, Vicent

2017-03-14

Given the ubiquity of hydride-transfer reactions in enzyme-catalyzed processes, identifying the appropriate computational method for evaluating such biological reactions is crucial to perform theoretical studies of these processes. In this paper, the hydride-transfer step catalyzed by thymidylate synthase (TSase) is studied by examining hybrid quantum mechanics/molecular mechanics (QM/MM) potentials via multiple semiempirical methods and the M06-2X hybrid density functional. Calculations of protium and tritium transfer in these reactions across a range of temperatures allowed calculation of the temperature dependence of kinetic isotope effects (KIE). Dynamics and quantum-tunneling effects are revealed to have little effect on the reaction rate, but are significant in determining the KIEs and their temperature dependence. A good agreement with experiments is found, especially when computed for RM1/MM simulations. The small temperature dependence of quantum tunneling corrections and the quasiclassical contribution term cancel each other, while the recrossing transmission coefficient seems to be temperature-independent over the interval of 5-40 °C.

Exploring the propagation of relativistic quantum wavepackets in the trajectory-based formulation

NASA Astrophysics Data System (ADS)

Tsai, Hung-Ming; Poirier, Bill

2016-03-01

In the context of nonrelativistic quantum mechanics, Gaussian wavepacket solutions of the time-dependent Schrödinger equation provide useful physical insight. This is not the case for relativistic quantum mechanics, however, for which both the Klein-Gordon and Dirac wave equations result in strange and counterintuitive wavepacket behaviors, even for free-particle Gaussians. These behaviors include zitterbewegung and other interference effects. As a potential remedy, this paper explores a new trajectory-based formulation of quantum mechanics, in which the wavefunction plays no role [Phys. Rev. X, 4, 040002 (2014)]. Quantum states are represented as ensembles of trajectories, whose mutual interaction is the source of all quantum effects observed in nature—suggesting a “many interacting worlds” interpretation. It is shown that the relativistic generalization of the trajectory-based formulation results in well-behaved free-particle Gaussian wavepacket solutions. In particular, probability density is positive and well-localized everywhere, and its spatial integral is conserved over time—in any inertial frame. Finally, the ensemble-averaged wavepacket motion is along a straight line path through spacetime. In this manner, the pathologies of the wave-based relativistic quantum theory, as applied to wavepacket propagation, are avoided.

Kibble Zurek mechanism of topological defect formation in quantum field theory with matrix product states

NASA Astrophysics Data System (ADS)

Gillman, Edward; Rajantie, Arttu

2018-05-01

The Kibble Zurek mechanism in a relativistic ϕ4 scalar field theory in D =(1 +1 ) is studied using uniform matrix product states. The equal time two point function in momentum space G2(k ) is approximated as the system is driven through a quantum phase transition at a variety of different quench rates τQ. We focus on looking for signatures of topological defect formation in the system and demonstrate the consistency of the picture that the two point function G2(k ) displays two characteristic scales, the defect density n and the kink width dK. Consequently, G2(k ) provides a clear signature for the formation of defects and a well defined measure of the defect density in the system. These results provide a benchmark for the use of tensor networks as powerful nonperturbative nonequilibrium methods for relativistic quantum field theory, providing a promising technique for the future study of high energy physics and cosmology.

Emission mechanisms in Al-rich AlGaN/AlN quantum wells assessed by excitation power dependent photoluminescence spectroscopy

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

Iwata, Yoshiya; Banal, Ryan G.; Ichikawa, Shuhei

2015-02-21

The optical properties of Al-rich AlGaN/AlN quantum wells are assessed by excitation-power-dependent time-integrated (TI) and time-resolved (TR) photoluminescence (PL) measurements. Two excitation sources, an optical parametric oscillator and the 4th harmonics of a Ti:sapphire laser, realize a wide range of excited carrier densities between 10{sup 12} and 10{sup 21 }cm{sup −3}. The emission mechanisms change from an exciton to an electron-hole plasma as the excitation power increases. Accordingly, the PL decay time is drastically reduced, and the integrated PL intensities increase in the following order: linearly, super-linearly, linearly again, and sub-linearly. The observed results are well accounted for by rate equationsmore » that consider the saturation effect of non-radiative recombination processes. Using both TIPL and TRPL measurements allows the density of non-radiative recombination centers, the internal quantum efficiency, and the radiative recombination coefficient to be reliably extracted.« less

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.

How measurement reversal could erroneously suggest the capability to discriminate the preparation basis of a quantum ensemble

NASA Astrophysics Data System (ADS)

Goyal, Sandeep K.; Singh, Rajeev; Ghosh, Sibasish

2016-01-01

Mixed states of a quantum system, represented by density operators, can be decomposed as a statistical mixture of pure states in a number of ways where each decomposition can be viewed as a different preparation recipe. However the fact that the density matrix contains full information about the ensemble makes it impossible to estimate the preparation basis for the quantum system. Here we present a measurement scheme to (seemingly) improve the performance of unsharp measurements. We argue that in some situations this scheme is capable of providing statistics from a single copy of the quantum system, thus making it possible to perform state tomography from a single copy. One of the by-products of the scheme is a way to distinguish between different preparation methods used to prepare the state of the quantum system. However, our numerical simulations disagree with our intuitive predictions. We show that a counterintuitive property of a biased classical random walk is responsible for the proposed mechanism not working.

Weak Measurement and Quantum Smoothing of a Superconducting Qubit

NASA Astrophysics Data System (ADS)

Tan, Dian

In quantum mechanics, the measurement outcome of an observable in a quantum system is intrinsically random, yielding a probability distribution. The state of the quantum system can be described by a density matrix rho(t), which depends on the information accumulated until time t, and represents our knowledge about the system. The density matrix rho(t) gives probabilities for the outcomes of measurements at time t. Further probing of the quantum system allows us to refine our prediction in hindsight. In this thesis, we experimentally examine a quantum smoothing theory in a superconducting qubit by introducing an auxiliary matrix E(t) which is conditioned on information obtained from time t to a final time T. With the complete information before and after time t, the pair of matrices [rho(t), E(t)] can be used to make smoothed predictions for the measurement outcome at time t. We apply the quantum smoothing theory in the case of continuous weak measurement unveiling the retrodicted quantum trajectories and weak values. In the case of strong projective measurement, while the density matrix rho(t) with only diagonal elements in a given basis |n〉 may be treated as a classical mixture, we demonstrate a failure of this classical mixture description in determining the smoothed probabilities for the measurement outcome at time t with both diagonal rho(t) and diagonal E(t). We study the correlations between quantum states and weak measurement signals and examine aspects of the time symmetry of continuous quantum measurement. We also extend our study of quantum smoothing theory to the case of resonance fluorescence of a superconducting qubit with homodyne measurement and observe some interesting effects such as the modification of the excited state probabilities, weak values, and evolution of the predicted and retrodicted trajectories.

Effect of threading defects on InGaN /GaN multiple quantum well light emitting diodes

NASA Astrophysics Data System (ADS)

Ferdous, M. S.; Wang, X.; Fairchild, M. N.; Hersee, S. D.

2007-12-01

Photoelectrochemical etching was used to measure the threading defect (TD) density in InGaN multiple quantum well light-emitting diodes (LEDs) fabricated from commercial quality epitaxial wafers. The TD density was measured in the LED active region and then correlated with the previously measured characteristics of these LEDs. It was found that the reverse leakage current increased exponentially with TD density. The temperature dependence of this dislocation-related leakage current was consistent with a hopping mechanism at low reverse-bias voltage and Poole-Frenkel emission at higher reverse-bias voltage. The peak intensity and spectral width of the LED electroluminescence were found to be only weakly dependent on TD density for the measured TD range of 1×107-2×108cm-2.

Large size self-assembled quantum rings: quantum size effect and modulation on the surface diffusion.

PubMed

Tong, Cunzhu; Yoon, Soon Fatt; Wang, Lijun

2012-09-24

We demonstrate experimentally the submicron size self-assembled (SA) GaAs quantum rings (QRs) by quantum size effect (QSE). An ultrathin In0.1 Ga0.9As layer with different thickness is deposited on the GaAs to modulate the surface nucleus diffusion barrier, and then the SA QRs are grown. It is found that the density of QRs is affected significantly by the thickness of inserted In0.1 Ga0.9As, and the diffusion barrier modulation reflects mainly on the first five monolayer . The physical mechanism behind is discussed. The further analysis shows that about 160 meV decrease in diffusion barrier can be achieved, which allows the SA QRs with density of as low as one QR per 6 μm2. Finally, the QRs with diameters of 438 nm and outer diameters of 736 nm are fabricated using QSE.

Comparative analysis of quantum cascade laser modeling based on density matrices and non-equilibrium Green's functions

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

Lindskog, M., E-mail: martin.lindskog@teorfys.lu.se; Wacker, A.; Wolf, J. M.

2014-09-08

We study the operation of an 8.5 μm quantum cascade laser based on GaInAs/AlInAs lattice matched to InP using three different simulation models based on density matrix (DM) and non-equilibrium Green's function (NEGF) formulations. The latter advanced scheme serves as a validation for the simpler DM schemes and, at the same time, provides additional insight, such as the temperatures of the sub-band carrier distributions. We find that for the particular quantum cascade laser studied here, the behavior is well described by simple quantum mechanical estimates based on Fermi's golden rule. As a consequence, the DM model, which includes second order currents,more » agrees well with the NEGF results. Both these simulations are in accordance with previously reported data and a second regrown device.« less

Crossover to the anomalous quantum regime in the extrinsic spin Hall effect of graphene

NASA Astrophysics Data System (ADS)

Ferreira, Aires; Milletari, Mirco

Recent reports of spin-orbit coupling enhancement in chemically modified graphene have opened doors to studies of the spin Hall effect with massless chiral fermions. Here, we theoretically investigate the interaction and impurity density dependence of the extrinsic spin Hall effect in spin-orbit coupled graphene. We present a nonperturbative quantum diagrammatic calculation of the spin Hall response function in the strong-coupling regime that incorporates skew scattering and anomalous impurity density-independent contributions on equal footing. The spin Hall conductivity dependence on Fermi energy and electron-impurity interaction strength reveals the existence of experimentally accessible regions where anomalous quantum processes dominate. Our findings suggest that spin-orbit-coupled graphene is an ideal model system for probing the competition between semiclassical and bona fide quantum scattering mechanisms underlying the spin Hall effect. A.F. gratefully acknowledges the financial support of the Royal Society (U.K.).

The Biharmonic Oscillator and Asymmetric Linear Potentials: From Classical Trajectories to Momentum-Space Probability Densities in the Extreme Quantum Limit

ERIC Educational Resources Information Center

Ruckle, L. J.; Belloni, M.; Robinett, R. W.

2012-01-01

The biharmonic oscillator and the asymmetric linear well are two confining power-law-type potentials for which complete bound-state solutions are possible in both classical and quantum mechanics. We examine these problems in detail, beginning with studies of their trajectories in position and momentum space, evaluation of the classical probability…

Optical investigation of carrier tunneling in semiconductor nanostructures

NASA Astrophysics Data System (ADS)

Emiliani, V.; Ceccherini, S.; Bogani, F.; Colocci, M.; Frova, A.; Shi, Song Stone

1997-08-01

The tunneling dynamics of excitons and free carriers in AlxGa1-xAs/GaAs asymmetric double quantum well and near-surface quantum well structures has been investigated by means of time-resolved optical techniques. The competing processes of carrier tunneling out of the quantum well and exciton formation and recombination inside the quantum well have been thoroughly studied in the range of the excitation densities relevant to device applications. A consistent picture capable of fully describing the carrier and exciton-tunneling mechanisms in both types of structures has been obtained and apparently contrasting results in the recent literature are clarified.

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.

Metric on the space of quantum states from relative entropy. Tomographic reconstruction

NASA Astrophysics Data System (ADS)

Man'ko, Vladimir I.; Marmo, Giuseppe; Ventriglia, Franco; Vitale, Patrizia

2017-08-01

In the framework of quantum information geometry, we derive, from quantum relative Tsallis entropy, a family of quantum metrics on the space of full rank, N level quantum states, by means of a suitably defined coordinate free differential calculus. The cases N=2, N=3 are discussed in detail and notable limits are analyzed. The radial limit procedure has been used to recover quantum metrics for lower rank states, such as pure states. By using the tomographic picture of quantum mechanics we have obtained the Fisher-Rao metric for the space of quantum tomograms and derived a reconstruction formula of the quantum metric of density states out of the tomographic one. A new inequality obtained for probabilities of three spin-1/2 projections in three perpendicular directions is proposed to be checked in experiments with superconducting circuits.

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.

Clarifying the link between von Neumann and thermodynamic entropies

NASA Astrophysics Data System (ADS)

Deville, Alain; Deville, Yannick

2013-01-01

The state of a quantum system being described by a density operator ρ, quantum statistical mechanics calls the quantity - kTr( ρln ρ), introduced by von Neumann, its von Neumann or statistical entropy. A 1999 Shenker's paper initiated a debate about its link with the entropy of phenomenological thermodynamics. Referring to Gibbs's and von Neumann's founding texts, we replace von Neumann's 1932 contribution in its historical context, after Gibbs's 1902 treatise and before the creation of the information entropy concept, which places boundaries into the debate. Reexamining von Neumann's reasoning, we stress that the part of his reasoning implied in the debate mainly uses thermodynamics, not quantum mechanics, and identify two implicit postulates. We thoroughly examine Shenker's and ensuing papers, insisting upon the presence of open thermodynamical subsystems, imposing us the use of the chemical potential concept. We briefly mention Landau's approach to the quantum entropy. On the whole, it is shown that von Neumann's viewpoint is right, and why Shenker's claim that von Neumann entropy "is not the quantum-mechanical correlate of thermodynamic entropy" can't be retained.

Perturbatively deformed defects in Pöschl-Teller-driven scenarios for quantum mechanics

NASA Astrophysics Data System (ADS)

Bernardini, Alex E.; da Rocha, Roldão

2016-07-01

Pöschl-Teller-driven solutions for quantum mechanical fluctuations are triggered off by single scalar field theories obtained through a systematic perturbative procedure for generating deformed defects. The analytical properties concerning the quantum fluctuations in one-dimension, zero-mode states, first- and second-excited states, and energy density profiles are all obtained from deformed topological and non-topological structures supported by real scalar fields. Results are firstly derived from an integrated λϕ4 theory, with corresponding generalizations applied to starting λχ4 and sine-Gordon theories. By focusing our calculations on structures supported by the λϕ4 theory, the outcome of our study suggests an exact quantitative correspondence to Pöschl-Teller-driven systems. Embedded into the perturbative quantum mechanics framework, such a correspondence turns into a helpful tool for computing excited states and continuous mode solutions, as well as their associated energy spectrum, for quantum fluctuations of perturbatively deformed structures. Perturbative deformations create distinct physical scenarios in the context of exactly solvable quantum systems and may also work as an analytical support for describing novel braneworld universes embedded into a 5-dimensional gravity bulk.

A multiscale quantum mechanics/electromagnetics method for device simulations.

PubMed

Yam, ChiYung; Meng, Lingyi; Zhang, Yu; Chen, GuanHua

2015-04-07

Multiscale modeling has become a popular tool for research applying to different areas including materials science, microelectronics, biology, chemistry, etc. In this tutorial review, we describe a newly developed multiscale computational method, incorporating quantum mechanics into electronic device modeling with the electromagnetic environment included through classical electrodynamics. In the quantum mechanics/electromagnetics (QM/EM) method, the regions of the system where active electron scattering processes take place are treated quantum mechanically, while the surroundings are described by Maxwell's equations and a semiclassical drift-diffusion model. The QM model and the EM model are solved, respectively, in different regions of the system in a self-consistent manner. Potential distributions and current densities at the interface between QM and EM regions are employed as the boundary conditions for the quantum mechanical and electromagnetic simulations, respectively. The method is illustrated in the simulation of several realistic systems. In the case of junctionless field-effect transistors, transfer characteristics are obtained and a good agreement between experiments and simulations is achieved. Optical properties of a tandem photovoltaic cell are studied and the simulations demonstrate that multiple QM regions are coupled through the classical EM model. Finally, the study of a carbon nanotube-based molecular device shows the accuracy and efficiency of the QM/EM method.

Simple and exact approach to the electronic polarization effect on the solvation free energy: formulation for quantum-mechanical/molecular-mechanical system and its applications to aqueous solutions.

PubMed

Takahashi, Hideaki; Omi, Atsushi; Morita, Akihiro; Matubayasi, Nobuyuki

2012-06-07

We present a simple and exact numerical approach to compute the free energy contribution δμ in solvation due to the electron density polarization and fluctuation of a quantum-mechanical solute in the quantum-mechanical/molecular-mechanical (QM/MM) simulation combined with the theory of the energy representation (QM/MM-ER). Since the electron density fluctuation is responsible for the many-body QM-MM interactions, the standard version of the energy representation method cannot be applied directly. Instead of decomposing the QM-MM polarization energy into the pairwise additive and non-additive contributions, we take sum of the polarization energies in the QM-MM interaction and adopt it as a new energy coordinate for the method of energy representation. Then, it is demonstrated that the free energy δμ can be exactly formulated in terms of the energy distribution functions for the solution and reference systems with respect to this energy coordinate. The benchmark tests were performed to examine the numerical efficiency of the method with respect to the changes in the individual properties of the solvent and the solute. Explicitly, we computed the solvation free energy of a QM water molecule in ambient and supercritical water, and also the free-energy change associated with the isomerization reaction of glycine from neutral to zwitterionic structure in aqueous solution. In all the systems examined, it was demonstrated that the computed free energy δμ agrees with the experimental value, irrespective of the choice of the reference electron density of the QM solute. The present method was also applied to a prototype reaction of adenosine 5'-triphosphate hydrolysis where the effect of the electron density fluctuation is substantial due to the excess charge. It was demonstrated that the experimental free energy of the reaction has been accurately reproduced with the present approach.

Unifying Theory of Low-Energy Nuclear Reaction and Transmutation Processes in Deuterated/hydrogenated Metals, Acoustic Cavitation, Glow Discharge, and Deuteron Beam Experiments

NASA Astrophysics Data System (ADS)

Kim, Yeong E.; Zubarev, Alexander L.

The most basic theoretical challenge for understanding low-energy nuclear reaction (LENR) and transmutation reaction (LETR) in condensed matters is to find mechanisms by which the large Coulomb barrier between fusing nuclei can be overcome. A unifying theory of LENR and LETR has been developed to provide possible mechanisms for the LENR and LETR processes in matters based on high-density nano-scale and micro-scale quantum plasmas. It is shown that recently developed theoretical models based on Bose-Einstein Fusion (BEF) mechanism and Quantum Plasma Nuclear Fusion (QPNF) mechanism are applicable to the results of many different types of LENR and LETR experiments.

Nucleic acid reactivity : challenges for next-generation semiempirical quantum models

PubMed Central

Huang, Ming; Giese, Timothy J.; York, Darrin M.

2016-01-01

Semiempirical quantum models are routinely used to study mechanisms of RNA catalysis and phosphoryl transfer reactions using combined quantum mechanical/molecular mechanical methods. Herein, we provide a broad assessment of the performance of existing semiempirical quantum models to describe nucleic acid structure and reactivity in order to quantify their limitations and guide the development of next-generation quantum models with improved accuracy. Neglect of diatomic diffierential overlap (NDDO) and self-consistent density-functional tight-binding (SCC-DFTB) semiempirical models are evaluated against high-level quantum mechanical benchmark calculations for seven biologically important data sets. The data sets include: proton affinities, polarizabilities, nucleobase dimer interactions, dimethyl phosphate anion, nucleoside sugar and glycosidic torsion conformations, and RNA phosphoryl transfer model reactions. As an additional baseline, comparisons are made with several commonly used density-functional models, including M062X and B3LYP (in some cases with dispersion corrections). The results show that, among the semiempirical models examined, the AM1/d-PhoT model is the most robust at predicting proton affinities. AM1/d-PhoT and DFTB3-3ob/OPhyd reproduce the MP2 potential energy surfaces of 6 associative RNA phosphoryl transfer model reactions reasonably well. Further, a recently developed linear-scaling “modified divide-and-conquer” model exhibits the most accurate results for binding energies of both hydrogen bonded and stacked nucleobase dimers. The semiempirical models considered here are shown to underestimate the isotropic polarizabilities of neutral molecules by approximately 30%. The semiempirical models also fail to adequately describe torsion profiles within the dimethyl phosphate anion, the nucleoside sugar ring puckers, and the rotations about the nucleoside glycosidic bond. The modeling of pentavalent phosphorus, particularly with thio substitutions often used experimentally as mechanistic probes, was problematic for all of the models considered. Analysis of the strengths and weakness of the models suggest that the creation of robust next-generation models should emphasize the improvement of relative conformational energies and barriers, and nonbond interactions. PMID:25943338

Process, System, Causality, and Quantum Mechanics: A Psychoanalysis of Animal Faith

NASA Astrophysics Data System (ADS)

Etter, Tom; Noyes, H. Pierre

We shall argue in this paper that a central piece of modern physics does not really belong to physics at all but to elementary probability theory. Given a joint probability distribution J on a set of random variables containing x and y, define a link between x and y to be the condition x=y on J. Define the {\\it state} D of a link x=y as the joint probability distribution matrix on x and y without the link. The two core laws of quantum mechanics are the Born probability rule, and the unitary dynamical law whose best known form is the Schrodinger's equation. Von Neumann formulated these two laws in the language of Hilbert space as prob(P) = trace(PD) and D'T = TD respectively, where P is a projection, D and D' are (von Neumann) density matrices, and T is a unitary transformation. We'll see that if we regard link states as density matrices, the algebraic forms of these two core laws occur as completely general theorems about links. When we extend probability theory by allowing cases to count negatively, we find that the Hilbert space framework of quantum mechanics proper emerges from the assumption that all D's are symmetrical in rows and columns. On the other hand, Markovian systems emerge when we assume that one of every linked variable pair has a uniform probability distribution. By representing quantum and Markovian structure in this way, we see clearly both how they differ, and also how they can coexist in natural harmony with each other, as they must in quantum measurement, which we'll examine in some detail. Looking beyond quantum mechanics, we see how both structures have their special places in a much larger continuum of formal systems that we have yet to look for in nature.

Chemical Potential for the Interacting Classical Gas and the Ideal Quantum Gas Obeying a Generalized Exclusion Principle

ERIC Educational Resources Information Center

Sevilla, F. J.; Olivares-Quiroz, L.

2012-01-01

In this work, we address the concept of the chemical potential [mu] in classical and quantum gases towards the calculation of the equation of state [mu] = [mu](n, T) where n is the particle density and "T" the absolute temperature using the methods of equilibrium statistical mechanics. Two cases seldom discussed in elementary textbooks are…

Mid-Infrared Quantum-Dot Quantum Cascade Laser: A Theoretical Feasibility Study

DOE PAGES

Michael, Stephan; Chow, Weng; Schneider, Hans

2016-05-01

In the framework of a microscopic model for intersubband gain from electrically pumped quantum-dot structures we investigate electrically pumped quantum-dots as active material for a mid-infrared quantum cascade laser. Our previous calculations have indicated that these structures could operate with reduced threshold current densities while also achieving a modal gain comparable to that of quantum well active materials. We study the influence of two important quantum-dot material parameters, here, namely inhomogeneous broadening and quantum-dot sheet density, on the performance of a proposed quantum cascade laser design. In terms of achieving a positive modal net gain, a high quantum-dot density canmore » compensate for moderately high inhomogeneous broadening, but at a cost of increased threshold current density. By minimizing quantum-dot density with presently achievable inhomogeneous broadening and total losses, significantly lower threshold densities than those reported in quantum-well quantum-cascade lasers are predicted by our theory.« less

Quantum mechanical tunneling in the automerization of cyclobutadiene

NASA Astrophysics Data System (ADS)

Schoonmaker, R.; Lancaster, T.; Clark, S. J.

2018-03-01

Cyclobutadiene has a four-membered carbon ring with two double bonds, but this highly strained molecular configuration is almost square and, via a coordinated motion, the nuclei quantum mechanically tunnels through the high-energy square state to a configuration equivalent to the initial configuration under a 90° rotation. This results in a square ground state, comprising a superposition of two molecular configurations, that is driven by quantum tunneling. Using a quantum mechanical model, and an effective nuclear potential from density functional theory, we calculate the vibrational energy spectrum and the accompanying wavefunctions. We use the wavefunctions to identify the motions of the molecule and detail how different motions can enhance or suppress the tunneling rate. This is relevant for kinematics of tunneling-driven reactions, and we discuss these implications. We are also able to provide a qualitative account of how the molecule will respond to an external perturbation and how this may enhance or suppress infra-red-active vibrational transitions.

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

Michael, Stephan; Chow, Weng; Schneider, Hans

In the framework of a microscopic model for intersubband gain from electrically pumped quantum-dot structures we investigate electrically pumped quantum-dots as active material for a mid-infrared quantum cascade laser. Our previous calculations have indicated that these structures could operate with reduced threshold current densities while also achieving a modal gain comparable to that of quantum well active materials. We study the influence of two important quantum-dot material parameters, here, namely inhomogeneous broadening and quantum-dot sheet density, on the performance of a proposed quantum cascade laser design. In terms of achieving a positive modal net gain, a high quantum-dot density canmore » compensate for moderately high inhomogeneous broadening, but at a cost of increased threshold current density. By minimizing quantum-dot density with presently achievable inhomogeneous broadening and total losses, significantly lower threshold densities than those reported in quantum-well quantum-cascade lasers are predicted by our theory.« less

A Perron-Frobenius type of theorem for quantum operations

NASA Astrophysics Data System (ADS)

Lagro, Matthew

Quantum random walks are a generalization of classical Markovian random walks to a quantum mechanical or quantum computing setting. Quantum walks have promising applications but are complicated by quantum decoherence. We prove that the long-time limiting behavior of the class of quantum operations which are the convex combination of norm one operators is governed by the eigenvectors with norm one eigenvalues which are shared by the operators. This class includes all operations formed by a coherent operation with positive probability of orthogonal measurement at each step. We also prove that any operation that has range contained in a low enough dimension subspace of the space of density operators has limiting behavior isomorphic to an associated Markov chain. A particular class of such operations are coherent operations followed by an orthogonal measurement. Applications of the convergence theorems to quantum walks are given.

Real-Time Quantum Dynamics of Long-Range Electronic Excitation Transfer in Plasmonic Nanoantennas.

PubMed

Ilawe, Niranjan V; Oviedo, M Belén; Wong, Bryan M

2017-08-08

Using large-scale, real-time, quantum dynamics calculations, we present a detailed analysis of electronic excitation transfer (EET) mechanisms in a multiparticle plasmonic nanoantenna system. Specifically, we utilize real-time, time-dependent, density functional tight binding (RT-TDDFTB) to provide a quantum-mechanical description (at an electronic/atomistic level of detail) for characterizing and analyzing these systems, without recourse to classical approximations. We also demonstrate highly long-range electronic couplings in these complex systems and find that the range of these couplings is more than twice the conventional cutoff limit considered by Förster resonance energy transfer (FRET)-based approaches. Furthermore, we attribute these unusually long-ranged electronic couplings to the coherent oscillations of conduction electrons in plasmonic nanoparticles. This long-range nature of plasmonic interactions has important ramifications for EET; in particular, we show that the commonly used "nearest-neighbor" FRET model is inadequate for accurately characterizing EET even in simple plasmonic antenna systems. These findings provide a real-time, quantum-mechanical perspective for understanding EET mechanisms and provide guidance in enhancing plasmonic properties in artificial light-harvesting systems.

Magnetotransport studies of mobility limiting mechanisms in undoped Si/SiGe heterostructures

NASA Astrophysics Data System (ADS)

Mi, X.; Hazard, T. M.; Payette, C.; Wang, K.; Zajac, D. M.; Cady, J. V.; Petta, J. R.

2015-07-01

We perform detailed magnetotransport studies on two-dimensional electron gases (2DEGs) formed in undoped Si/SiGe heterostructures in order to identify the electron mobility limiting mechanisms. By analyzing data from 26 different heterostructures, we observe a strong correlation between the background oxygen concentration in the Si quantum well and the maximum mobility. The highest-quality wafer supports a 2DEG with mobility μ =160 000 cm 2/Vs at a density n =2.17 ×1011 /cm 2 and exhibits a metal-to-insulator transition at a critical density nc=0.46 ×1011 /cm 2. We extract a valley splitting Δv˜150 μ eV at a magnetic field B =1.8 T. These results provide evidence that undoped Si/SiGe heterostructures are suitable for the fabrication of few-electron quantum dots.

A Concise Introduction to Quantum Mechanics

NASA Astrophysics Data System (ADS)

Swanson, Mark S.

2018-02-01

Assuming a background in basic classical physics, multivariable calculus, and differential equations, A Concise Introduction to Quantum Mechanics provides a self-contained presentation of the mathematics and physics of quantum mechanics. The relevant aspects of classical mechanics and electrodynamics are reviewed, and the basic concepts of wave-particle duality are developed as a logical outgrowth of experiments involving blackbody radiation, the photoelectric effect, and electron diffraction. The Copenhagen interpretation of the wave function and its relation to the particle probability density is presented in conjunction with Fourier analysis and its generalization to function spaces. These concepts are combined to analyze the system consisting of a particle confined to a box, developing the probabilistic interpretation of observations and their associated expectation values. The Schrödinger equation is then derived by using these results and demanding both Galilean invariance of the probability density and Newtonian energy-momentum relations. The general properties of the Schrödinger equation and its solutions are analyzed, and the theory of observables is developed along with the associated Heisenberg uncertainty principle. Basic applications of wave mechanics are made to free wave packet spreading, barrier penetration, the simple harmonic oscillator, the Hydrogen atom, and an electric charge in a uniform magnetic field. In addition, Dirac notation, elements of Hilbert space theory, operator techniques, and matrix algebra are presented and used to analyze coherent states, the linear potential, two state oscillations, and electron diffraction. Applications are made to photon and electron spin and the addition of angular momentum, and direct product multiparticle states are used to formulate both the Pauli exclusion principle and quantum decoherence. The book concludes with an introduction to the rotation group and the general properties of angular momentum.

Vibrational analysis and quantum chemical calculations of 2,2‧-bipyridine Zinc(II) halide complexes

NASA Astrophysics Data System (ADS)

Ozel, Aysen E.; Kecel, Serda; Akyuz, Sevim

2007-05-01

In this study the molecular structure and vibrational spectra of Zn(2,2'-bipyridine)X 2 (X = Cl and Br) complexes were studied in their ground states by computational vibrational study and scaled quantum mechanical (SQM) analysis. The geometry optimization, vibrational wavenumber and intensity calculations of free and coordinated 2,2'-bipyridine were carried out with the Gaussian03 program package by using Hartree-Fock (HF) and Density Functional Theory (DFT) with B3LYP functional and 6-31G (d,p) basis set. The total energy distributions (TED) of the vibrational modes were calculated by using Scaled Quantum Mechanical (SQM) analysis. Fundamentals were characterised by their total energy distributions. Coordination sensitive modes of 2,2'-bipyridine were determined.

Critical density of a soliton gas

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

El, G. A., E-mail: g.el@lboro.ac.uk

We quantify the notion of a dense soliton gas by establishing an upper bound for the integrated density of states of the quantum-mechanical Schrödinger operator associated with the Korteweg–de Vries soliton gas dynamics. As a by-product of our derivation, we find the speed of sound in the soliton gas with Gaussian spectral distribution function.

Critical density of a soliton gas

NASA Astrophysics Data System (ADS)

El, G. A.

2016-02-01

We quantify the notion of a dense soliton gas by establishing an upper bound for the integrated density of states of the quantum-mechanical Schrödinger operator associated with the Korteweg-de Vries soliton gas dynamics. As a by-product of our derivation, we find the speed of sound in the soliton gas with Gaussian spectral distribution function.

A quantum measure of the multiverse

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

Vilenkin, Alexander, E-mail: vilenkin@cosmos.phy.tufts.edu

2014-05-01

It has been recently suggested that probabilities of different events in the multiverse are given by the frequencies at which these events are encountered along the worldline of a geodesic observer (the ''watcher''). Here I discuss an extension of this probability measure to quantum theory. The proposed extension is gauge-invariant, as is the classical version of this measure. Observations of the watcher are described by a reduced density matrix, and the frequencies of events can be found using the decoherent histories formalism of Quantum Mechanics (adapted to open systems). The quantum watcher measure makes predictions in agreement with the standardmore » Born rule of QM.« less

The Madelung Picture as a Foundation of Geometric Quantum Theory

NASA Astrophysics Data System (ADS)

Reddiger, Maik

2017-10-01

Despite its age, quantum theory still suffers from serious conceptual difficulties. To create clarity, mathematical physicists have been attempting to formulate quantum theory geometrically and to find a rigorous method of quantization, but this has not resolved the problem. In this article we argue that a quantum theory recursing to quantization algorithms is necessarily incomplete. To provide an alternative approach, we show that the Schrödinger equation is a consequence of three partial differential equations governing the time evolution of a given probability density. These equations, discovered by Madelung, naturally ground the Schrödinger theory in Newtonian mechanics and Kolmogorovian probability theory. A variety of far-reaching consequences for the projection postulate, the correspondence principle, the measurement problem, the uncertainty principle, and the modeling of particle creation and annihilation are immediate. We also give a speculative interpretation of the equations following Bohm, Vigier and Tsekov, by claiming that quantum mechanical behavior is possibly caused by gravitational background noise.

Path-integral approach to the Wigner-Kirkwood expansion.

PubMed

Jizba, Petr; Zatloukal, Václav

2014-01-01

We study the high-temperature behavior of quantum-mechanical path integrals. Starting from the Feynman-Kac formula, we derive a functional representation of the Wigner-Kirkwood perturbation expansion for quantum Boltzmann densities. As shown by its applications to different potentials, the presented expansion turns out to be quite efficient in generating analytic form of the higher-order expansion coefficients. To put some flesh on the bare bones, we apply the expansion to obtain basic thermodynamic functions of the one-dimensional anharmonic oscillator. Further salient issues, such as generalization to the Bloch density matrix and comparison with the more customary world-line formulation, are discussed.

Here and now: the intersection of computational science, quantum-mechanical simulations, and materials science

NASA Astrophysics Data System (ADS)

Marzari, Nicola

The last 30 years have seen the steady and exhilarating development of powerful quantum-simulation engines for extended systems, dedicated to the solution of the Kohn-Sham equations of density-functional theory, often augmented by density-functional perturbation theory, many-body perturbation theory, time-dependent density-functional theory, dynamical mean-field theory, and quantum Monte Carlo. Their implementation on massively parallel architectures, now leveraging also GPUs and accelerators, has started a massive effort in the prediction from first principles of many or of complex materials properties, leading the way to the exascale through the combination of HPC (high-performance computing) and HTC (high-throughput computing). Challenges and opportunities abound: complementing hardware and software investments and design; developing the materials' informatics infrastructure needed to encode knowledge into complex protocols and workflows of calculations; managing and curating data; resisting the complacency that we have already reached the predictive accuracy needed for materials design, or a robust level of verification of the different quantum engines. In this talk I will provide an overview of these challenges, with the ultimate prize being the computational understanding, prediction, and design of properties and performance for novel or complex materials and devices.

Bell's theorem and the problem of decidability between the views of Einstein and Bohr.

PubMed

Hess, K; Philipp, W

2001-12-04

Einstein, Podolsky, and Rosen (EPR) have designed a gedanken experiment that suggested a theory that was more complete than quantum mechanics. The EPR design was later realized in various forms, with experimental results close to the quantum mechanical prediction. The experimental results by themselves have no bearing on the EPR claim that quantum mechanics must be incomplete nor on the existence of hidden parameters. However, the well known inequalities of Bell are based on the assumption that local hidden parameters exist and, when combined with conflicting experimental results, do appear to prove that local hidden parameters cannot exist. This fact leaves only instantaneous actions at a distance (called "spooky" by Einstein) to explain the experiments. The Bell inequalities are based on a mathematical model of the EPR experiments. They have no experimental confirmation, because they contradict the results of all EPR experiments. In addition to the assumption that hidden parameters exist, Bell tacitly makes a variety of other assumptions; for instance, he assumes that the hidden parameters are governed by a single probability measure independent of the analyzer settings. We argue that the mathematical model of Bell excludes a large set of local hidden variables and a large variety of probability densities. Our set of local hidden variables includes time-like correlated parameters and a generalized probability density. We prove that our extended space of local hidden variables does permit derivation of the quantum result and is consistent with all known experiments.

Nonadiabatic Molecular Dynamics and Orthogonality Constrained Density Functional Theory

NASA Astrophysics Data System (ADS)

Shushkov, Philip Georgiev

The exact quantum dynamics of realistic, multidimensional systems remains a formidable computational challenge. In many chemical processes, however, quantum effects such as tunneling, zero-point energy quantization, and nonadiabatic transitions play an important role. Therefore, approximate approaches that improve on the classical mechanical framework are of special practical interest. We propose a novel ring polymer surface hopping method for the calculation of chemical rate constants. The method blends two approaches, namely ring polymer molecular dynamics that accounts for tunneling and zero-point energy quantization, and surface hopping that incorporates nonadiabatic transitions. We test the method against exact quantum mechanical calculations for a one-dimensional, two-state model system. The method reproduces quite accurately the tunneling contribution to the rate and the distribution of reactants between the electronic states for this model system. Semiclassical instanton theory, an approach related to ring polymer molecular dynamics, accounts for tunneling by the use of periodic classical trajectories on the inverted potential energy surface. We study a model of electron transfer in solution, a chemical process where nonadiabatic events are prominent. By representing the tunneling electron with a ring polymer, we derive Marcus theory of electron transfer from semiclassical instanton theory after a careful analysis of the tunneling mode. We demonstrate that semiclassical instanton theory can recover the limit of Fermi's Golden Rule rate in a low-temperature, deep-tunneling regime. Mixed quantum-classical dynamics treats a few important degrees of freedom quantum mechanically, while classical mechanics describes affordably the rest of the system. But the interface of quantum and classical description is a challenging theoretical problem, especially for low-energy chemical processes. We therefore focus on the semiclassical limit of the coupled nuclear-electronic dynamics. We show that the time-dependent Schrodinger equation for the electrons employed in the widely used fewest switches surface hopping method is applicable only in the limit of nearly identical classical trajectories on the different potential energy surfaces. We propose a short-time decoupling algorithm that restricts the use of the Schrodinger equation only to the interaction regions. We test the short-time approximation on three model systems against exact quantum-mechanical calculations. The approximation improves the performance of the surface hopping approach. Nonadiabatic molecular dynamics simulations require the efficient and accurate computation of ground and excited state potential energy surfaces. Unlike the ground state calculations where standard methods exist, the computation of excited state properties is a challenging task. We employ time-independent density functional theory, in which the excited state energy is represented as a functional of the total density. We suggest an adiabatic-like approximation that simplifies the excited state exchange-correlation functional. We also derive a set of minimal conditions to impose exactly the orthogonality of the excited state Kohn-Sham determinant to the ground state determinant. This leads to an efficient, variational algorithm for the self-consistent optimization of the excited state energy. Finally, we assess the quality of the excitation energies obtained by the new method on a set of 28 organic molecules. The new approach provides results of similar accuracy to time-dependent density functional theory.

Differential geometry-based solvation and electrolyte transport models for biomolecular modeling: a review

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

Wei, Guowei; Baker, Nathan A.

2016-11-11

This chapter reviews the differential geometry-based solvation and electrolyte transport for biomolecular solvation that have been developed over the past decade. A key component of these methods is the differential geometry of surfaces theory, as applied to the solvent-solute boundary. In these approaches, the solvent-solute boundary is determined by a variational principle that determines the major physical observables of interest, for example, biomolecular surface area, enclosed volume, electrostatic potential, ion density, electron density, etc. Recently, differential geometry theory has been used to define the surfaces that separate the microscopic (solute) domains for biomolecules from the macroscopic (solvent) domains. In thesemore » approaches, the microscopic domains are modeled with atomistic or quantum mechanical descriptions, while continuum mechanics models (including fluid mechanics, elastic mechanics, and continuum electrostatics) are applied to the macroscopic domains. This multiphysics description is integrated through an energy functional formalism and the resulting Euler-Lagrange equation is employed to derive a variety of governing partial differential equations for different solvation and transport processes; e.g., the Laplace-Beltrami equation for the solvent-solute interface, Poisson or Poisson-Boltzmann equations for electrostatic potentials, the Nernst-Planck equation for ion densities, and the Kohn-Sham equation for solute electron density. Extensive validation of these models has been carried out over hundreds of molecules, including proteins and ion channels, and the experimental data have been compared in terms of solvation energies, voltage-current curves, and density distributions. We also propose a new quantum model for electrolyte transport.« less

Exciton recombination dynamics in CdSe nanowires: bimolecular to three-carrier Auger kinetics.

PubMed

Robel, István; Bunker, Bruce A; Kamat, Prashant V; Kuno, Masaru

2006-07-01

Ultrafast relaxation dynamics of charge carriers in CdSe quantum wires with diameters between 6 and 8 nm are studied as a function of carrier density. At high electron-hole pair densities above 10(19) cm(-3) the dominant process for carrier cooling is the "bimolecular" Auger recombination of one-dimensional (1D) excitons. However, below this excitation level an unexpected transition from a bimolecular (exciton-exciton) to a three-carrier Auger relaxation mechanism occurs. Thus, depending on excitation intensity, electron-hole pair relaxation dynamics in the nanowires exhibit either 1D or 0D (quantum dot) character. This dual nature of the recovery kinetics defines an optimal intensity for achieving optical gain in solution-grown nanowires given the different carrier-density-dependent scaling of relaxation rates in either regime.

Holonomy, quantum mechanics and the signal-tuned Gabor approach to the striate cortex

NASA Astrophysics Data System (ADS)

Torreão, José R. A.

2016-02-01

It has been suggested that an appeal to holographic and quantum properties will be ultimately required for the understanding of higher brain functions. On the other hand, successful quantum-like approaches to cognitive and behavioral processes bear witness to the usefulness of quantum prescriptions as applied to the analysis of complex non-quantum systems. Here, we show that the signal-tuned Gabor approach for modeling cortical neurons, although not based on quantum assumptions, also admits a quantum-like interpretation. Recently, the equation of motion for the signal-tuned complex cell response has been derived and proven equivalent to the Schrödinger equation for a dissipative quantum system whose solutions come under two guises: as plane-wave and Airy-packet responses. By interpreting the squared magnitude of the plane-wave solution as a probability density, in accordance with the quantum mechanics prescription, we arrive at a Poisson spiking probability — a common model of neuronal response — while spike propagation can be described by the Airy-packet solution. The signal-tuned approach is also proven consistent with holonomic brain theories, as it is based on Gabor functions which provide a holographic representation of the cell’s input, in the sense that any restricted subset of these functions still allows stimulus reconstruction.

Exact and Optimal Quantum Mechanics/Molecular Mechanics Boundaries.

PubMed

Sun, Qiming; Chan, Garnet Kin-Lic

2014-09-09

Motivated by recent work in density matrix embedding theory, we define exact link orbitals that capture all quantum mechanical (QM) effects across arbitrary quantum mechanics/molecular mechanics (QM/MM) boundaries. Exact link orbitals are rigorously defined from the full QM solution, and their number is equal to the number of orbitals in the primary QM region. Truncating the exact set yields a smaller set of link orbitals optimal with respect to reproducing the primary region density matrix. We use the optimal link orbitals to obtain insight into the limits of QM/MM boundary treatments. We further analyze the popular general hybrid orbital (GHO) QM/MM boundary across a test suite of molecules. We find that GHOs are often good proxies for the most important optimal link orbital, although there is little detailed correlation between the detailed GHO composition and optimal link orbital valence weights. The optimal theory shows that anions and cations cannot be described by a single link orbital. However, expanding to include the second most important optimal link orbital in the boundary recovers an accurate description. The second optimal link orbital takes the chemically intuitive form of a donor or acceptor orbital for charge redistribution, suggesting that optimal link orbitals can be used as interpretative tools for electron transfer. We further find that two optimal link orbitals are also sufficient for boundaries that cut across double bonds. Finally, we suggest how to construct "approximately" optimal link orbitals for practical QM/MM calculations.

Principles of Quantum Mechanics

NASA Astrophysics Data System (ADS)

Landé, Alfred

2013-10-01

Preface; Introduction: 1. Observation and interpretation; 2. Difficulties of the classical theories; 3. The purpose of quantum theory; Part I. Elementary Theory of Observation (Principle of Complementarity): 4. Refraction in inhomogeneous media (force fields); 5. Scattering of charged rays; 6. Refraction and reflection at a plane; 7. Absolute values of momentum and wave length; 8. Double ray of matter diffracting light waves; 9. Double ray of matter diffracting photons; 10. Microscopic observation of ρ (x) and σ (p); 11. Complementarity; 12. Mathematical relation between ρ (x) and σ (p) for free particles; 13. General relation between ρ (q) and σ (p); 14. Crystals; 15. Transition density and transition probability; 16. Resultant values of physical functions; matrix elements; 17. Pulsating density; 18. General relation between ρ (t) and σ (є); 19. Transition density; matrix elements; Part II. The Principle of Uncertainty: 20. Optical observation of density in matter packets; 21. Distribution of momenta in matter packets; 22. Mathematical relation between ρ and σ; 23. Causality; 24. Uncertainty; 25. Uncertainty due to optical observation; 26. Dissipation of matter packets; rays in Wilson Chamber; 27. Density maximum in time; 28. Uncertainty of energy and time; 29. Compton effect; 30. Bothe-Geiger and Compton-Simon experiments; 31. Doppler effect; Raman effect; 32. Elementary bundles of rays; 33. Jeans' number of degrees of freedom; 34. Uncertainty of electromagnetic field components; Part III. The Principle of Interference and Schrödinger's equation: 35. Physical functions; 36. Interference of probabilities for p and q; 37. General interference of probabilities; 38. Differential equations for Ψp (q) and Xq (p); 39. Differential equation for фβ (q); 40. The general probability amplitude Φβ' (Q); 41. Point transformations; 42. General theorem of interference; 43. Conjugate variables; 44. Schrödinger's equation for conservative systems; 45. Schrödinger's equation for non-conservative systems; 46. Pertubation theory; 47. Orthogonality, normalization and Hermitian conjugacy; 48. General matrix elements; Part IV. The Principle of Correspondence: 49. Contact transformations in classical mechanics; 50. Point transformations; 51. Contact transformations in quantum mechanics; 52. Constants of motion and angular co-ordinates; 53. Periodic orbits; 54. De Broglie and Schrödinger function; correspondence to classical mechanics; 55. Packets of probability; 56. Correspondence to hydrodynamics; 57. Motion and scattering of wave packets; 58. Formal correspondence between classical and quantum mechanics; Part V. Mathematical Appendix: Principle of Invariance: 59. The general theorem of transformation; 60. Operator calculus; 61. Exchange relations; three criteria for conjugacy; 62. First method of canonical transformation; 63. Second method of canonical transformation; 64. Proof of the transformation theorem; 65. Invariance of the matrix elements against unitary transformations; 66. Matrix mechanics; Index of literature; Index of names and subjects.

On the minimum quantum requirement of photosynthesis.

PubMed

Zeinalov, Yuzeir

2009-01-01

An analysis of the shape of photosynthetic light curves is presented and the existence of the initial non-linear part is shown as a consequence of the operation of the non-cooperative (Kok's) mechanism of oxygen evolution or the effect of dark respiration. The effect of nonlinearity on the quantum efficiency (yield) and quantum requirement is reconsidered. The essential conclusions are: 1) The non-linearity of the light curves cannot be compensated using suspensions of algae or chloroplasts with high (>1.0) optical density or absorbance. 2) The values of the maxima of the quantum efficiency curves or the values of the minima of the quantum requirement curves cannot be used for estimation of the exact value of the maximum quantum efficiency and the minimum quantum requirement. The estimation of the maximum quantum efficiency or the minimum quantum requirement should be performed only after extrapolation of the linear part at higher light intensities of the quantum requirement curves to "0" light intensity.

What Density Functional Theory could do for Quantum Information

NASA Astrophysics Data System (ADS)

Mattsson, Ann

2015-03-01

The Hohenberg-Kohn theorem of Density Functional Theory (DFT), and extensions thereof, tells us that all properties of a system of electrons can be determined through their density, which uniquely determines the many-body wave-function. Given access to the appropriate, universal, functionals of the density we would, in theory, be able to determine all observables of any electronic system, without explicit reference to the wave-function. On the other hand, the wave-function is at the core of Quantum Information (QI), with the wave-function of a set of qubits being the central computational resource in a quantum computer. While there is seemingly little overlap between DFT and QI, reliance upon observables form a key connection. Though the time-evolution of the wave-function and associated phase information is fundamental to quantum computation, the initial and final states of a quantum computer are characterized by observables of the system. While observables can be extracted directly from a system's wave-function, DFT tells us that we may be able to intuit a method for extracting them from its density. In this talk, I will review the fundamentals of DFT and how these principles connect to the world of QI. This will range from DFT's utility in the engineering of physical qubits, to the possibility of using it to efficiently (but approximately) simulate Hamiltonians at the logical level. The apparent paradox of describing algorithms based on the quantum mechanical many-body wave-function with a DFT-like theory based on observables will remain a focus throughout. The ultimate goal of this talk is to initiate a dialog about what DFT could do for QI, in theory and in practice. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.

Ab initio molecular dynamics with nuclear quantum effects at classical cost: Ring polymer contraction for density functional theory.

PubMed

Marsalek, Ondrej; Markland, Thomas E

2016-02-07

Path integral molecular dynamics simulations, combined with an ab initio evaluation of interactions using electronic structure theory, incorporate the quantum mechanical nature of both the electrons and nuclei, which are essential to accurately describe systems containing light nuclei. However, path integral simulations have traditionally required a computational cost around two orders of magnitude greater than treating the nuclei classically, making them prohibitively costly for most applications. Here we show that the cost of path integral simulations can be dramatically reduced by extending our ring polymer contraction approach to ab initio molecular dynamics simulations. By using density functional tight binding as a reference system, we show that our ring polymer contraction scheme gives rapid and systematic convergence to the full path integral density functional theory result. We demonstrate the efficiency of this approach in ab initio simulations of liquid water and the reactive protonated and deprotonated water dimer systems. We find that the vast majority of the nuclear quantum effects are accurately captured using contraction to just the ring polymer centroid, which requires the same number of density functional theory calculations as a classical simulation. Combined with a multiple time step scheme using the same reference system, which allows the time step to be increased, this approach is as fast as a typical classical ab initio molecular dynamics simulation and 35× faster than a full path integral calculation, while still exactly including the quantum sampling of nuclei. This development thus offers a route to routinely include nuclear quantum effects in ab initio molecular dynamics simulations at negligible computational cost.

Nonuniform continuum model for solvatochromism based on frozen-density embedding theory.

PubMed

Shedge, Sapana Vitthal; Wesolowski, Tomasz A

2014-10-20

Frozen-density embedding theory (FDET) provides the formal framework for multilevel numerical simulations, such that a selected subsystem is described at the quantum mechanical level, whereas its environment is described by means of the electron density (frozen density; ${\\rho _{\\rm{B}} (\\vec r)}$). The frozen density ${\\rho _{\\rm{B}} (\\vec r)}$ is usually obtained from some lower-level quantum mechanical methods applied to the environment, but FDET is not limited to such choices for ${\\rho _{\\rm{B}} (\\vec r)}$. The present work concerns the application of FDET, in which ${\\rho _{\\rm{B}} (\\vec r)}$ is the statistically averaged electron density of the solvent ${\\left\\langle {\\rho _{\\rm{B}} (\\vec r)} \\right\\rangle }$. The specific solute-solvent interactions are represented in a statistical manner in ${\\left\\langle {\\rho _{\\rm{B}} (\\vec r)} \\right\\rangle }$. A full self-consistent treatment of solvated chromophore, thus involves a single geometry of the chromophore in a given state and the corresponding ${\\left\\langle {\\rho _{\\rm{B}} (\\vec r)} \\right\\rangle }$. We show that the coupling between the two descriptors might be made in an approximate manner that is applicable for both absorption and emission. The proposed protocol leads to accurate (error in the range of 0.05 eV) descriptions of the solvatochromic shifts in both absorption and emission. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Nano-Transistor Modeling: Two Dimensional Green's Function Method

NASA Technical Reports Server (NTRS)

Svizhenko, Alexei; Anantram, M. P.; Govindan, T. R.; Biegel, Bryan

2001-01-01

Two quantum mechanical effects that impact the operation of nanoscale transistors are inversion layer energy quantization and ballistic transport. While the qualitative effects of these features are reasonably understood, a comprehensive study of device physics in two dimensions is lacking. Our work addresses this shortcoming and provides: (a) a framework to quantitatively explore device physics issues such as the source-drain and gate leakage currents, DIBL (Drain Induced Barrier Lowering), and threshold voltage shift due to quantization, and b) a means of benchmarking quantum corrections to semiclassical models (such as density-gradient and quantum-corrected MEDICI).

Stimulated emission in quantum well laser diodes

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

Blood, P.

1989-07-03

We observe that stimulated emission from inhomogeneously pumped quantum well laser diodes is shifted down in energy compared with the subband transition energy. Measured spontaneous emission spectra show that this stimulated emission is due to band-to-band transitions shifted by renormalization at high injected carrier densities, and we suggest that this same mechanism explains reported observations of stimulated emission from inhomogeneously photopumped structures which previously have been interpreted as evidence for longitudinal optic (LO) phonon participation. We show that LO phonon participation cannot account for the photon energy of stimulated emission from conventional homogeneously pumped quantum well laser diodes.

Quantum theory of multiscale coarse-graining.

PubMed

Han, Yining; Jin, Jaehyeok; Wagner, Jacob W; Voth, Gregory A

2018-03-14

Coarse-grained (CG) models serve as a powerful tool to simulate molecular systems at much longer temporal and spatial scales. Previously, CG models and methods have been built upon classical statistical mechanics. The present paper develops a theory and numerical methodology for coarse-graining in quantum statistical mechanics, by generalizing the multiscale coarse-graining (MS-CG) method to quantum Boltzmann statistics. A rigorous derivation of the sufficient thermodynamic consistency condition is first presented via imaginary time Feynman path integrals. It identifies the optimal choice of CG action functional and effective quantum CG (qCG) force field to generate a quantum MS-CG (qMS-CG) description of the equilibrium system that is consistent with the quantum fine-grained model projected onto the CG variables. A variational principle then provides a class of algorithms for optimally approximating the qMS-CG force fields. Specifically, a variational method based on force matching, which was also adopted in the classical MS-CG theory, is generalized to quantum Boltzmann statistics. The qMS-CG numerical algorithms and practical issues in implementing this variational minimization procedure are also discussed. Then, two numerical examples are presented to demonstrate the method. Finally, as an alternative strategy, a quasi-classical approximation for the thermal density matrix expressed in the CG variables is derived. This approach provides an interesting physical picture for coarse-graining in quantum Boltzmann statistical mechanics in which the consistency with the quantum particle delocalization is obviously manifest, and it opens up an avenue for using path integral centroid-based effective classical force fields in a coarse-graining methodology.

A modified gradient approach for the growth of low-density InAs quantum dot molecules by molecular beam epitaxy

NASA Astrophysics Data System (ADS)

Sharma, Nandlal; Reuter, Dirk

2017-11-01

Two vertically stacked quantum dots that are electronically coupled, so called quantum dot molecules, are of great interest for the realization of solid state building blocks for quantum communication networks. We present a modified gradient approach to realize InAs quantum dot molecules with a low areal density so that single quantum dot molecules can be optically addressed. The individual quantum dot layers were prepared by solid source molecular beam epitaxy depositing InAs on GaAs(100). The bottom quantum dot layer has been grown without substrate rotation resulting in an In-gradient across the surface, which translated into a density gradient with low quantum dot density in a certain region of the wafer. For the top quantum dot layer, separated from the bottom quantum dot layer by a 6 nm thick GaAs barrier, various InAs amounts were deposited without an In-gradient. In spite of the absence of an In-gradient, a pronounced density gradient is observed for the top quantum dots. Even for an In-amount slightly below the critical thickness for a single dot layer, a density gradient in the top quantum dot layer, which seems to reproduce the density gradient in the bottom layer, is observed. For more or less In, respectively, deviations from this behavior occur. We suggest that the obvious influence of the bottom quantum dot layer on the growth of the top quantum dots is due to the strain field induced by the buried dots.

Quantum mechanical study of solvent effects in a prototype S{sub N}2 reaction in solution: Cl{sup −} attack on CH{sub 3}Cl

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

Kuechler, Erich R.; Department of Chemistry, University of Minnesota, Minneapolis, Minnesota 55455-0431; York, Darrin M., E-mail: york@biomaps.rutgers.edu

2014-02-07

The nucleophilic attack of a chloride ion on methyl chloride is an important prototype S{sub N}2 reaction in organic chemistry that is known to be sensitive to the effects of the surrounding solvent. Herein, we develop a highly accurate Specific Reaction Parameter (SRP) model based on the Austin Model 1 Hamiltonian for chlorine to study the effects of solvation into an aqueous environment on the reaction mechanism. To accomplish this task, we apply high-level quantum mechanical calculations to study the reaction in the gas phase and combined quantum mechanical/molecular mechanical simulations with TIP3P and TIP4P-ew water models and the resultingmore » free energy profiles are compared with those determined from simulations using other fast semi-empirical quantum models. Both gas phase and solution results with the SRP model agree very well with experiment and provide insight into the specific role of solvent on the reaction coordinate. Overall, the newly parameterized SRP Hamiltonian is able to reproduce both the gas phase and solution phase barriers, suggesting it is an accurate and robust model for simulations in the aqueous phase at greatly reduced computational cost relative to comparably accurate ab initio and density functional models.« less

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

NASA Astrophysics Data System (ADS)

Kuechler, Erich R.; York, Darrin M.

2014-02-01

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

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

PubMed

Kuechler, Erich R; York, Darrin M

2014-02-07

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

Parametric control in coupled fermionic oscillators

NASA Astrophysics Data System (ADS)

Ghosh, Arnab

2014-10-01

A simple model of parametric coupling between two fermionic oscillators is considered. Statistical properties, in particular the mean and variance of quanta for a single mode, are described by means of a time-dependent reduced density operator for the system and the associated P function. The density operator for fermionic fields as introduced by Cahill and Glauber [K. E. Cahill and R. J. Glauber, Phys. Rev. A 59, 1538 (1999), 10.1103/PhysRevA.59.1538] thus can be shown to provide a quantum mechanical description of the fields closely resembling their bosonic counterpart. In doing so, special emphasis is given to population trapping, and quantum control over the states of the system.

Quantum mechanical/molecular mechanical/continuum style solvation model: second order Møller-Plesset perturbation theory.

PubMed

Thellamurege, Nandun M; Si, Dejun; Cui, Fengchao; Li, Hui

2014-05-07

A combined quantum mechanical/molecular mechanical/continuum (QM/MM/C) style second order Møller-Plesset perturbation theory (MP2) method that incorporates induced dipole polarizable force field and induced surface charge continuum solvation model is established. The Z-vector method is modified to include induced dipoles and induced surface charges to determine the MP2 response density matrix, which can be used to evaluate MP2 properties. In particular, analytic nuclear gradient is derived and implemented for this method. Using the Assisted Model Building with Energy Refinement induced dipole polarizable protein force field, the QM/MM/C style MP2 method is used to study the hydrogen bonding distances and strengths of the photoactive yellow protein chromopore in the wild type and the Glu46Gln mutant.

Nonuniform quantum turbulence in superfluids

NASA Astrophysics Data System (ADS)

Nemirovskii, Sergey K.

2018-04-01

The problem of quantum turbulence in a channel with an inhomogeneous counterflow of superfluid turbulent helium is studied. The counterflow velocity Vns x(y ) along the channel is supposed to have a parabolic profile in the transverse direction y . Such statement corresponds to the recent numerical simulation by Khomenko et al. [Phys. Rev. B 91, 180504 (2015), 10.1103/PhysRevB.91.180504]. The authors reported about a sophisticated behavior of the vortex-line density (VLD) L (r ,t ) , different from L ∝Vns x(y) 2 , which follows from the straightforward application of the conventional Vinen theory. It is clear that Vinen theory should be refined by taking into account transverse effects, and the way it ought to be done is the subject of active discussion in the literature. In this work, we discuss several possible mechanisms of the transverse flux of VLD L (r ,t ) which should be incorporated in the standard Vinen equation to describe adequately the inhomogeneous quantum turbulence. It is shown that the most effective among these mechanisms is the one that is related to the phase-slippage phenomenon. The use of this flux in the modernized Vinen equation corrects the situation with an unusual distribution of the vortex-line density, and satisfactorily describes the behavior L (r ,t ) both in stationary and nonstationary situations. The general problem of the phenomenological Vinen theory in the case of nonuniform and nonstationary quantum turbulence is thoroughly discussed.

Quantum-classical correspondence for the inverted oscillator

NASA Astrophysics Data System (ADS)

Maamache, Mustapha; Ryeol Choi, Jeong

2017-11-01

While quantum-classical correspondence for a system is a very fundamental problem in modern physics, the understanding of its mechanism is often elusive, so the methods used and the results of detailed theoretical analysis have been accompanied by active debate. In this study, the differences and similarities between quantum and classical behavior for an inverted oscillator have been analyzed based on the description of a complete generalized Airy function-type quantum wave solution. The inverted oscillator model plays an important role in several branches of cosmology and particle physics. The quantum wave packet of the system is composed of many sub-packets that are localized at different positions with regular intervals between them. It is shown from illustrations of the probability density that, although the quantum trajectory of the wave propagation is somewhat different from the corresponding classical one, the difference becomes relatively small when the classical excitation is sufficiently high. We have confirmed that a quantum wave packet moving along a positive or negative direction accelerates over time like a classical wave. From these main interpretations and others in the text, we conclude that our theory exquisitely illustrates quantum and classical correspondence for the system, which is a crucial concept in quantum mechanics. Supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (NRF-2016R1D1A1A09919503)

Growth of low disorder GaAs/AlGaAs heterostructures by molecular beam epitaxy for the study of correlated electron phases in two dimensions

NASA Astrophysics Data System (ADS)

Watson, John D.

The unparalleled quality of GaAs/AlGaAs heterostructures grown by molecular beam epitaxy has enabled a wide range of experiments probing interaction effects in two-dimensional electron and hole gases. This dissertation presents work aimed at further understanding the key material-related issues currently limiting the quality of these 2D systems, particularly in relation to the fractional quantum Hall effect in the 2nd Landau level and spin-based implementations of quantum computation. The manuscript begins with a theoretical introduction to the quantum Hall effect which outlines the experimental conditions necessary to study the physics of interest and motivates the use of the semiconductor growth and cryogenic measurement techniques outlined in chapters 2 and 3, respectively. In addition to a generic introduction to the molecular beam epitaxy growth technique, chapter 2 summarizes some of what was learned about the material purity issues currently limiting the low temperature electron mobility. Finally, a series of appendices are included which detail the experimental methods used over the course of the research. Chapter 4 presents an experiment examining transport in a low density two-dimensional hole system in which the hole density could be varied by means of an evaporated back gate. At low temperature, the mobility reached a maximum of 2.6 x 106 cm2/Vs at a density of 6.2 x 1010 cm-2 which is the highest reported mobility in a two-dimensional hole system to date. In addition, it was found that the mobility as a function of density did not follow a power law with a single exponent. Instead, it was found that the power law varied with density, indicating a cross-over between dominant scattering mechanisms at low density and high density. At low density the mobility was found to be limited by remote ionized impurity scattering, while at high density the dominant scattering mechanism was found to be background impurity scattering. Chapter 5 details an experiment examining transport in a series of two-dimensional hole gases in which the dopant setback distance and the Al mole fraction in the barriers of the quantum well were varied. The hole density was tuned in this way from 0.18 -- 1.9 x 1011 cm-2. Surprisingly, the mobility at T = 0.3 K was found to peak at 2.3 x 10 6 cm-2 at an intermediate density of 6.5 x 10 10 cm-2. Self-consistent Schrodinger/Poisson calculations were performed for each wafer to examine the scattering rates due to a variety of potentials at low temperature. The drop in mobility at high density could be accounted for with the inclusion of interface roughness scattering, but using the same interface roughness scattering parameters for similar two-dimensional electron gases produced inconsistent results. This leaves open the possibility of contributions from other scattering mechanisms in the hole samples at high density. Chapter 6 presents an in-depth study of in-situ backgated two-dimensional gases used for studying the fragile fractional quantum Hall states in the 2nd Landau level. It was found that leakage currents as small as 4 pA could cause noticeable heating of the electron gas if the lattice was not properly thermally anchored to the cryostat. However, it was also found that when the heterostructure design and device fabrication recipe were properly optimized, gate voltages as large as 4 V could be applied before the leakage turned on, allowing the density to be tuned from full depletion to over 4 x 1011 cm-2. As a result, heating effects at dilution refrigerator temperatures were negligible and the gap at nu = 5/2 could be tuned continuously with density to a maximum value of 625 mK, the largest reported to date. An unusual evolution of the reentrant integer quantum Hall states as a function of density is also reported. Such devices should prove useful for the study of electron correlations in nanostructures in the 2nd Landau level.

Multicomponent density functional theory embedding formulation.

PubMed

Culpitt, Tanner; Brorsen, Kurt R; Pak, Michael V; Hammes-Schiffer, Sharon

2016-07-28

Multicomponent density functional theory (DFT) methods have been developed to treat two types of particles, such as electrons and nuclei, quantum mechanically at the same level. In the nuclear-electronic orbital (NEO) approach, all electrons and select nuclei, typically key protons, are treated quantum mechanically. For multicomponent DFT methods developed within the NEO framework, electron-proton correlation functionals based on explicitly correlated wavefunctions have been designed and used in conjunction with well-established electronic exchange-correlation functionals. Herein a general theory for multicomponent embedded DFT is developed to enable the accurate treatment of larger systems. In the general theory, the total electronic density is separated into two subsystem densities, denoted as regular and special, and different electron-proton correlation functionals are used for these two electronic densities. In the specific implementation, the special electron density is defined in terms of spatially localized Kohn-Sham electronic orbitals, and electron-proton correlation is included only for the special electron density. The electron-proton correlation functional depends on only the special electron density and the proton density, whereas the electronic exchange-correlation functional depends on the total electronic density. This scheme includes the essential electron-proton correlation, which is a relatively local effect, as well as the electronic exchange-correlation for the entire system. This multicomponent DFT-in-DFT embedding theory is applied to the HCN and FHF(-) molecules in conjunction with two different electron-proton correlation functionals and three different electronic exchange-correlation functionals. The results illustrate that this approach provides qualitatively accurate nuclear densities in a computationally tractable manner. The general theory is also easily extended to other types of partitioning schemes for multicomponent systems.

Multicomponent density functional theory embedding formulation

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

Culpitt, Tanner; Brorsen, Kurt R.; Pak, Michael V.

Multicomponent density functional theory (DFT) methods have been developed to treat two types of particles, such as electrons and nuclei, quantum mechanically at the same level. In the nuclear-electronic orbital (NEO) approach, all electrons and select nuclei, typically key protons, are treated quantum mechanically. For multicomponent DFT methods developed within the NEO framework, electron-proton correlation functionals based on explicitly correlated wavefunctions have been designed and used in conjunction with well-established electronic exchange-correlation functionals. Herein a general theory for multicomponent embedded DFT is developed to enable the accurate treatment of larger systems. In the general theory, the total electronic density ismore » separated into two subsystem densities, denoted as regular and special, and different electron-proton correlation functionals are used for these two electronic densities. In the specific implementation, the special electron density is defined in terms of spatially localized Kohn-Sham electronic orbitals, and electron-proton correlation is included only for the special electron density. The electron-proton correlation functional depends on only the special electron density and the proton density, whereas the electronic exchange-correlation functional depends on the total electronic density. This scheme includes the essential electron-proton correlation, which is a relatively local effect, as well as the electronic exchange-correlation for the entire system. This multicomponent DFT-in-DFT embedding theory is applied to the HCN and FHF{sup −} molecules in conjunction with two different electron-proton correlation functionals and three different electronic exchange-correlation functionals. The results illustrate that this approach provides qualitatively accurate nuclear densities in a computationally tractable manner. The general theory is also easily extended to other types of partitioning schemes for multicomponent systems.« less

Quantum nonlocality does not exist

PubMed Central

Tipler, Frank J.

2014-01-01

Quantum nonlocality is shown to be an artifact of the Copenhagen interpretation, in which each observed quantity has exactly one value at any instant. In reality, all physical systems obey quantum mechanics, which obeys no such rule. Locality is restored if observed and observer are both assumed to obey quantum mechanics, as in the many-worlds interpretation (MWI). Using the MWI, I show that the quantum side of Bell’s inequality, generally believed nonlocal, is really due to a series of three measurements (not two as in the standard, oversimplified analysis), all three of which have only local effects. Thus, experiments confirming “nonlocality” are actually confirming the MWI. The mistaken interpretation of nonlocality experiments depends crucially on a question-begging version of the Born interpretation, which makes sense only in “collapse” versions of quantum theory, about the meaning of the modulus of the wave function, so I use the interpretation based on the MWI, namely that the wave function is a world density amplitude, not a probability amplitude. This view allows the Born interpretation to be derived directly from the Schrödinger equation, by applying the Schrödinger equation to both the observed and the observer. PMID:25015084

Quantum nonlocality does not exist.

PubMed

Tipler, Frank J

2014-08-05

Quantum nonlocality is shown to be an artifact of the Copenhagen interpretation, in which each observed quantity has exactly one value at any instant. In reality, all physical systems obey quantum mechanics, which obeys no such rule. Locality is restored if observed and observer are both assumed to obey quantum mechanics, as in the many-worlds interpretation (MWI). Using the MWI, I show that the quantum side of Bell's inequality, generally believed nonlocal, is really due to a series of three measurements (not two as in the standard, oversimplified analysis), all three of which have only local effects. Thus, experiments confirming "nonlocality" are actually confirming the MWI. The mistaken interpretation of nonlocality experiments depends crucially on a question-begging version of the Born interpretation, which makes sense only in "collapse" versions of quantum theory, about the meaning of the modulus of the wave function, so I use the interpretation based on the MWI, namely that the wave function is a world density amplitude, not a probability amplitude. This view allows the Born interpretation to be derived directly from the Schrödinger equation, by applying the Schrödinger equation to both the observed and the observer.

Vibrational Properties of Hydrogen-Bonded Systems Using the Multireference Generalization to the "On-the-Fly" Electronic Structure within Quantum Wavepacket ab Initio Molecular Dynamics (QWAIMD).

PubMed

Li, Junjie; Li, Xiaohu; Iyengar, Srinivasan S

2014-06-10

We discuss a multiconfigurational treatment of the "on-the-fly" electronic structure within the quantum wavepacket ab initio molecular dynamics (QWAIMD) method for coupled treatment of quantum nuclear effects with electronic structural effects. Here, multiple single-particle electronic density matrices are simultaneously propagated with a quantum nuclear wavepacket and other classical nuclear degrees of freedom. The multiple density matrices are coupled through a nonorthogonal configuration interaction (NOCI) procedure to construct the instantaneous potential surface. An adaptive-mesh-guided set of basis functions composed of Gaussian primitives are used to simplify the electronic structure calculations. Specifically, with the replacement of the atom-centered basis functions positioned on the centers of the quantum-mechanically treated nuclei by a mesh-guided band of basis functions, the two-electron integrals used to compute the electronic structure potential surface become independent of the quantum nuclear variable and hence reusable along the entire Cartesian grid representing the quantum nuclear coordinates. This reduces the computational complexity involved in obtaining a potential surface and facilitates the interpretation of the individual density matrices as representative diabatic states. The parametric nuclear position dependence of the diabatic states is evaluated at the initial time-step using a Shannon-entropy-based sampling function that depends on an approximation to the quantum nuclear wavepacket and the potential surface. This development is meant as a precursor to an on-the-fly fully multireference electronic structure procedure embedded, on-the-fly, within a quantum nuclear dynamics formalism. We benchmark the current development by computing structural, dynamic, and spectroscopic features for a series of bihalide hydrogen-bonded systems: FHF(-), ClHCl(-), BrHBr(-), and BrHCl(-). We find that the donor-acceptor structural features are in good agreement with experiments. Spectroscopic features are computed using a unified velocity/flux autocorrelation function and include vibrational fundamentals and combination bands. These agree well with experiments and other theories.

Quantum chi-squared and goodness of fit testing

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

Temme, Kristan; Verstraete, Frank

2015-01-15

A quantum mechanical hypothesis test is presented for the hypothesis that a certain setup produces a given quantum state. Although the classical and the quantum problems are very much related to each other, the quantum problem is much richer due to the additional optimization over the measurement basis. A goodness of fit test for i.i.d quantum states is developed and a max-min characterization for the optimal measurement is introduced. We find the quantum measurement which leads both to the maximal Pitman and Bahadur efficiencies, and determine the associated divergence rates. We discuss the relationship of the quantum goodness of fitmore » test to the problem of estimating multiple parameters from a density matrix. These problems are found to be closely related and we show that the largest error of an optimal strategy, determined by the smallest eigenvalue of the Fisher information matrix, is given by the divergence rate of the goodness of fit test.« less

A Static and Dynamic Investigation of Quantum Nonlinear Transport in Highly Dense and Mobile 2D Electron Systems

NASA Astrophysics Data System (ADS)

Dietrich, Scott

Heterostructures made of semiconductor materials may be one of most versatile environments for the study of the physics of electron transport in two dimensions. These systems are highly customizable and demonstrate a wide range of interesting physical phenomena. In response to both microwave radiation and DC excitations, strongly nonlinear transport that gives rise to non-equilibrium electron states has been reported and investigated. We have studied GaAs quantum wells with a high density of high mobility two-dimensional electrons placed in a quantizing magnetic field. This study presents the observation of several nonlinear transport mechanisms produced by the quantum nature of these materials. The quantum scattering rate, 1tau/q, is an important parameter in these systems, defining the width of the quantized energy levels. Traditional methods of extracting 1tau/q involve studying the amplitude of Shubnikov-de Haas oscillations. We analyze the quantum positive magnetoresistance due to the cyclotron motion of electrons in a magnetic field. This method gives 1tau/q and has the additional benefit of providing access to the strength of electron-electron interactions, which is not possible by conventional techniques. The temperature dependence of the quantum scattering rate is found to be proportional to the square of the temperature and is in very good agreement with theory that considers electron-electron interactions in 2D systems. In quantum wells with a small scattering rate - which corresponds to well-defined Landau levels - quantum oscillations of nonlinear resistance that are independent of magnetic field strength have been observed. These oscillations are periodic in applied bias current and are connected to quantum oscillations of resistance at zero bias: either Shubnikov-de Haas oscillations for single subband systems or magnetointersubband oscillations for two subband systems. The bias-induced oscillations can be explained by a spatial variation of electron density across the sample. The theoretical model predicts the period of these oscillations to depend on the total electron density, which has been confirmed by controlling the density through a voltage top-gate on the sample. The peculiar nonlinear mechanism of quantal heating has garned much attention recently. This bulk phenomenon is a quantum manifestation of Joule heating where an applied bias current causes selective flattening in the electron distribution function but conserves overall broadening. This produces a highly non-equilibrium distribution of electrons that drastically effects the transport properties of the system. Recent studies have proposed contributions from edge states and/or skipping orbitals. We have shown that these contributions are minimal by studying the transition to the zero differential conductance state and comparing results between Hall and Corbino geometries. This demonstrated quantal heating as the dominant nonlinear mechanism in these systems. To study the dynamics of quantal heating, we applied microwave radiation simultaneously from two sources at frequencies ƒ1 and ƒ2 and measured the response of the system at the difference frequency, ƒ=|ƒ 1-ƒ2|. This provides direct access to the rate of inelastic scattering processes, 1tau/in, that tend to bring the electron distribution back to thermal equilibrium. While conventional measurements of the temperature dependence indicate that 1tau/in is proportional to temperature, recent DC investigations and our new dynamic measurements show either T2 or T3 dependence in different magnetic fields. Our microwave experiment is the first direct access to the inelastic relaxation rate and confirms the non-linear temperature dependence.

Explaining electric conductivity using the particle-in-a-box model: quantum superposition is the key

NASA Astrophysics Data System (ADS)

Sivanesan, Umaseh; Tsang, Kin; Izmaylov, Artur F.

2017-12-01

Most of the textbooks explaining electric conductivity in the context of quantum mechanics provide either incomplete or semi-classical explanations that are not connected with the elementary concepts of quantum mechanics. We illustrate the conduction phenomena using the simplest model system in quantum dynamics, a particle in a box (PIB). To induce the particle dynamics, a linear potential tilting the bottom of the box is introduced, which is equivalent to imposing a constant electric field for a charged particle. Although the PIB model represents a closed system that cannot have a flow of electrons through the system, we consider the oscillatory dynamics of the particle probability density as the analogue of the electric current. Relating the amplitude and other parameters of the particle oscillatory dynamics with the gap between the ground and excited states of the PIB model allows us to demonstrate one of the most basic dependencies of electric conductivity on the valence-conduction band gap of the material.

Periodic Toda lattice in quantum mechanics

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

Matsuyama, A.

The quantum mechanical periodic Toda lattice is studied by the direct diagonalization of the Hamiltonian. The eigenstates are classified according to the irreducible representations of the dihedral group D[sub N]. It is shown that Gutzwiller's quantization conditions are satisfied and they have a one-to-one correspondence to the irreducible representation of the D[sub N] group. The authors have also carried out the semiclassical quantization of the periodic Toda lattice by the EBK formulation. The eigenvalues of the semiclassical quantization have a one-to-one correspondence to the integer quantum numbers, and those quantum numbers also have a close relationship to the symmetry ofmore » the state. Numerical calculations have been done for N = 3, 4, 5, and 6 particle periodic Toda lattices. The distributions of the eigenvalues are systematic and distinguished by the symmetry of the state. As illustrative examples, amplitudes of the wave functions and density distributions are shown. 14 refs., 8 figs., 11 tabs.« less

Quantum mechanical force field for hydrogen fluoride with explicit electronic polarization.

PubMed

Mazack, Michael J M; Gao, Jiali

2014-05-28

The explicit polarization (X-Pol) theory is a fragment-based quantum chemical method that explicitly models the internal electronic polarization and intermolecular interactions of a chemical system. X-Pol theory provides a framework to construct a quantum mechanical force field, which we have extended to liquid hydrogen fluoride (HF) in this work. The parameterization, called XPHF, is built upon the same formalism introduced for the XP3P model of liquid water, which is based on the polarized molecular orbital (PMO) semiempirical quantum chemistry method and the dipole-preserving polarization consistent point charge model. We introduce a fluorine parameter set for PMO, and find good agreement for various gas-phase results of small HF clusters compared to experiments and ab initio calculations at the M06-2X/MG3S level of theory. In addition, the XPHF model shows reasonable agreement with experiments for a variety of structural and thermodynamic properties in the liquid state, including radial distribution functions, interaction energies, diffusion coefficients, and densities at various state points.

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.

Equivalent Quantum Equations in a System Inspired by Bouncing Droplets Experiments

NASA Astrophysics Data System (ADS)

Borghesi, Christian

2017-07-01

In this paper we study a classical and theoretical system which consists of an elastic medium carrying transverse waves and one point-like high elastic medium density, called concretion. We compute the equation of motion for the concretion as well as the wave equation of this system. Afterwards we always consider the case where the concretion is not the wave source any longer. Then the concretion obeys a general and covariant guidance formula, which leads in low-velocity approximation to an equivalent de Broglie-Bohm guidance formula. The concretion moves then as if exists an equivalent quantum potential. A strictly equivalent free Schrödinger equation is retrieved, as well as the quantum stationary states in a linear or spherical cavity. We compute the energy (and momentum) of the concretion, naturally defined from the energy (and momentum) density of the vibrating elastic medium. Provided one condition about the amplitude of oscillation is fulfilled, it strikingly appears that the energy and momentum of the concretion not only are written in the same form as in quantum mechanics, but also encapsulate equivalent relativistic formulas.

On the theory of quantum measurement

NASA Technical Reports Server (NTRS)

Haus, Hermann A.; Kaertner, Franz X.

1994-01-01

Many so called paradoxes of quantum mechanics are clarified when the measurement equipment is treated as a quantized system. Every measurement involves nonlinear processes. Self consistent formulations of nonlinear quantum optics are relatively simple. Hence optical measurements, such as the quantum nondemolition (QND) measurement of photon number, are particularly well suited for such a treatment. It shows that the so called 'collapse of the wave function' is not needed for the interpretation of the measurement process. Coherence of the density matrix of the signal is progressively reduced with increasing accuracy of the photon number determination. If the QND measurement is incorporated into the double slit experiment, the contrast ratio of the fringes is found to decrease with increasing information on the photon number in one of the two paths.

Free-energy analysis of the electron-density fluctuation in the quantum-mechanical/molecular-mechanical simulation combined with the theory of energy representation.

PubMed

Matubayasi, Nobuyuki; Takahashi, Hideaki

2012-01-28

The relationship is investigated for QM/MM (quantum-mechanical/molecular-mechanical) systems between the fluctuations of the electronic state of the QM subsystem and of the solvation effect due to the QM-MM interaction. The free-energy change due to the electron-density fluctuation around its average is highlighted, and is evaluated through an approximate functional formulated in terms of distribution functions of the many-body coupling (pairwise non-additive) part of the QM-MM interaction energy. A set of QM/MM simulations are conducted in MM water solvent for QM water solute in ambient and supercritical conditions and for QM glycine solute in the neutral and zwitterionic forms. The variation of the electronic distortion energy of the QM solute in the course of QM/MM simulation is then shown to be compensated by the corresponding variation of the free energy of solvation. The solvation free energy conditioned by the electronic distortion energy is further analyzed with its components. It is found that the many-body contribution is essentially equal between the free energy and the average sum of solute-solvent interaction energy. © 2012 American Institute of Physics

Use of the Lorentz-operator in relativistic quantum mechanics to guarentee a single-energy root

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

Ritchie, A B

1998-08-01

The Lorentz-operator form of relativistic quantum mechanics, with relativistic wave equation i{h_bar}{partial_derivative}{psi}/{partial_derivative}t=(mc{sup 2}{gamma}+e{Phi}){psi}, is implemented to guarantee a single-energy root. The Lorentz factor as modified by Pauli's ansatz is given by {gamma}={radical}1+[{rvec {sigma}}{center_dot}(i{h_bar}{rvec {del}}+(e/c){rvec A})]{sup 2}/m{sup 2}c{sup 2}, such that the theory is appropriate for electrons. Magnetic fine structure in the Lorentz relativistic wave equation emerges on the use of an appropriate operator form of the Lienard-Wiechert four- potential ({Phi},{rvec A}) from electromagnetic theory. Although computationally more intensive the advantage of the theory is the elimination of the negative-root of the energy and an interpretation of the wave function basedmore » on a one-particle, positive definite probability density like that of nonrelativistic quantum mechanics.« less

Ab initio molecular dynamics with nuclear quantum effects at classical cost: Ring polymer contraction for density functional theory

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

Marsalek, Ondrej; Markland, Thomas E., E-mail: tmarkland@stanford.edu

Path integral molecular dynamics simulations, combined with an ab initio evaluation of interactions using electronic structure theory, incorporate the quantum mechanical nature of both the electrons and nuclei, which are essential to accurately describe systems containing light nuclei. However, path integral simulations have traditionally required a computational cost around two orders of magnitude greater than treating the nuclei classically, making them prohibitively costly for most applications. Here we show that the cost of path integral simulations can be dramatically reduced by extending our ring polymer contraction approach to ab initio molecular dynamics simulations. By using density functional tight binding asmore » a reference system, we show that our ring polymer contraction scheme gives rapid and systematic convergence to the full path integral density functional theory result. We demonstrate the efficiency of this approach in ab initio simulations of liquid water and the reactive protonated and deprotonated water dimer systems. We find that the vast majority of the nuclear quantum effects are accurately captured using contraction to just the ring polymer centroid, which requires the same number of density functional theory calculations as a classical simulation. Combined with a multiple time step scheme using the same reference system, which allows the time step to be increased, this approach is as fast as a typical classical ab initio molecular dynamics simulation and 35× faster than a full path integral calculation, while still exactly including the quantum sampling of nuclei. This development thus offers a route to routinely include nuclear quantum effects in ab initio molecular dynamics simulations at negligible computational cost.« less

Induced Angular Momentum

ERIC Educational Resources Information Center

Parker, G. W.

1978-01-01

Discusses, classically and quantum mechanically, the angular momentum induced in the bound motion of an electron by an external magnetic field. Calculates the current density and its magnetic moment, and then uses two methods to solve the first-order perturbation theory equation for the required eigenfunction. (Author/GA)

Cobalt-doped ZnO nanocrystals: quantum confinement and surface effects from ab initio methods.

PubMed

Schoenhalz, Aline L; Dalpian, Gustavo M

2013-10-14

Cobalt-doped ZnO nanocrystals were studied through ab initio methods based on the Density Functional Theory. Both quantum confinement and surface effects were explicitly taken into account. When only quantum confinement effects are considered, Co atoms interact through a superexchange mechanism, stabilizing an antiferromagnetic ground state. Usually, this is the case for high quality nanoparticles with perfect surface saturation. When the surfaces were considered, a strong hybridization between the Co atoms and surfaces was observed, strongly changing their electronic and magnetic properties. Our results indicated that the surfaces might qualitatively change the properties of impurities in semiconductor nanocrystals.

Noncommuting observables in quantum detection and estimation theory

NASA Technical Reports Server (NTRS)

Helstrom, C. W.

1972-01-01

Basing decisions and estimates on simultaneous approximate measurements of noncommuting observables in a quantum receiver is shown to be equivalent to measuring commuting projection operators on a larger Hilbert space than that of the receiver itself. The quantum-mechanical Cramer-Rao inequalities derived from right logarithmic derivatives and symmetrized logarithmic derivatives of the density operator are compared, and it is shown that the latter give superior lower bounds on the error variances of individual unbiased estimates of arrival time and carrier frequency of a coherent signal. For a suitably weighted sum of the error variances of simultaneous estimates of these, the former yield the superior lower bound under some conditions.

Electron acceleration in quantum plasma with spin-up and spin-down exchange interaction

NASA Astrophysics Data System (ADS)

Kumar, Punit; Singh, Shiv; Ahmad, Nafees

2018-05-01

Electron acceleration by ponderomotive force of an intense circularly polarized laser pulse in high density magnetized quantum plasma with two different spin states embedded in external static magnetic field. The basic mechanism involves electron acceleration by axial gradient in the ponderomotive potential of laser. The effects of Bohm potential, fermi pressure and intrinsic spin of electron have been taken into account. A simple solution for ponderomotive electron acceleration has been established and effect of spin polarization is analyzed.

Quantum mechanical/molecular mechanical/continuum style solvation model: Second order Møller-Plesset perturbation theory

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

Thellamurege, Nandun M.; Si, Dejun; Cui, Fengchao

A combined quantum mechanical/molecular mechanical/continuum (QM/MM/C) style second order Møller-Plesset perturbation theory (MP2) method that incorporates induced dipole polarizable force field and induced surface charge continuum solvation model is established. The Z-vector method is modified to include induced dipoles and induced surface charges to determine the MP2 response density matrix, which can be used to evaluate MP2 properties. In particular, analytic nuclear gradient is derived and implemented for this method. Using the Assisted Model Building with Energy Refinement induced dipole polarizable protein force field, the QM/MM/C style MP2 method is used to study the hydrogen bonding distances and strengths ofmore » the photoactive yellow protein chromopore in the wild type and the Glu46Gln mutant.« less

Higher-Order Interference in Extensions of Quantum Theory

NASA Astrophysics Data System (ADS)

Lee, Ciarán M.; Selby, John H.

2017-01-01

Quantum interference, manifest in the two slit experiment, lies at the heart of several quantum computational speed-ups and provides a striking example of a quantum phenomenon with no classical counterpart. An intriguing feature of quantum interference arises in a variant of the standard two slit experiment, in which there are three, rather than two, slits. The interference pattern in this set-up can be written in terms of the two and one slit patterns obtained by blocking one, or more, of the slits. This is in stark contrast with the standard two slit experiment, where the interference pattern cannot be written as a sum of the one slit patterns. This was first noted by Rafael Sorkin, who raised the question of why quantum theory only exhibits irreducible interference in the two slit experiment. One approach to this problem is to compare the predictions of quantum theory to those of operationally-defined `foil' theories, in the hope of determining whether theories that do exhibit higher-order interference suffer from pathological—or at least undesirable—features. In this paper two proposed extensions of quantum theory are considered: the theory of Density Cubes proposed by Dakić, Paterek and Brukner, which has been shown to exhibit irreducible interference in the three slit set-up, and the Quartic Quantum Theory of Życzkowski. The theory of Density Cubes will be shown to provide an advantage over quantum theory in a certain computational task and to posses a well-defined mechanism which leads to the emergence of quantum theory—analogous to the emergence of classical physics from quantum theory via decoherence. Despite this, the axioms used to define Density Cubes will be shown to be insufficient to uniquely characterise the theory. In comparison, Quartic Quantum Theory is a well-defined theory and we demonstrate that it exhibits irreducible interference to all orders. This feature of Życzkowski's theory is argued not to be a genuine phenomenon, but to arise from an ambiguity in the current definition of higher-order interference in operationally-defined theories. Thus, to begin to understand why quantum theory is limited to a certain kind of interference, a new definition of higher-order interference is needed that is applicable to, and makes good operational sense in, arbitrary operationally-defined theories.

Prediction of molecular crystal structures by a crystallographic QM/MM model with full space-group symmetry.

PubMed

Mörschel, Philipp; Schmidt, Martin U

2015-01-01

A crystallographic quantum-mechanical/molecular-mechanical model (c-QM/MM model) with full space-group symmetry has been developed for molecular crystals. The lattice energy was calculated by quantum-mechanical methods for short-range interactions and force-field methods for long-range interactions. The quantum-mechanical calculations covered the interactions within the molecule and the interactions of a reference molecule with each of the surrounding 12-15 molecules. The interactions with all other molecules were treated by force-field methods. In each optimization step the energies in the QM and MM shells were calculated separately as single-point energies; after adding both energy contributions, the crystal structure (including the lattice parameters) was optimized accordingly. The space-group symmetry was maintained throughout. Crystal structures with more than one molecule per asymmetric unit, e.g. structures with Z' = 2, hydrates and solvates, have been optimized as well. Test calculations with different quantum-mechanical methods on nine small organic molecules revealed that the density functional theory methods with dispersion correction using the B97-D functional with 6-31G* basis set in combination with the DREIDING force field reproduced the experimental crystal structures with good accuracy. Subsequently the c-QM/MM method was applied to nine compounds from the CCDC blind tests resulting in good energy rankings and excellent geometric accuracies.

Correlated evolution of structure and mechanical loss of a sputtered silica film

NASA Astrophysics Data System (ADS)

Granata, Massimo; Coillet, Elodie; Martinez, Valérie; Dolique, Vincent; Amato, Alex; Canepa, Maurizio; Margueritat, Jérémie; Martinet, Christine; Mermet, Alain; Michel, Christophe; Pinard, Laurent; Sassolas, Benoît; Cagnoli, Gianpietro

2018-05-01

Energy dissipation in amorphous coatings severely affects high-precision optical and quantum transducers. In order to isolate the source of coating loss, we performed an extensive study of Raman scattering and mechanical loss of a thermally treated sputtered silica coating. Our results show that loss is correlated with the population of three-membered rings of Si-O4 tetrahedral units and support the evidence that thermal treatment reduces the density of metastable states separated by a characteristic energy of about 0.5 eV in favor of an increase of the density of states separated by smaller activation energies.

Atomic Calculations with a One-Parameter, Single Integral Method.

ERIC Educational Resources Information Center

Baretty, Reinaldo; Garcia, Carmelo

1989-01-01

Presents an energy function E(p) containing a single integral and one variational parameter, alpha. Represents all two-electron integrals within the local density approximation as a single integral. Identifies this as a simple treatment for use in an introductory quantum mechanics course. (MVL)

Universal core model for multiple-gate field-effect transistors with short channel and quantum mechanical effects

NASA Astrophysics Data System (ADS)

Shin, Yong Hyeon; Bae, Min Soo; Park, Chuntaek; Park, Joung Won; Park, Hyunwoo; Lee, Yong Ju; Yun, Ilgu

2018-06-01

A universal core model for multiple-gate (MG) field-effect transistors (FETs) with short channel effects (SCEs) and quantum mechanical effects (QMEs) is proposed. By using a Young’s approximation based solution for one-dimensional Poisson’s equations the total inversion charge density (Q inv ) in the channel is modeled for double-gate (DG) and surrounding-gate SG (SG) FETs, following which a universal charge model is derived based on the similarity of the solutions, including for quadruple-gate (QG) FETs. For triple-gate (TG) FETs, the average of DG and QG FETs are used. A SCEs model is also proposed considering the potential difference between the channel’s surface and center. Finally, a QMEs model for MG FETs is developed using the quantum correction compact model. The proposed universal core model is validated on commercially available three-dimensional ATLAS numerical simulations.

Quantum chemical modeling of enzymatic reactions: the case of 4-oxalocrotonate tautomerase.

PubMed

Sevastik, Robin; Himo, Fahmi

2007-12-01

The reaction mechanism of 4-oxalocrotonate tautomerase (4-OT) is studied using the density functional theory method B3LYP. This enzyme catalyzes the isomerisation of unconjugated alpha-keto acids to their conjugated isomers. Two different quantum chemical models of the active site are devised and the potential energy curves for the reaction are computed. The calculations support the proposed reaction mechanism in which Pro-1 acts as a base to shuttle a proton from the C3 to the C5 position of the substrate. The first step (proton transfer from C3 to proline) is shown to be the rate-limiting step. The energy of the charge-separated intermediate (protonated proline-deprotonated substrate) is calculated to be quite low, in accordance with measured pKa values. The results of the two models are used to evaluate the methodology employed in modeling enzyme active sites using quantum chemical cluster models.

NMR lineshape equations for hindered methyl group: a comparison of the semi-classical and quantum mechanical models

NASA Astrophysics Data System (ADS)

Bernatowicz, P.; Szymański, S.

2003-09-01

The semiclassical and quantum mechanical NMR lineshape equations for a hindered methyl group are compared. In both the approaches, the stochastic dynamics can be interpreted in terms of a progressive symmetrization of the spin density matrix. However, the respective ways of achieving the same limiting symmetry can be remarkably different. From numerical lineshape simulations it is inferred that in the regime of intermediate exchange, where the conventional theory predicts occurrence of a single Lorentzian, the actual spectrum can have nontrivial features. This observation may open new perspectives in the search for nonclassical effects in the stochastic behavior of methyl groups in liquid-phase NMR.

Multipolar Ewald methods, 1: theory, accuracy, and performance.

PubMed

Giese, Timothy J; Panteva, Maria T; Chen, Haoyuan; York, Darrin M

2015-02-10

The Ewald, Particle Mesh Ewald (PME), and Fast Fourier–Poisson (FFP) methods are developed for systems composed of spherical multipole moment expansions. A unified set of equations is derived that takes advantage of a spherical tensor gradient operator formalism in both real space and reciprocal space to allow extension to arbitrary multipole order. The implementation of these methods into a novel linear-scaling modified “divide-and-conquer” (mDC) quantum mechanical force field is discussed. The evaluation times and relative force errors are compared between the three methods, as a function of multipole expansion order. Timings and errors are also compared within the context of the quantum mechanical force field, which encounters primary errors related to the quality of reproducing electrostatic forces for a given density matrix and secondary errors resulting from the propagation of the approximate electrostatics into the self-consistent field procedure, which yields a converged, variational, but nonetheless approximate density matrix. Condensed-phase simulations of an mDC water model are performed with the multipolar PME method and compared to an electrostatic cutoff method, which is shown to artificially increase the density of water and heat of vaporization relative to full electrostatic treatment.

Scattering mechanisms in shallow undoped Si/SiGe quantum wells

NASA Astrophysics Data System (ADS)

Laroche, Dominique; Huang, Shih-Hsien; Nielsen, Erik; Chuang, Yen; Li, Jiun-Yun; Liu, Chih-Wen; Lu, Tzu-Ming

We report the magneto-transport and scattering mechanism analysis of a series of increasingly shallow Si/SiGe quantum wells with the shallowest 2DEG located only ~ 10 nm away from the surface. The peak mobility increases with increasing depth, suggesting that charge centers near the oxide/semiconductor interface is the main source of disorder. The power-law exponent of the mobility versus density curve, μ ~nα , is extracted as a function of the depth. At intermediate densities, the power-law dependence is characterized by α ~ 2 . 3 while at the highest achievable densities for devices with intermediate depth, an exponent α ~ 5 is observed. We propose, and show by simulations, that this increase in α is explained by a non-equilibrium model where electrons migrating to the surface smooth out the potential landscape seen by the 2DEG. This work has been supported by the Division of Materials Sciences and Engineering, Office of Basic Energy Sciences, U.S. Department of Energy (DOE). Sandia National Laboratories is a multi program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. DOE's National Nuclear Security Administration under contract DE-AC04-94AL

Quantum Mechanical Study of γ-Fe2O3 Nanoparticle as a Nanocarrier for Anticancer Drug Delivery

NASA Astrophysics Data System (ADS)

Lari, Hadi; Morsali, Ali; Heravi, Mohammad Momen

2018-05-01

Using density functional theory (DFT), noncovalent interactions and four mechanisms of covalent functionalization of melphalan anticancer drug onto γ-Fe2O3 nanoparticles have been studied. Quantum molecular descriptors of noncovalent configurations were investigated. It was specified that binding of melphalan onto γ-Fe2O3 nanoparticles is thermodynamically suitable. Hardness and the gap of energy between LUMO and HOMO of melphalan are higher than the noncovalent configurations, showing the reactivity of drug increases in the presence of γ-Fe2O3 nanoparticles. Melphalan can bond to γ-Fe2O3 nanoparticles through NH2 (k1 mechanism), OH (k2 mechanism), C=O (k3 mechanism) and Cl (k4 mechanism) groups. The activation energies, the activation enthalpies and the activation Gibbs free energies of these reactions were calculated. Thermodynamic data indicate that k3 mechanism is exothermic and spontaneous and can take place at room temperature. These results could be generalized to other similar drugs.

Nucleic acid reactivity: challenges for next-generation semiempirical quantum models.

PubMed

Huang, Ming; Giese, Timothy J; York, Darrin M

2015-07-05

Semiempirical quantum models are routinely used to study mechanisms of RNA catalysis and phosphoryl transfer reactions using combined quantum mechanical (QM)/molecular mechanical methods. Herein, we provide a broad assessment of the performance of existing semiempirical quantum models to describe nucleic acid structure and reactivity to quantify their limitations and guide the development of next-generation quantum models with improved accuracy. Neglect of diatomic differential overlap and self-consistent density-functional tight-binding semiempirical models are evaluated against high-level QM benchmark calculations for seven biologically important datasets. The datasets include: proton affinities, polarizabilities, nucleobase dimer interactions, dimethyl phosphate anion, nucleoside sugar and glycosidic torsion conformations, and RNA phosphoryl transfer model reactions. As an additional baseline, comparisons are made with several commonly used density-functional models, including M062X and B3LYP (in some cases with dispersion corrections). The results show that, among the semiempirical models examined, the AM1/d-PhoT model is the most robust at predicting proton affinities. AM1/d-PhoT and DFTB3-3ob/OPhyd reproduce the MP2 potential energy surfaces of 6 associative RNA phosphoryl transfer model reactions reasonably well. Further, a recently developed linear-scaling "modified divide-and-conquer" model exhibits the most accurate results for binding energies of both hydrogen bonded and stacked nucleobase dimers. The semiempirical models considered here are shown to underestimate the isotropic polarizabilities of neutral molecules by approximately 30%. The semiempirical models also fail to adequately describe torsion profiles for the dimethyl phosphate anion, the nucleoside sugar ring puckers, and the rotations about the nucleoside glycosidic bond. The modeling of pentavalent phosphorus, particularly with thio substitutions often used experimentally as mechanistic probes, was problematic for all of the models considered. Analysis of the strengths and weakness of the models suggests that the creation of robust next-generation models should emphasize the improvement of relative conformational energies and barriers, and nonbonded interactions. © 2015 Wiley Periodicals, Inc.

The emergent Copenhagen interpretation of quantum mechanics

NASA Astrophysics Data System (ADS)

Hollowood, Timothy J.

2014-05-01

We introduce a new and conceptually simple interpretation of quantum mechanics based on reduced density matrices of sub-systems from which the standard Copenhagen interpretation emerges as an effective description of macroscopically large systems. This interpretation describes a world in which definite measurement results are obtained with probabilities that reproduce the Born rule. Wave function collapse is seen to be a useful but fundamentally unnecessary piece of prudent book keeping which is only valid for macro-systems. The new interpretation lies in a class of modal interpretations in that it applies to quantum systems that interact with a much larger environment. However, we show that it does not suffer from the problems that have plagued similar modal interpretations like macroscopic superpositions and rapid flipping between macroscopically distinct states. We describe how the interpretation fits neatly together with fully quantum formulations of statistical mechanics and that a measurement process can be viewed as a process of ergodicity breaking analogous to a phase transition. The key feature of the new interpretation is that joint probabilities for the ergodic subsets of states of disjoint macro-systems only arise as emergent quantities. Finally we give an account of the EPR-Bohm thought experiment and show that the interpretation implies the violation of the Bell inequality characteristic of quantum mechanics but in a way that is rather novel. The final conclusion is that the Copenhagen interpretation gives a completely satisfactory phenomenology of macro-systems interacting with micro-systems.

Grid-Based Projector Augmented Wave (GPAW) Implementation of Quantum Mechanics/Molecular Mechanics (QM/MM) Electrostatic Embedding and Application to a Solvated Diplatinum Complex.

PubMed

Dohn, A O; Jónsson, E Ö; Levi, G; Mortensen, J J; Lopez-Acevedo, O; Thygesen, K S; Jacobsen, K W; Ulstrup, J; Henriksen, N E; Møller, K B; Jónsson, H

2017-12-12

A multiscale density functional theory-quantum mechanics/molecular mechanics (DFT-QM/MM) scheme is presented, based on an efficient electrostatic coupling between the electronic density obtained from a grid-based projector augmented wave (GPAW) implementation of density functional theory and a classical potential energy function. The scheme is implemented in a general fashion and can be used with various choices for the descriptions of the QM or MM regions. Tests on H 2 O clusters, ranging from dimer to decamer show that no systematic energy errors are introduced by the coupling that exceeds the differences in the QM and MM descriptions. Over 1 ns of liquid water, Born-Oppenheimer QM/MM molecular dynamics (MD) are sampled combining 10 parallel simulations, showing consistent liquid water structure over the QM/MM border. The method is applied in extensive parallel MD simulations of an aqueous solution of the diplatinum [Pt 2 (P 2 O 5 H 2 ) 4 ] 4- complex (PtPOP), spanning a total time period of roughly half a nanosecond. An average Pt-Pt distance deviating only 0.01 Å from experimental results, and a ground-state Pt-Pt oscillation frequency deviating by <2% from experimental results were obtained. The simulations highlight a remarkable harmonicity of the Pt-Pt oscillation, while also showing clear signs of Pt-H hydrogen bonding and directional coordination of water molecules along the Pt-Pt axis of the complex.

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

NASA Astrophysics Data System (ADS)

Bondarev, B. V.

1986-04-01

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

Quantum-limited heat conduction over macroscopic distances

NASA Astrophysics Data System (ADS)

Partanen, Matti; Tan, Kuan Yen; Govenius, Joonas; Lake, Russell E.; Mäkelä, Miika K.; Tanttu, Tuomo; Möttönen, Mikko

2016-05-01

The emerging quantum technological apparatuses, such as the quantum computer, call for extreme performance in thermal engineering. Cold distant heat sinks are needed for the quantized electric degrees of freedom owing to the increasing packaging density and heat dissipation. Importantly, quantum mechanics sets a fundamental upper limit for the flow of information and heat, which is quantified by the quantum of thermal conductance. However, the short distance between the heat-exchanging bodies in the previous experiments hinders their applicability in quantum technology. Here, we present experimental observations of quantum-limited heat conduction over macroscopic distances extending to a metre. We achieved this improvement of four orders of magnitude in the distance by utilizing microwave photons travelling in superconducting transmission lines. Thus, it seems that quantum-limited heat conduction has no fundamental distance cutoff. This work establishes the integration of normal-metal components into the framework of circuit quantum electrodynamics, which provides a basis for the superconducting quantum computer. Especially, our results facilitate remote cooling of nanoelectronic devices using faraway in situ-tunable heat sinks. Furthermore, quantum-limited heat conduction is important in contemporary thermodynamics. Here, the long distance may lead to ultimately efficient mesoscopic heat engines with promising practical applications.

A study of density effects in plasmas using analytical approximations for the self-consistent potential

NASA Astrophysics Data System (ADS)

Poirier, M.

2015-06-01

Density effects in ionized matter require particular attention since they modify energies, wavefunctions and transition rates with respect to the isolated-ion situation. The approach chosen in this paper is based on the ion-sphere model involving a Thomas-Fermi-like description for free electrons, the bound electrons being described by a full quantum mechanical formalism. This permits to deal with plasmas out of thermal local equilibrium, assuming only a Maxwell distribution for free electrons. For H-like ions, such a theory provides simple and rather accurate analytical approximations for the potential created by free electrons. Emphasis is put on the plasma potential rather than on the electron density, since the energies and wavefunctions depend directly on this potential. Beyond the uniform electron gas model, temperature effects may be analyzed. In the case of H-like ions, this formalism provides analytical perturbative expressions for the energies, wavefunctions and transition rates. Explicit expressions are given in the case of maximum orbital quantum number, and compare satisfactorily with results from a direct integration of the radial Schrödinger equation. Some formulas for lower orbital quantum numbers are also proposed.

Nuclear quantum effects of light and heavy water studied by all-electron first principles path integral simulations

NASA Astrophysics Data System (ADS)

Machida, Masahiko; Kato, Koichiro; Shiga, Motoyuki

2018-03-01

The isotopologs of liquid water, H2O, D2O, and T2O, are studied systematically by first principles PIMD simulations, in which the whole entity of the electrons and nuclei are treated quantum mechanically. The simulation results are in reasonable agreement with available experimental data on isotope effects, in particular, on the peak shift in the radial distributions of H2O and D2O and the shift in the evaporation energies. It is found that, due to differences in nuclear quantum effects, the H atoms in the OH bonds more easily access the dissociative region up to the hydrogen bond center than the D (T) atoms in the OD (OT) bonds. The accuracy and limitation in the use of the current density-functional-theory-based first principles PIMD simulations are also discussed. It is argued that the inclusion of the dispersion correction or relevant improvements in the density functionals are required for the quantitative estimation of isotope effects.

Is nuclear matter a quantum crystal?

NASA Technical Reports Server (NTRS)

Canuto, V.; Chitre, S. M.

1973-01-01

A possible alternative to the ordinary gas-like computation for nuclear matter is investigated under the assumption that the nucleons are arranged in a lattice. BCC, FCC and HCP structures are investigated. Only HCP shows a minimum in the energy vs. density curve with a modest binding energy of -1.5 MeV. The very low density limit is investigated and sensible results are obtained only if the tensor force decreases with the density. A study of the elastic properties indicates that the previous structures are mechanically unstable against shearing stresses.

Quantum mechanical force fields for condensed phase molecular simulations

NASA Astrophysics Data System (ADS)

Giese, Timothy J.; York, Darrin M.

2017-09-01

Molecular simulations are powerful tools for providing atomic-level details into complex chemical and physical processes that occur in the condensed phase. For strongly interacting systems where quantum many-body effects are known to play an important role, density-functional methods are often used to provide the model with the potential energy used to drive dynamics. These methods, however, suffer from two major drawbacks. First, they are often too computationally intensive to practically apply to large systems over long time scales, limiting their scope of application. Second, there remain challenges for these models to obtain the necessary level of accuracy for weak non-bonded interactions to obtain quantitative accuracy for a wide range of condensed phase properties. Quantum mechanical force fields (QMFFs) provide a potential solution to both of these limitations. In this review, we address recent advances in the development of QMFFs for condensed phase simulations. In particular, we examine the development of QMFF models using both approximate and ab initio density-functional models, the treatment of short-ranged non-bonded and long-ranged electrostatic interactions, and stability issues in molecular dynamics calculations. Example calculations are provided for crystalline systems, liquid water, and ionic liquids. We conclude with a perspective for emerging challenges and future research directions.

Why use DFT methods in the study of carbohydrates?

USDA-ARS?s Scientific Manuscript database

The recent advances in density functional theory (DFT) and computer technology allow us to study systems with more than 100 atoms routinely. This makes it feasible to study large carbohydrate molecules via quantum mechanical methods, whereas in the past, studies of carbohydrates were restricted to ...

Generalization of the Förster resonance energy transfer theory for quantum mechanical modulation of the donor-acceptor coupling

NASA Astrophysics Data System (ADS)

Jang, Seogjoo

2007-11-01

The Förster resonance energy transfer theory is generalized for inelastic situations with quantum mechanical modulation of the donor-acceptor coupling. Under the assumption that the modulations are independent of the electronic excitation of the donor and the acceptor, a general rate expression is derived, which involves two dimensional frequency-domain convolution of the donor emission line shape, the acceptor absorption line shape, and the spectral density of the modulation of the donor-acceptor coupling. For two models of modulation, detailed rate expressions are derived. The first model is the fluctuation of the donor-acceptor distance, approximated as a quantum harmonic oscillator coupled to a bath of other quantum harmonic oscillators. The distance fluctuation results in additional terms in the rate, which in the small fluctuation limit depend on the inverse eighth power of the donor-acceptor distance. The second model is the fluctuation of the torsional angle between the two transition dipoles, which is modeled as a quantum harmonic oscillator coupled to a bath of quantum harmonic oscillators and causes sinusoidal modulation of the donor-acceptor coupling. The rate expression has new elastic and inelastic terms, depending sensitively on the value of the minimum energy torsional angle. Experimental implications of the present theory and some of the open theoretical issues are discussed.

Resonant electronic excitation energy transfer by exchange mechanism in the quantum dot system

NASA Astrophysics Data System (ADS)

Chikalova-Luzina, O. P.; Samosvat, D. M.; Vyatkin, V. M.; Zegrya, G. G.

2017-11-01

A microscopic theory of nonradiative resonance energy transfer between spherical A3B5 semiconductor quantum dots by the exchange mechanism is suggested. The interdot Coulomb interaction is taken into consideration. It is assumed that the quantum dot-donor and the quantum dot-acceptor are made from the same A3B5 compound and are embedded in the matrix of another material that produces potential barriers for electrons and holes. The dependences of the energy transfer rate on the quantum-dot system parameters are found in the frame of the Kane model that provides the most adequate description of the real spectra of A3B5 semiconductors. The analytical treatment is carried out with using the density matrix method, which enabled us to perform an energy transfer analysis both in the weak-interaction approximation and in the strong-interaction approximation. The numerical calculations showed the saturation of the energy transfer rate at the distances between the donor and the acceptor approaching the contact one. The contributions of the exchange and direct Coulomb intractions can be of the same order at the small distances and can have the same value in the saturation range.

The quantum Zeno effect in double well tunnelling

NASA Astrophysics Data System (ADS)

Lerner, L.

2018-05-01

Measurement lies at the heart of quantum theory, and introductory textbooks in quantum mechanics cover the measurement problem in topics such as the Schrödinger’s cat thought experiment, the EPR problem, and the quantum Zeno effect (QZE). In this article we present a new treatment of the QZE suitable for undergraduate students, for the case of a particle tunnelling between two wells while being observed in one of the wells. The analysis shows that as the observation rate increases, the tunnelling rate tends towards zero, in accordance with Zeno’s maxim ‘a watched pot never boils’. The method relies on decoherence theory, which replaces aspects of quantum collapse by the Schrödinger evolution of an open system, and its recently simplified treatment for undergraduates. Our presentation uses concepts familiar to undergraduate students, so that calculations involving many-body theory and the formal properties of the density matrix are avoided.

Frictional lubricity enhanced by quantum mechanics.

PubMed

Zanca, Tommaso; Pellegrini, Franco; Santoro, Giuseppe E; Tosatti, Erio

2018-04-03

The quantum motion of nuclei, generally ignored in the physics of sliding friction, can affect in an important manner the frictional dissipation of a light particle forced to slide in an optical lattice. The density matrix-calculated evolution of the quantum version of the basic Prandtl-Tomlinson model, describing the dragging by an external force of a point particle in a periodic potential, shows that purely classical friction predictions can be very wrong. The strongest quantum effect occurs not for weak but for strong periodic potentials, where barriers are high but energy levels in each well are discrete, and resonant Rabi or Landau-Zener tunneling to states in the nearest well can preempt classical stick-slip with nonnegligible efficiency, depending on the forcing speed. The resulting permeation of otherwise unsurmountable barriers is predicted to cause quantum lubricity, a phenomenon which we expect should be observable in the recently implemented sliding cold ion experiments.

Quantum image pseudocolor coding based on the density-stratified method

NASA Astrophysics Data System (ADS)

Jiang, Nan; Wu, Wenya; Wang, Luo; Zhao, Na

2015-05-01

Pseudocolor processing is a branch of image enhancement. It dyes grayscale images to color images to make the images more beautiful or to highlight some parts on the images. This paper proposes a quantum image pseudocolor coding scheme based on the density-stratified method which defines a colormap and changes the density value from gray to color parallel according to the colormap. Firstly, two data structures: quantum image GQIR and quantum colormap QCR are reviewed or proposed. Then, the quantum density-stratified algorithm is presented. Based on them, the quantum realization in the form of circuits is given. The main advantages of the quantum version for pseudocolor processing over the classical approach are that it needs less memory and can speed up the computation. Two kinds of examples help us to describe the scheme further. Finally, the future work are analyzed.

Quantum crystallographic charge density of urea

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

Wall, Michael E.

Standard X-ray crystallography methods use free-atom models to calculate mean unit-cell charge densities. Real molecules, however, have shared charge that is not captured accurately using free-atom models. To address this limitation, a charge density model of crystalline urea was calculated using high-level quantum theory and was refined against publicly available ultra-high-resolution experimental Bragg data, including the effects of atomic displacement parameters. The resulting quantum crystallographic model was compared with models obtained using spherical atom or multipole methods. Despite using only the same number of free parameters as the spherical atom model, the agreement of the quantum model with the datamore » is comparable to the multipole model. The static, theoretical crystalline charge density of the quantum model is distinct from the multipole model, indicating the quantum model provides substantially new information. Hydrogen thermal ellipsoids in the quantum model were very similar to those obtained using neutron crystallography, indicating that quantum crystallography can increase the accuracy of the X-ray crystallographic atomic displacement parameters. Lastly, the results demonstrate the feasibility and benefits of integrating fully periodic quantum charge density calculations into ultra-high-resolution X-ray crystallographic model building and refinement.« less

Quantum crystallographic charge density of urea

DOE PAGES

Wall, Michael E.

2016-06-08

Standard X-ray crystallography methods use free-atom models to calculate mean unit-cell charge densities. Real molecules, however, have shared charge that is not captured accurately using free-atom models. To address this limitation, a charge density model of crystalline urea was calculated using high-level quantum theory and was refined against publicly available ultra-high-resolution experimental Bragg data, including the effects of atomic displacement parameters. The resulting quantum crystallographic model was compared with models obtained using spherical atom or multipole methods. Despite using only the same number of free parameters as the spherical atom model, the agreement of the quantum model with the datamore » is comparable to the multipole model. The static, theoretical crystalline charge density of the quantum model is distinct from the multipole model, indicating the quantum model provides substantially new information. Hydrogen thermal ellipsoids in the quantum model were very similar to those obtained using neutron crystallography, indicating that quantum crystallography can increase the accuracy of the X-ray crystallographic atomic displacement parameters. Lastly, the results demonstrate the feasibility and benefits of integrating fully periodic quantum charge density calculations into ultra-high-resolution X-ray crystallographic model building and refinement.« less

Multi-Dimensional Quantum Effect Simulation Using a Density-Gradient Model and Script-Level Programming Techniques

NASA Technical Reports Server (NTRS)

Rafferty, Connor S.; Biegel, Bryan A.; Yu, Zhi-Ping; Ancona, Mario G.; Bude, J.; Dutton, Robert W.; Saini, Subhash (Technical Monitor)

1998-01-01

A density-gradient (DG) model is used to calculate quantum-mechanical corrections to classical carrier transport in MOS (Metal Oxide Semiconductor) inversion/accumulation layers. The model is compared to measured data and to a fully self-consistent coupled Schrodinger and Poisson equation (SCSP) solver. Good agreement is demonstrated for MOS capacitors with gate oxide as thin as 21 A. It is then applied to study carrier distribution in ultra short MOSFETs (Metal Oxide Semiconductor Field Effect Transistor) with surface roughness. This work represents the first implementation of the DG formulation on multidimensional unstructured meshes. It was enabled by a powerful scripting approach which provides an easy-to-use and flexible framework for solving the fourth-order PDEs (Partial Differential Equation) of the DG model.

The Colour of the Noble Metals.

ERIC Educational Resources Information Center

Poole, R. T.

1983-01-01

Examines the physical basis for colors of noble metals (copper, silver, gold) developed from energy conservation/quantum mechanical view of free electron photoabsorption. Describes production of absorption edges produced by change in density of occupied valence electron states in the d-band, which allows stronger absorption in the visible photon…

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

Strubbe, David

Octopus is a scientific program aimed at the ab initio virtual experimentation on a hopefully ever-increasing range of system types. Electrons are described quantum-mechanically within density-functional theory (DFT), in its time-dependent form (TDDFT) when doing simulations in time. Nuclei are described classically as point particles. Electron-nucleus interaction is described within the pseudopotential approximation.

Optimum quantum receiver for detecting weak signals in PAM communication systems

NASA Astrophysics Data System (ADS)

Sharma, Navneet; Rawat, Tarun Kumar; Parthasarathy, Harish; Gautam, Kumar

2017-09-01

This paper deals with the modeling of an optimum quantum receiver for pulse amplitude modulator (PAM) communication systems. The information bearing sequence {I_k}_{k=0}^{N-1} is estimated using the maximum likelihood (ML) method. The ML method is based on quantum mechanical measurements of an observable X in the Hilbert space of the quantum system at discrete times, when the Hamiltonian of the system is perturbed by an operator obtained by modulating a potential V with a PAM signal derived from the information bearing sequence {I_k}_{k=0}^{N-1}. The measurement process at each time instant causes collapse of the system state to an observable eigenstate. All probabilities of getting different outcomes from an observable are calculated using the perturbed evolution operator combined with the collapse postulate. For given probability densities, calculation of the mean square error evaluates the performance of the receiver. Finally, we present an example involving estimating an information bearing sequence that modulates a quantum electromagnetic field incident on a quantum harmonic oscillator.

Spin relaxation dynamics of holes in intrinsic GaAs quantum wells studied by transient circular dichromatic absorption spectroscopy at room temperature.

PubMed

Fang, Shaoyin; Zhu, Ruidan; Lai, Tianshu

2017-03-21

Spin relaxation dynamics of holes in intrinsic GaAs quantum wells is studied using time-resolved circular dichromatic absorption spectroscopy at room temperature. It is found that ultrafast dynamics is dominated by the cooperative contributions of band filling and many-body effects. The relative contribution of the two effects is opposite in strength for electrons and holes. As a result, transient circular dichromatic differential transmission (TCD-DT) with co- and cross-circularly polarized pump and probe presents different strength at several picosecond delay time. Ultrafast spin relaxation dynamics of excited holes is sensitively reflected in TCD-DT with cross-circularly polarized pump and probe. A model, including coherent artifact, thermalization of nonthermal carriers and the cooperative contribution of band filling and many-body effects, is developed, and used to fit TCD-DT with cross-circularly polarized pump and probe. Spin relaxation time of holes is achieved as a function of excited hole density for the first time at room temperature, and increases with hole density, which disagrees with a theoretical prediction based on EY spin relaxation mechanism, implying that EY mechanism may be not dominant hole spin relaxation mechanism at room temperature, but DP mechanism is dominant possibly.

Ab Initio Modeling of Structure and Properties of Single and Mixed Alkali Silicate Glasses.

PubMed

Baral, Khagendra; Li, Aize; Ching, Wai-Yim

2017-10-12

A density functional theory (DFT)-based ab initio molecular dynamics (AIMD) has been applied to simulate models of single and mixed alkali silicate glasses with two different molar concentrations of alkali oxides. The structural environments and spatial distributions of alkali ions in the 10 simulated models with 20% and 30% of Li, Na, K and equal proportions of Li-Na and Na-K are studied in detail for subtle variations among the models. Quantum mechanical calculations of electronic structures, interatomic bonding, and mechanical and optical properties are carried out for each of the models, and the results are compared with available experimental observation and other simulations. The calculated results are in good agreement with the experimental data. We have used the novel concept of using the total bond order density (TBOD), a quantum mechanical metric, to characterize internal cohesion in these glass models. The mixed alkali effect (MAE) is visible in the bulk mechanical properties but not obvious in other physical properties studied in this paper. We show that Li doping deviates from expected trend due to the much stronger Li-O bonding than those of Na and K doping. The approach used in this study is in contrast with current studies in alkali-doped silicate glasses based only on geometric characterizations.

Physical Concepts and Mathematical Symbols

NASA Astrophysics Data System (ADS)

Grelland, Hans Herlof

2007-12-01

According to traditional empiricist philosophy of science, concepts and meaning grow out of sense experience, and the mathematical structure of a physical theory is nothing but a formalisation of a given meaning-content. This view seems to work well in classical mechanics. But it breaks down in quantum physics, where we have a self-supported mathematical structure which resists any conceptual or pictorial interpretation in the traditional sense. Thus, traditional empiricism is flawed. Quantum physics teaches us that mathematics is a language in itself which extends beyond ordinary language. To understand the meaning of this extended language, we have to explore how new concepts and intuitions grow out of mathematics, not the other way around. The symbolic structure is prior to its meaning. This point of view is called linguistic empiricism, to stress that the connection with experience is still crucial. As cases, I compare the concept of stiffness in classical mechanics and the concept of electron density in quantum mechanics. The last case demonstrates that the wave function has a richer interpretation than the probabilistic one concerning measurement of position.

Current algebra, statistical mechanics and quantum models

NASA Astrophysics Data System (ADS)

Vilela Mendes, R.

2017-11-01

Results obtained in the past for free boson systems at zero and nonzero temperatures are revisited to clarify the physical meaning of current algebra reducible functionals which are associated to systems with density fluctuations, leading to observable effects on phase transitions. To use current algebra as a tool for the formulation of quantum statistical mechanics amounts to the construction of unitary representations of diffeomorphism groups. Two mathematical equivalent procedures exist for this purpose. One searches for quasi-invariant measures on configuration spaces, the other for a cyclic vector in Hilbert space. Here, one argues that the second approach is closer to the physical intuition when modelling complex systems. An example of application of the current algebra methodology to the pairing phenomenon in two-dimensional fermion systems is discussed.

Formation of E-cyanomethamine in a nitrile rich environment

NASA Astrophysics Data System (ADS)

Shivani; Misra, Alka; Tandon, Poonam

2017-01-01

Recently a new molecule, cyanomethamine, has been detected towards Sagittarius B2(N) (Sgr B2(N)). Studying the formation mechanisms of complex interstellar molecules is difficult. Hence, a theoretical quantum chemical approach for analyzing the reaction mechanism describing the formation of interstellar cyanomethamine through detected interstellar molecules and radicals (NCCN+H) is discussed in the present work. Calculations are performed by using quantum chemical techniques, such as Density Functional Theory (DFT) and Møller-Plesset perturbation (MP2) theory with a 6-311G(d,p) basis set, both in the gas phase and in icy grains. The proposed reaction path (NCCN+H+H) has exothermicity with no barrier which indicates the possibility of cyanomethamine formation in the interstellar medium.

Quantum Glass of Interacting Bosons with Off-Diagonal Disorder

NASA Astrophysics Data System (ADS)

Piekarska, A. M.; Kopeć, T. K.

2018-04-01

We study disordered interacting bosons described by the Bose-Hubbard model with Gaussian-distributed random tunneling amplitudes. It is shown that the off-diagonal disorder induces a spin-glass-like ground state, characterized by randomly frozen quantum-mechanical U(1) phases of bosons. To access criticality, we employ the "n -replica trick," as in the spin-glass theory, and the Trotter-Suzuki method for decomposition of the statistical density operator, along with numerical calculations. The interplay between disorder, quantum, and thermal fluctuations leads to phase diagrams exhibiting a glassy state of bosons, which are studied as a function of model parameters. The considered system may be relevant for quantum simulators of optical-lattice bosons, where the randomness can be introduced in a controlled way. The latter is supported by a proposition of experimental realization of the system in question.

Quantum and isotope effects in lithium metal

NASA Astrophysics Data System (ADS)

Ackland, Graeme J.; Dunuwille, Mihindra; Martinez-Canales, Miguel; Loa, Ingo; Zhang, Rong; Sinogeikin, Stanislav; Cai, Weizhao; Deemyad, Shanti

2017-06-01

The crystal structure of elements at zero pressure and temperature is the most fundamental information in condensed matter physics. For decades it has been believed that lithium, the simplest metallic element, has a complicated ground-state crystal structure. Using synchrotron x-ray diffraction in diamond anvil cells and multiscale simulations with density functional theory and molecular dynamics, we show that the previously accepted martensitic ground state is metastable. The actual ground state is face-centered cubic (fcc). We find that isotopes of lithium, under similar thermal paths, exhibit a considerable difference in martensitic transition temperature. Lithium exhibits nuclear quantum mechanical effects, serving as a metallic intermediate between helium, with its quantum effect-dominated structures, and the higher-mass elements. By disentangling the quantum kinetic complexities, we prove that fcc lithium is the ground state, and we synthesize it by decompression.

Quantum Entanglement of Matter and Geometry in Large Systems

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

Hogan, Craig J.

2014-12-04

Standard quantum mechanics and gravity are used to estimate the mass and size of idealized gravitating systems where position states of matter and geometry become indeterminate. It is proposed that well-known inconsistencies of standard quantum field theory with general relativity on macroscopic scales can be reconciled by nonstandard, nonlocal entanglement of field states with quantum states of geometry. Wave functions of particle world lines are used to estimate scales of geometrical entanglement and emergent locality. Simple models of entanglement predict coherent fluctuations in position of massive bodies, of Planck scale origin, measurable on a laboratory scale, and may account formore » the fact that the information density of long lived position states in Standard Model fields, which is determined by the strong interactions, is the same as that determined holographically by the cosmological constant.« less

Light-front representation of chiral dynamics with Δ isobar and large-N c relations

DOE PAGES

Granados, C.; Weiss, C.

2016-06-13

Transverse densities describe the spatial distribution of electromagnetic current in the nucleon at fixed light-front time. At peripheral distances b = O(M π –1) the densities are governed by chiral dynamics and can be calculated model-independently using chiral effective field theory (EFT). Recent work has shown that the EFT results can be represented in first-quantized form, as overlap integrals of chiral light-front wave functions describing the transition of the nucleon to soft-pion-nucleon intermediate states, resulting in a quantum-mechanical picture of the peripheral transverse densities. We now extend this representation to include intermediate states with Δ isobars and implement relations basedmore » on the large-N c limit of QCD. We derive the wave function overlap formulas for the Δ contributions to the peripheral transverse densities by way of a three-dimensional reduction of relativistic chiral EFT expressions. Our procedure effectively maintains rotational invariance and avoids the ambiguities with higher-spin particles in the light-front time-ordered approach. We study the interplay of πN and πΔ intermediate states in the quantum-mechanical picture of the densities in a transversely polarized nucleon. We show that the correct N c-scaling of the charge and magnetization densities emerges as the result of the particular combination of currents generated by intermediate states with degenerate N and Δ. The off-shell behavior of the chiral EFT is summarized in contact terms and can be studied easily. As a result, the methods developed here can be applied to other peripheral densities and to moments of the nucleon's generalized parton distributions.« less

Simulating biochemical physics with computers: 1. Enzyme catalysis by phosphotriesterase and phosphodiesterase; 2. Integration-free path-integral method for quantum-statistical calculations

NASA Astrophysics Data System (ADS)

Wong, Kin-Yiu

We have simulated two enzymatic reactions with molecular dynamics (MD) and combined quantum mechanical/molecular mechanical (QM/MM) techniques. One reaction is the hydrolysis of the insecticide paraoxon catalyzed by phosphotriesterase (PTE). PTE is a bioremediation candidate for environments contaminated by toxic nerve gases (e.g., sarin) or pesticides. Based on the potential of mean force (PMF) and the structural changes of the active site during the catalysis, we propose a revised reaction mechanism for PTE. Another reaction is the hydrolysis of the second-messenger cyclic adenosine 3'-5'-monophosphate (cAMP) catalyzed by phosphodiesterase (PDE). Cyclicnucleotide PDE is a vital protein in signal-transduction pathways and thus a popular target for inhibition by drugs (e.g., ViagraRTM). A two-dimensional (2-D) free-energy profile has been generated showing that the catalysis by PDE proceeds in a two-step SN2-type mechanism. Furthermore, to characterize a chemical reaction mechanism in experiment, a direct probe is measuring kinetic isotope effects (KIEs). KIEs primarily arise from internuclear quantum-statistical effects, e.g., quantum tunneling and quantization of vibration. To systematically incorporate the quantum-statistical effects during MD simulations, we have developed an automated integration-free path-integral (AIF-PI) method based on Kleinert's variational perturbation theory for the centroid density of Feynman's path integral. Using this analytic method, we have performed ab initio pathintegral calculations to study the origin of KIEs on several series of proton-transfer reactions from carboxylic acids to aryl substituted alpha-methoxystyrenes in water. In addition, we also demonstrate that the AIF-PI method can be used to systematically compute the exact value of zero-point energy (beyond the harmonic approximation) by simply minimizing the centroid effective potential.

Polarization State of Light Scattered from Quantum Plasmonic Dimer Antennas.

PubMed

Yang, Longkun; Wang, Hancong; Fang, Yan; Li, Zhipeng

2016-01-26

Plasmonic antennas are able to concentrate and re-emit light in a controllable manner through strong coupling between metallic nanostructures. Only recently has it found that quantum mechanical effects can drastically change the coupling strength as the feature size approaches atomic scales. Here, we present a comprehensive experimental and theoretical study of the evolution of the resonance peak and its polarization state as the dimer-antenna gap narrows to subnanometer scale. We clearly can identify the classical plasmonic regime, a crossover regime where nonlocal screening plays an important role, and the quantum regime where a charge transfer plasmon appears due to interparticle electron tunneling. Moreover, as the gap decreases from tens of to a few nanometers, the bonding dipole mode tends to emit photons with increasing polarizability. When the gap narrows to quantum regime, a significant depolarization of the mode emission is observed due to the reduction of the charge density of coupled quantum plasmons. These results would be beneficial for the understanding of quantum effects on emitting-polarization of nanoantennas and the development of quantum-based photonic nanodevices.

Quantum-like model of processing of information in the brain based on classical electromagnetic field.

PubMed

Khrennikov, Andrei

2011-09-01

We propose a model of quantum-like (QL) processing of mental information. This model is based on quantum information theory. However, in contrast to models of "quantum physical brain" reducing mental activity (at least at the highest level) to quantum physical phenomena in the brain, our model matches well with the basic neuronal paradigm of the cognitive science. QL information processing is based (surprisingly) on classical electromagnetic signals induced by joint activity of neurons. This novel approach to quantum information is based on representation of quantum mechanics as a version of classical signal theory which was recently elaborated by the author. The brain uses the QL representation (QLR) for working with abstract concepts; concrete images are described by classical information theory. Two processes, classical and QL, are performed parallely. Moreover, information is actively transmitted from one representation to another. A QL concept given in our model by a density operator can generate a variety of concrete images given by temporal realizations of the corresponding (Gaussian) random signal. This signal has the covariance operator coinciding with the density operator encoding the abstract concept under consideration. The presence of various temporal scales in the brain plays the crucial role in creation of QLR in the brain. Moreover, in our model electromagnetic noise produced by neurons is a source of superstrong QL correlations between processes in different spatial domains in the brain; the binding problem is solved on the QL level, but with the aid of the classical background fluctuations. Copyright © 2011 Elsevier Ireland Ltd. All rights reserved.

S/G-1: an ab initio force-field blending frozen Hermite Gaussian densities and distributed multipoles. Proof of concept and first applications to metal cations.

PubMed

Chaudret, Robin; Gresh, Nohad; Narth, Christophe; Lagardère, Louis; Darden, Thomas A; Cisneros, G Andrés; Piquemal, Jean-Philip

2014-09-04

We demonstrate as a proof of principle the capabilities of a novel hybrid MM'/MM polarizable force field to integrate short-range quantum effects in molecular mechanics (MM) through the use of Gaussian electrostatics. This lead to a further gain in accuracy in the representation of the first coordination shell of metal ions. It uses advanced electrostatics and couples two point dipole polarizable force fields, namely, the Gaussian electrostatic model (GEM), a model based on density fitting, which uses fitted electronic densities to evaluate nonbonded interactions, and SIBFA (sum of interactions between fragments ab initio computed), which resorts to distributed multipoles. To understand the benefits of the use of Gaussian electrostatics, we evaluate first the accuracy of GEM, which is a pure density-based Gaussian electrostatics model on a test Ca(II)-H2O complex. GEM is shown to further improve the agreement of MM polarization with ab initio reference results. Indeed, GEM introduces nonclassical effects by modeling the short-range quantum behavior of electric fields and therefore enables a straightforward (and selective) inclusion of the sole overlap-dependent exchange-polarization repulsive contribution by means of a Gaussian damping function acting on the GEM fields. The S/G-1 scheme is then introduced. Upon limiting the use of Gaussian electrostatics to metal centers only, it is shown to be able to capture the dominant quantum effects at play on the metal coordination sphere. S/G-1 is able to accurately reproduce ab initio total interaction energies within closed-shell metal complexes regarding each individual contribution including the separate contributions of induction, polarization, and charge-transfer. Applications of the method are provided for various systems including the HIV-1 NCp7-Zn(II) metalloprotein. S/G-1 is then extended to heavy metal complexes. Tested on Hg(II) water complexes, S/G-1 is shown to accurately model polarization up to quadrupolar response level. This opens up the possibility of embodying explicit scalar relativistic effects in molecular mechanics thanks to the direct transferability of ab initio pseudopotentials. Therefore, incorporating GEM-like electron density for a metal cation enable the introduction of nonambiguous short-range quantum effects within any point-dipole based polarizable force field without the need of an extensive parametrization.

Dissipation of ‘dark energy’ by cortex in knowledge retrieval

NASA Astrophysics Data System (ADS)

Capolupo, Antonio; Freeman, Walter J.; Vitiello, Giuseppe

2013-03-01

We have devised a thermodynamic model of cortical neurodynamics expressed at the classical level by neural networks and at the quantum level by dissipative quantum field theory. Our model is based on features in the spatial images of cortical activity newly revealed by high-density electrode arrays. We have incorporated the mechanism and necessity for so-called dark energy in knowledge retrieval. We have extended the model first using the Carnot cycle to define our measures for energy, entropy and temperature, and then using the Rankine cycle to incorporate criticality and phase transitions. We describe the dynamics of two interactive fields of neural activity that express knowledge, one at high and the other at low energy density, and the two operators that create and annihilate the fields. We postulate that the extremely high density of energy sequestered briefly in cortical activity patterns can account for the vividness, richness of associations, and emotional intensity of memories recalled by stimuli.

Dissipation of 'dark energy' by cortex in knowledge retrieval.

PubMed

Capolupo, Antonio; Freeman, Walter J; Vitiello, Giuseppe

2013-03-01

We have devised a thermodynamic model of cortical neurodynamics expressed at the classical level by neural networks and at the quantum level by dissipative quantum field theory. Our model is based on features in the spatial images of cortical activity newly revealed by high-density electrode arrays. We have incorporated the mechanism and necessity for so-called dark energy in knowledge retrieval. We have extended the model first using the Carnot cycle to define our measures for energy, entropy and temperature, and then using the Rankine cycle to incorporate criticality and phase transitions. We describe the dynamics of two interactive fields of neural activity that express knowledge, one at high and the other at low energy density, and the two operators that create and annihilate the fields. We postulate that the extremely high density of energy sequestered briefly in cortical activity patterns can account for the vividness, richness of associations, and emotional intensity of memories recalled by stimuli. Copyright © 2013 Elsevier B.V. All rights reserved.

Schrödinger problem, Lévy processes, and noise in relativistic quantum mechanics

NASA Astrophysics Data System (ADS)

Garbaczewski, Piotr; Klauder, John R.; Olkiewicz, Robert

1995-05-01

The main purpose of the paper is an essentially probabilistic analysis of relativistic quantum mechanics. It is based on the assumption that whenever probability distributions arise, there exists a stochastic process that is either responsible for the temporal evolution of a given measure or preserves the measure in the stationary case. Our departure point is the so-called Schrödinger problem of probabilistic evolution, which provides for a unique Markov stochastic interpolation between any given pair of boundary probability densities for a process covering a fixed, finite duration of time, provided we have decided a priori what kind of primordial dynamical semigroup transition mechanism is involved. In the nonrelativistic theory, including quantum mechanics, Feynman-Kac-like kernels are the building blocks for suitable transition probability densities of the process. In the standard ``free'' case (Feynman-Kac potential equal to zero) the familiar Wiener noise is recovered. In the framework of the Schrödinger problem, the ``free noise'' can also be extended to any infinitely divisible probability law, as covered by the Lévy-Khintchine formula. Since the relativistic Hamiltonians ||∇|| and √-Δ+m2 -m are known to generate such laws, we focus on them for the analysis of probabilistic phenomena, which are shown to be associated with the relativistic wave (D'Alembert) and matter-wave (Klein-Gordon) equations, respectively. We show that such stochastic processes exist and are spatial jump processes. In general, in the presence of external potentials, they do not share the Markov property, except for stationary situations. A concrete example of the pseudodifferential Cauchy-Schrödinger evolution is analyzed in detail. The relativistic covariance of related wave equations is exploited to demonstrate how the associated stochastic jump processes comply with the principles of special relativity.

Influencing factors on the size uniformity of self-assembled SiGe quantum rings grown by molecular beam epitaxy.

PubMed

Cui, J; Lv, Y; Yang, X J; Fan, Y L; Zhong, Z; Jiang, Z M

2011-03-25

The size uniformity of self-assembled SiGe quantum rings, which are formed by capping SiGe quantum dots with a thin Si layer, is found to be greatly influenced by the growth temperature and the areal density of SiGe quantum dots. Higher growth temperature benefits the size uniformity of quantum dots, but results in low Ge concentration as well as asymmetric Ge distribution in the dots, which induces the subsequently formed quantum rings to be asymmetric in shape or even broken somewhere in the ridge of rings. Low growth temperature degrades the size uniformity of quantum dots, and thus that of quantum rings. A high areal density results in the expansion and coalescence of neighboring quantum dots to form a chain, rather than quantum rings. Uniform quantum rings with a size dispersion of 4.6% and an areal density of 7.8×10(8) cm(-2) are obtained at the optimized growth temperature of 640°C.

FIBER AND INTEGRATED OPTICS. OTHER TOPICS IN QUANTUM ELECTRONICS: Laser generation of dislocations and mechanism of anisotropic melting of semiconductor surfaces

NASA Astrophysics Data System (ADS)

Volodin, B. L.; Emel'yanov, Vladimir I.

1990-05-01

An analysis is made of a vacancy-deformation mechanism of generation of dislocations by laser radiation involving condensation of laser-induced vacancies when the vacancy concentration exceeds a certain critical value. The theory can be used to estimate the radius of the resultant dislocation loops and their density. It is used to interpret anisotropic laser melting of semiconductor surfaces.

Imaging the Ultrafast Photoelectron Transfer Process in Alizarin-TiO2.

PubMed

Gomez, Tatiana; Hermann, Gunter; Zarate, Ximena; Pérez-Torres, Jhon Fredy; Tremblay, Jean Christophe

2015-07-30

In this work, we adopt a quantum mechanical approach based on time-dependent density functional theory (TDDFT) to study the optical and electronic properties of alizarin supported on TiO2 nano-crystallites, as a prototypical dye-sensitized solar cell. To ensure proper alignment of the donor (alizarin) and acceptor (TiO2 nano-crystallite) levels, static optical excitation spectra are simulated using time-dependent density functional theory in response. The ultrafast photoelectron transfer from the dye to the cluster is simulated using an explicitly time-dependent, one-electron TDDFT ansatz. The model considers the δ-pulse excitation of a single active electron localized in the dye to the complete set of energetically accessible, delocalized molecular orbitals of the dye/nano-crystallite complex. A set of quantum mechanical tools derived from the transition electronic flux density is introduced to visualize and analyze the process in real time. The evolution of the created wave packet subject to absorbing boundary conditions at the borders of the cluster reveal that, while the electrons of the aromatic rings of alizarin are heavily involved in an ultrafast charge redistribution between the carbonyl groups of the dye molecule, they do not contribute positively to the electron injection and, overall, they delay the process.

Propensity, Probability, and Quantum Theory

NASA Astrophysics Data System (ADS)

Ballentine, Leslie E.

2016-08-01

Quantum mechanics and probability theory share one peculiarity. Both have well established mathematical formalisms, yet both are subject to controversy about the meaning and interpretation of their basic concepts. Since probability plays a fundamental role in QM, the conceptual problems of one theory can affect the other. We first classify the interpretations of probability into three major classes: (a) inferential probability, (b) ensemble probability, and (c) propensity. Class (a) is the basis of inductive logic; (b) deals with the frequencies of events in repeatable experiments; (c) describes a form of causality that is weaker than determinism. An important, but neglected, paper by P. Humphreys demonstrated that propensity must differ mathematically, as well as conceptually, from probability, but he did not develop a theory of propensity. Such a theory is developed in this paper. Propensity theory shares many, but not all, of the axioms of probability theory. As a consequence, propensity supports the Law of Large Numbers from probability theory, but does not support Bayes theorem. Although there are particular problems within QM to which any of the classes of probability may be applied, it is argued that the intrinsic quantum probabilities (calculated from a state vector or density matrix) are most naturally interpreted as quantum propensities. This does not alter the familiar statistical interpretation of QM. But the interpretation of quantum states as representing knowledge is untenable. Examples show that a density matrix fails to represent knowledge.

Time dependent Schrödinger equation for black hole evaporation: No information loss

NASA Astrophysics Data System (ADS)

Corda, Christian

2015-02-01

In 1976 S. Hawking claimed that "Because part of the information about the state of the system is lost down the hole, the final situation is represented by a density matrix rather than a pure quantum state".1 In a series of papers, together with collaborators, we naturally interpreted BH quasi-normal modes (QNMs) in terms of quantum levels discussing a model of excited BH somewhat similar to the historical semi-classical Bohr model of the structure of a hydrogen atom. Here we explicitly write down, for the same model, a time dependent Schrödinger equation for the system composed by Hawking radiation and BH QNMs. The physical state and the correspondent wave function are written in terms of a unitary evolution matrix instead of a density matrix. Thus, the final state results to be a pure quantum state instead of a mixed one. Hence, Hawking's claim is falsified because BHs result to be well defined quantum mechanical systems, having ordered, discrete quantum spectra, which respect 't Hooft's assumption that Schrödinger equations can be used universally for all dynamics in the universe. As a consequence, information comes out in BH evaporation in terms of pure states in a unitary time dependent evolution. In Section 4 of this paper we show that the present approach permits also to solve the entanglement problem connected with the information paradox.

Density-matrix-based algorithm for solving eigenvalue problems

NASA Astrophysics Data System (ADS)

Polizzi, Eric

2009-03-01

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

Electronic Structures of Strained InAs x P1-x by Density Functional Theory.

PubMed

Lee, Seung Mi; Kim, Min-Young; Kim, Young Heon

2018-09-01

We investigated the effects of strain on the electronic structures of InAsxP1-x using quantum mechanical density functional theory calculations. The electronic band gap and electron effective mass decreased with the increase of the uniaxial tensile strain along the [0001] direction of wurtzite InAs0.75P0.25. Therefore, faster electron movements are expected. These theoretical results are in good agreement with the experimental measurements of InAs0.75P0.25 nanowire.

Surface chemistry and density distribution influence on visible luminescence of silicon quantum dots: an experimental and theoretical approach.

PubMed

Dutt, Ateet; Matsumoto, Yasuhiro; Santana-Rodríguez, G; Ramos, Estrella; Monroy, B Marel; Santoyo Salazar, J

2017-01-04

The impact of the surface reconstruction of the density distribution and photoluminescence of silicon quantum dots (QDs) embedded in a silicon oxide matrix (SiO x ) has been studied. Annealing treatments carried out on the as-deposited samples provoked the effusion of hydrogen species. Moreover, depending on the surrounding density and coalescence of QDs, they resulted in a change in the average size of the particles depending on the initial local environment. The shift in the luminescence spectra all over the visible region (blue, green and red) shows a strong dependence on the resultant change in the size and/or the passivation environment of QDs. Density functional theoretical (DFT) calculations support this fact and explain the possible electronic transitions (HOMO-LUMO gap) involved. Passivation in the presence of oxygen species lowers the band gap of Si 29 and Si 35 nanoclusters up to 1.7 eV, whereas, surface passivation in the environment of hydrogen species increases the band gap up to 4.4 eV. These results show a good agreement with the quantum confinement model described in this work and explain the shift in the luminescence all over the visible region. The results reported here offer vital insight into the mechanism of emission from silicon quantum dots which has been one of the most debated topics in the last two decades. QDs with multiple size distribution in different local environments (band gap) observed in this work could be used for the fabrication of light emission diodes (LEDs) or shift-conversion thin films in third generation efficient tandem solar cells for the maximum absorption of the solar spectrum in different wavelength regions.

Quasimodular instanton partition function and the elliptic solution of Korteweg-de Vries equations

NASA Astrophysics Data System (ADS)

He, Wei

2015-02-01

The Gauge/Bethe correspondence relates Omega-deformed N = 2 supersymmetric gauge theories to some quantum integrable models, in simple cases the integrable models can be treated as solvable quantum mechanics models. For SU(2) gauge theory with an adjoint matter, or with 4 fundamental matters, the potential of corresponding quantum model is the elliptic function. If the mass of matter takes special value then the potential is an elliptic solution of KdV hierarchy. We show that the deformed prepotential of gauge theory can be obtained from the average densities of conserved charges of the classical KdV solution, the UV gauge coupling dependence is assembled into the Eisenstein series. The gauge theory with adjoint mass is taken as the example.

Large-scale semidefinite programming for many-electron quantum mechanics.

PubMed

Mazziotti, David A

2011-02-25

The energy of a many-electron quantum system can be approximated by a constrained optimization of the two-electron reduced density matrix (2-RDM) that is solvable in polynomial time by semidefinite programming (SDP). Here we develop a SDP method for computing strongly correlated 2-RDMs that is 10-20 times faster than previous methods [D. A. Mazziotti, Phys. Rev. Lett. 93, 213001 (2004)]. We illustrate with (i) the dissociation of N(2) and (ii) the metal-to-insulator transition of H(50). For H(50) the SDP problem has 9.4×10(6) variables. This advance also expands the feasibility of large-scale applications in quantum information, control, statistics, and economics. © 2011 American Physical Society

Large-Scale Semidefinite Programming for Many-Electron Quantum Mechanics

NASA Astrophysics Data System (ADS)

Mazziotti, David A.

2011-02-01

The energy of a many-electron quantum system can be approximated by a constrained optimization of the two-electron reduced density matrix (2-RDM) that is solvable in polynomial time by semidefinite programming (SDP). Here we develop a SDP method for computing strongly correlated 2-RDMs that is 10-20 times faster than previous methods [D. A. Mazziotti, Phys. Rev. Lett. 93, 213001 (2004)PRLTAO0031-900710.1103/PhysRevLett.93.213001]. We illustrate with (i) the dissociation of N2 and (ii) the metal-to-insulator transition of H50. For H50 the SDP problem has 9.4×106 variables. This advance also expands the feasibility of large-scale applications in quantum information, control, statistics, and economics.

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

NASA Technical Reports Server (NTRS)

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

1988-01-01

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

Quantum phases of spinful Fermi gases in optical cavities

NASA Astrophysics Data System (ADS)

Colella, E.; Citro, R.; Barsanti, M.; Rossini, D.; Chiofalo, M.-L.

2018-04-01

We explore the quantum phases emerging from the interplay between spin and motional degrees of freedom of a one-dimensional quantum fluid of spinful fermionic atoms, effectively interacting via a photon-mediating mechanism with tunable sign and strength g , as it can be realized in present-day experiments with optical cavities. We find the emergence, in the very same system, of spin- and atomic-density wave ordering, accompanied by the occurrence of superfluidity for g >0 , while cavity photons are seen to drive strong correlations at all g values, with fermionic character for g >0 , and bosonic character for g <0 . Due to the long-range nature of interactions, to infer these results we combine mean-field and exact-diagonalization methods supported by bosonization analysis.

Nuclear magnetic resonance in high magnetic field: Application to condensed matter physics

NASA Astrophysics Data System (ADS)

Berthier, Claude; Horvatić, Mladen; Julien, Marc-Henri; Mayaffre, Hadrien; Krämer, Steffen

2017-05-01

In this review, we describe the potentialities offered by the nuclear magnetic resonance (NMR) technique to explore at a microscopic level new quantum states of condensed matter induced by high magnetic fields. We focus on experiments realised in resistive (up to 34 T) or hybrid (up to 45 T) magnets, which open a large access to these quantum phase transitions. After an introduction on NMR observables, we consider several topics: quantum spin systems (spin-Peierls transition, spin ladders, spin nematic phases, magnetisation plateaus, and Bose-Einstein condensation of triplet excitations), the field-induced charge density wave (CDW) in high-Tc superconductors, and exotic superconductivity including the Fulde-Ferrel-Larkin-Ovchinnikov superconducting state and the field-induced superconductivity due to the Jaccarino-Peter mechanism.

Sharpening the second law of thermodynamics with the quantum Bayes theorem.

PubMed

Gharibyan, Hrant; Tegmark, Max

2014-09-01

We prove a generalization of the classic Groenewold-Lindblad entropy inequality, combining decoherence and the quantum Bayes theorem into a simple unified picture where decoherence increases entropy while observation decreases it. This provides a rigorous quantum-mechanical version of the second law of thermodynamics, governing how the entropy of a system (the entropy of its density matrix, partial-traced over the environment and conditioned on what is known) evolves under general decoherence and observation. The powerful tool of spectral majorization enables both simple alternative proofs of the classic Lindblad and Holevo inequalities without using strong subadditivity, and also novel inequalities for decoherence and observation that hold not only for von Neumann entropy, but also for arbitrary concave entropies.

Emergence of currents as a transient quantum effect in nonequilibrium systems

NASA Astrophysics Data System (ADS)

Granot, Er'El; Marchewka, Avi

2011-09-01

Most current calculations are based on equilibrium or semi-equilibrium models. However, except for very special scenarios (like ring configuration), the current cannot exist in equilibrium. Moreover, unlike with equilibrium scenarios, there is no generic approach to confront out-of-equilibrium currents. In this paper we used recent studies on transient quantum mechanics to solve the current, which appears in the presence of very high density gradients and fast transients. It shows that the emerging current appears instantaneously, and although the density beyond the discontinuity is initially negligible the currents there have a finite value, and remain constant for a finite period. It is shown that this nonequilibrium effect can be measured in real experiments (such as cooled rubidium atoms), where the discontinuity is replaced with a finite width (hundreds of nanometers) gradient.

Conduction mechanism change with transport oxide layer thickness in oxide hetero-interface diode

NASA Astrophysics Data System (ADS)

Nam, Bu-il; Park, Jong Seo; Lim, Keon-Hee; Ahn, Yong-keon; Lee, Jinwon; Park, Jun-woo; Cho, Nam-Kwang; Lee, Donggun; Lee, Han-Bo-Ram; Kim, Youn Sang

2017-07-01

An effective and facile strategy is proposed to demonstrate an engineered oxide hetero-interface of a thin film diode with a high current density and low operating voltage. The electrical characteristics of an oxide hetero-interface thin film diode are governed by two theoretical models: the space charge-limited current model and the Fowler-Nordheim (F-N) tunneling model. Interestingly, the dominant mechanism strongly depends on the insulator thickness, and the mechanism change occurs at a critical thickness. This paper shows that conduction mechanisms of oxide hetero-interface thin film diodes depend on thicknesses of transport oxide layers and that current densities of these can be exponentially increased through quantum tunneling in the diodes with the thicknesses less than 10 nm. These oxide hetero-interface diodes have great potential for low-powered transparent nanoscale applications.

Cosmological implications of quantum mechanics parametrization of dark energy

NASA Astrophysics Data System (ADS)

Szydłowski, Marek; Stachowski, Aleksander; Urbanowski, Krzysztof

2017-08-01

We consider the cosmology with the running dark energy. The parametrization of dark energy is derived from the quantum process of transition from the false vacuum state to the true vacuum state. This model is the generalized interacting CDM model. We consider the energy density of dark energy parametrization, which is given by the Breit-Wigner energy distribution function. The idea of the process of the quantum mechanical decay of unstable states was formulated by Krauss and Dent. We used this idea in our considerations. In this model is an energy transfer in the dark sector. In this evolutional scenario the universe starts from the false vacuum state and goes to the true vacuum state of the present day universe. The intermediate regime during the passage from false to true vacuum states takes place. In this way the cosmological constant problem can be tried to solve. We estimate the cosmological parameters for this model. This model is in a good agreement with the astronomical data and is practically indistinguishable from CDM model.

High mobility In0.75Ga0.25As quantum wells in an InAs phonon lattice

NASA Astrophysics Data System (ADS)

Chen, C.; Holmes, S. N.; Farrer, I.; Beere, H. E.; Ritchie, D. A.

2018-03-01

InGaAs based devices are great complements to silicon for CMOS, as they provide an increased carrier saturation velocity, lower operating voltage and reduced power dissipation (International technology roadmap for semiconductors (www.itrs2.net)). In this work we show that In0.75Ga0.25As quantum wells with a high mobility, 15 000 to 20 000 cm2 V-1 s-1 at ambient temperature, show an InAs-like phonon with an energy of 28.8 meV, frequency of 232 cm-1 that dominates the polar-optical mode scattering from  ˜70 K to 300 K. The measured optical phonon frequency is insensitive to the carrier density modulated with a surface gate or LED illumination. We model the electron scattering mechanisms as a function of temperature and identify mechanisms that limit the electron mobility in In0.75Ga0.25As quantum wells. Background impurity scattering starts to dominate for temperatures  <100 K. In the high mobility In0.75Ga0.25As quantum well, GaAs-like phonons do not couple to the electron gas unlike the case of In0.53Ga0.47As quantum wells.

Hidden Statistics Approach to Quantum Simulations

NASA Technical Reports Server (NTRS)

Zak, Michail

2010-01-01

Recent advances in quantum information theory have inspired an explosion of interest in new quantum algorithms for solving hard computational (quantum and non-quantum) problems. The basic principle of quantum computation is that the quantum properties can be used to represent structure data, and that quantum mechanisms can be devised and built to perform operations with this data. Three basic non-classical properties of quantum mechanics superposition, entanglement, and direct-product decomposability were main reasons for optimism about capabilities of quantum computers that promised simultaneous processing of large massifs of highly correlated data. Unfortunately, these advantages of quantum mechanics came with a high price. One major problem is keeping the components of the computer in a coherent state, as the slightest interaction with the external world would cause the system to decohere. That is why the hardware implementation of a quantum computer is still unsolved. The basic idea of this work is to create a new kind of dynamical system that would preserve the main three properties of quantum physics superposition, entanglement, and direct-product decomposability while allowing one to measure its state variables using classical methods. In other words, such a system would reinforce the advantages and minimize limitations of both quantum and classical aspects. Based upon a concept of hidden statistics, a new kind of dynamical system for simulation of Schroedinger equation is proposed. The system represents a modified Madelung version of Schroedinger equation. It preserves superposition, entanglement, and direct-product decomposability while allowing one to measure its state variables using classical methods. Such an optimal combination of characteristics is a perfect match for simulating quantum systems. The model includes a transitional component of quantum potential (that has been overlooked in previous treatment of the Madelung equation). The role of the transitional potential is to provide a jump from a deterministic state to a random state with prescribed probability density. This jump is triggered by blowup instability due to violation of Lipschitz condition generated by the quantum potential. As a result, the dynamics attains quantum properties on a classical scale. The model can be implemented physically as an analog VLSI-based (very-large-scale integration-based) computer, or numerically on a digital computer. This work opens a way of developing fundamentally new algorithms for quantum simulations of exponentially complex problems that expand NASA capabilities in conducting space activities. It has been illustrated that the complexity of simulations of particle interaction can be reduced from an exponential one to a polynomial one.

Force-field functor theory: classical force-fields which reproduce equilibrium quantum distributions

PubMed Central

Babbush, Ryan; Parkhill, John; Aspuru-Guzik, Alán

2013-01-01

Feynman and Hibbs were the first to variationally determine an effective potential whose associated classical canonical ensemble approximates the exact quantum partition function. We examine the existence of a map between the local potential and an effective classical potential which matches the exact quantum equilibrium density and partition function. The usefulness of such a mapping rests in its ability to readily improve Born-Oppenheimer potentials for use with classical sampling. We show that such a map is unique and must exist. To explore the feasibility of using this result to improve classical molecular mechanics, we numerically produce a map from a library of randomly generated one-dimensional potential/effective potential pairs then evaluate its performance on independent test problems. We also apply the map to simulate liquid para-hydrogen, finding that the resulting radial pair distribution functions agree well with path integral Monte Carlo simulations. The surprising accessibility and transferability of the technique suggest a quantitative route to adapting Born-Oppenheimer potentials, with a motivation similar in spirit to the powerful ideas and approximations of density functional theory. PMID:24790954

Multiscale Electrodynamics/Time-Dependent Density Functional Theory Modeling of Coupled Plasmon/Molecule Excitations

NASA Astrophysics Data System (ADS)

Lopata, Kenneth; Smith, Holden

The coupled dynamics of molecular chromophores and plasmons at surface of metal nanostructures are important for a range of processes such as molecular sensing, light harvesting, and near-field photochemistry. Modeling these dynamics from first principles, however, is challenging, as the large system sizes precludes a purely quantum mechanical treatment. In this talk I will present an approach based on propagating the plasmonic currents and fields using electrodynamics (finite-difference time-domain) with each chromophore described using an isolated quantum sub-region embedded in the overall classical background. This approach can be readily parallelized over these quantum regions, which enables large multiscale simulations of tens or hundreds of dyes, each of which is described individually by real-time time-dependent density functional theory. Application to gold nanoparticles coated with malachite green and rhodamine 6G monolayers shows good agreement with experimentally measured coupling spectra, including the polariton peaks, as well as the plasmon and molecular depletions. This research was supported by the Louisiana Board of Regents Research Competitiveness Subprogram under Contract Number LEQSF(2014-17)-RD-A-0.

Can quantum coherent solar cells break detailed balance?

NASA Astrophysics Data System (ADS)

Kirk, Alexander P.

2015-07-01

Carefully engineered coherent quantum states have been proposed as a design attribute that is hypothesized to enable solar photovoltaic cells to break the detailed balance (or radiative) limit of power conversion efficiency by possibly causing radiative recombination to be suppressed. However, in full compliance with the principles of statistical mechanics and the laws of thermodynamics, specially prepared coherent quantum states do not allow a solar photovoltaic cell—a quantum threshold energy conversion device—to exceed the detailed balance limit of power conversion efficiency. At the condition given by steady-state open circuit operation with zero nonradiative recombination, the photon absorption rate (or carrier photogeneration rate) must balance the photon emission rate (or carrier radiative recombination rate) thus ensuring that detailed balance prevails. Quantum state transitions, entropy-generating hot carrier relaxation, and photon absorption and emission rate balancing are employed holistically and self-consistently along with calculations of current density, voltage, and power conversion efficiency to explain why detailed balance may not be violated in solar photovoltaic cells.

Dynamics of the quantum search and quench-induced first-order phase transitions.

PubMed

Coulamy, Ivan B; Saguia, Andreia; Sarandy, Marcelo S

2017-02-01

We investigate the excitation dynamics at a first-order quantum phase transition (QPT). More specifically, we consider the quench-induced QPT in the quantum search algorithm, which aims at finding out a marked element in an unstructured list. We begin by deriving the exact dynamics of the model, which is shown to obey a Riccati differential equation. Then, we discuss the probabilities of success by adopting either global or local adiabaticity strategies. Moreover, we determine the disturbance of the quantum criticality as a function of the system size. In particular, we show that the critical point exponentially converges to its thermodynamic limit even in a fast evolution regime, which is characterized by both entanglement QPT estimators and the Schmidt gap. The excitation pattern is manifested in terms of quantum domain walls separated by kinks. The kink density is then shown to follow an exponential scaling as a function of the evolution speed, which can be interpreted as a Kibble-Zurek mechanism for first-order QPTs.

Study of quantum confinement effects in ZnO nanostructures

NASA Astrophysics Data System (ADS)

Movlarooy, Tayebeh

2018-03-01

Motivation to fact that zinc oxide nanowires and nanotubes with successful synthesis and the mechanism of formation, stability and electronic properties have been investigated; in this study the structural, electronic properties and quantum confinement effects of zinc oxide nanotubes and nanowires with different diameters are discussed. The calculations within density functional theory and the pseudo potential approximation are done. The electronic structure and energy gap for Armchair and zigzag ZnO nanotubes with a diameter of about 4 to 55 Angstrom and ZnO nanowires with a diameter range of 4 to 23 Å is calculated. The results revealed that due to the quantum confinement effects, by reducing the diameter of nanowires and nanotubes, the energy gap increases. Zinc oxide semiconductor nanostructures since having direct band gap with size-dependent and quantum confinement effect are recommended as an appropriate candidate for making nanoscale optoelectronic devices.

Decay of homogeneous two-dimensional quantum turbulence

NASA Astrophysics Data System (ADS)

Baggaley, Andrew W.; Barenghi, Carlo F.

2018-03-01

We numerically simulate the free decay of two-dimensional quantum turbulence in a large, homogeneous Bose-Einstein condensate. The large number of vortices, the uniformity of the density profile, and the absence of boundaries (where vortices can drift out of the condensate) isolate the annihilation of vortex-antivortex pairs as the only mechanism which reduces the number of vortices, Nv, during the turbulence decay. The results clearly reveal that vortex annihilation is a four-vortex process, confirming the decay law Nv˜t-1 /3 where t is time, which was inferred from experiments with relatively few vortices in small harmonically trapped condensates.

Why there is something rather than nothing: cosmological constant from summing over everything in lorentzian quantum gravity.

PubMed

Barvinsky, A O

2007-08-17

The density matrix of the Universe for the microcanonical ensemble in quantum cosmology describes an equipartition in the physical phase space of the theory (sum over everything), but in terms of the observable spacetime geometry this ensemble is peaked about the set of recently obtained cosmological instantons limited to a bounded range of the cosmological constant. This suggests the mechanism of constraining the landscape of string vacua and a possible solution to the dark energy problem in the form of the quasiequilibrium decay of the microcanonical state of the Universe.

Simple expression for the quantum Fisher information matrix

NASA Astrophysics Data System (ADS)

Šafránek, Dominik

2018-04-01

Quantum Fisher information matrix (QFIM) is a cornerstone of modern quantum metrology and quantum information geometry. Apart from optimal estimation, it finds applications in description of quantum speed limits, quantum criticality, quantum phase transitions, coherence, entanglement, and irreversibility. We derive a surprisingly simple formula for this quantity, which, unlike previously known general expression, does not require diagonalization of the density matrix, and is provably at least as efficient. With a minor modification, this formula can be used to compute QFIM for any finite-dimensional density matrix. Because of its simplicity, it could also shed more light on the quantum information geometry in general.

Extended Lagrangian Density Functional Tight-Binding Molecular Dynamics for Molecules and Solids.

PubMed

Aradi, Bálint; Niklasson, Anders M N; Frauenheim, Thomas

2015-07-14

A computationally fast quantum mechanical molecular dynamics scheme using an extended Lagrangian density functional tight-binding formulation has been developed and implemented in the DFTB+ electronic structure program package for simulations of solids and molecular systems. The scheme combines the computational speed of self-consistent density functional tight-binding theory with the efficiency and long-term accuracy of extended Lagrangian Born-Oppenheimer molecular dynamics. For systems without self-consistent charge instabilities, only a single diagonalization or construction of the single-particle density matrix is required in each time step. The molecular dynamics simulation scheme can be applied to a broad range of problems in materials science, chemistry, and biology.

A comprehensive evaluation of factors that influence the spin polarization of electrons emitted from bulk GaAs photocathodes

DOE PAGES

Liu, Wei; Poelker, Matt; Peng, Xincun; ...

2017-07-19

Here, the degree of polarization of photoemitted electrons extracted from bulk unstrained GaAs photocathodes is usually considerably less than the theoretical maximum value of 50%, as a result of depolarization mechanisms that originate within the photocathode material and at the vacuum surface interface. This paper provides a comprehensive review of depolarization mechanisms and presents a systematic experimental evaluation of polarization sensitivities to temperature, dopant density, quantum efficiency, and crystal orientation. The highest measured polarization was similar to 50%, consistent with the maximum theoretical value, obtained from a photocathode sample with relatively low dopant concentration and cooled to 77 K. Inmore » general, measurements indicate electron spin polarization can be enhanced at the expense of photoelectron yield (or quantum efficiency).« less

QSPR models for various physical properties of carbohydrates based on molecular mechanics and quantum chemical calculations.

PubMed

Dyekjaer, Jane Dannow; Jónsdóttir, Svava Osk

2004-01-22

Quantitative Structure-Property Relationships (QSPR) have been developed for a series of monosaccharides, including the physical properties of partial molar heat capacity, heat of solution, melting point, heat of fusion, glass-transition temperature, and solid state density. The models were based on molecular descriptors obtained from molecular mechanics and quantum chemical calculations, combined with other types of descriptors. Saccharides exhibit a large degree of conformational flexibility, therefore a methodology for selecting the energetically most favorable conformers has been developed, and was used for the development of the QSPR models. In most cases good correlations were obtained for monosaccharides. For five of the properties predictions were made for disaccharides, and the predicted values for the partial molar heat capacities were in excellent agreement with experimental values.

A comprehensive evaluation of factors that influence the spin polarization of electrons emitted from bulk GaAs photocathodes

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

Liu, Wei; Poelker, Matt; Peng, Xincun

Here, the degree of polarization of photoemitted electrons extracted from bulk unstrained GaAs photocathodes is usually considerably less than the theoretical maximum value of 50%, as a result of depolarization mechanisms that originate within the photocathode material and at the vacuum surface interface. This paper provides a comprehensive review of depolarization mechanisms and presents a systematic experimental evaluation of polarization sensitivities to temperature, dopant density, quantum efficiency, and crystal orientation. The highest measured polarization was similar to 50%, consistent with the maximum theoretical value, obtained from a photocathode sample with relatively low dopant concentration and cooled to 77 K. Inmore » general, measurements indicate electron spin polarization can be enhanced at the expense of photoelectron yield (or quantum efficiency).« less

Molecular Electron Density Theory: A Modern View of Reactivity in Organic Chemistry.

PubMed

Domingo, Luis R

2016-09-30

A new theory for the study of the reactivity in Organic Chemistry, named Molecular Electron Density Theory (MEDT), is proposed herein. MEDT is based on the idea that while the electron density distribution at the ground state is responsible for physical and chemical molecular properties, as proposed by the Density Functional Theory (DFT), the capability for changes in electron density is responsible for molecular reactivity. Within MEDT, the reactivity in Organic Chemistry is studied through a rigorous quantum chemical analysis of the changes of the electron density as well as the energies associated with these changes along the reaction path in order to understand experimental outcomes. Studies performed using MEDT allow establishing a modern rationalisation and to gain insight into molecular mechanisms and reactivity in Organic Chemistry.

Imaging the He2 quantum halo state using a free electron laser

PubMed Central

Zeller, Stefan; Kunitski, Maksim; Voigtsberger, Jörg; Kalinin, Anton; Schottelius, Alexander; Schober, Carl; Waitz, Markus; Sann, Hendrik; Hartung, Alexander; Bauer, Tobias; Pitzer, Martin; Trinter, Florian; Goihl, Christoph; Janke, Christian; Richter, Martin; Kastirke, Gregor; Weller, Miriam; Czasch, Achim; Kitzler, Markus; Braune, Markus; Grisenti, Robert E.; Schmidt, Lothar Ph. H.; Schöffler, Markus S.; Williams, Joshua B.; Jahnke, Till; Dörner, Reinhard

2016-01-01

Quantum tunneling is a ubiquitous phenomenon in nature and crucial for many technological applications. It allows quantum particles to reach regions in space which are energetically not accessible according to classical mechanics. In this “tunneling region,” the particle density is known to decay exponentially. This behavior is universal across all energy scales from nuclear physics to chemistry and solid state systems. Although typically only a small fraction of a particle wavefunction extends into the tunneling region, we present here an extreme quantum system: a gigantic molecule consisting of two helium atoms, with an 80% probability that its two nuclei will be found in this classical forbidden region. This circumstance allows us to directly image the exponentially decaying density of a tunneling particle, which we achieved for over two orders of magnitude. Imaging a tunneling particle shows one of the few features of our world that is truly universal: the probability to find one of the constituents of bound matter far away is never zero but decreases exponentially. The results were obtained by Coulomb explosion imaging using a free electron laser and furthermore yielded He2’s binding energy of 151.9±13.3 neV, which is in agreement with most recent calculations. PMID:27930299

Strain-Engineering of Graphene Based Topological Quantum Devices

NASA Astrophysics Data System (ADS)

Diniz, Ginetom S.; Guassi, Marcos R.; Qu, Fanyao

2015-03-01

We have investigated the spin-charge transport in quantum devices based on graphene nanoribbons (GNR). Our calculation is based on the surface Green's function technique, considering the presence of an uniform uniaxial strain, spin-orbit interactions (SOIs), exchange field and a smooth staggered potential. We propose the use of uniaxial strain as an efficient mechanism to tune the conductance profiles of GNR with different edge terminations. Our results show that distinct behaviors can be achieved: for armchair GNR there is a complete suppression of the conductance close to the Fermi level with the formation of a band gap that depends on the direction and strength of the strain deformation, while for zigzag GNR there is only a small conductance suppression. We also discuss the effects of SOIs and the appearance of spin-resolved conductance oscillations, and the local density of states of these GNR devices in the quantum anomalous Hall regime. Furthermore, we demonstrate that the local density of states show that depending on the smoothness of the staggered potential, the edge states of AGNR can either emerge or be suppressed. These emerging states can be probed by scanning tunneling microscope. Our findings can be potentially used in novel GNR based topological quantum devices. Supported by FAP-DF, CNPq and CAPES.

Particle detection and non-detection in a quantum time of arrival measurement

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

Sombillo, Denny Lane B., E-mail: dsombillo@nip.upd.edu.ph; Galapon, Eric A.

2016-01-15

The standard time-of-arrival distribution cannot reproduce both the temporal and the spatial profile of the modulus squared of the time-evolved wave function for an arbitrary initial state. In particular, the time-of-arrival distribution gives a non-vanishing probability even if the wave function is zero at a given point for all values of time. This poses a problem in the standard formulation of quantum mechanics where one quantizes a classical observable and uses its spectral resolution to calculate the corresponding distribution. In this work, we show that the modulus squared of the time-evolved wave function is in fact contained in one ofmore » the degenerate eigenfunctions of the quantized time-of-arrival operator. This generalizes our understanding of quantum arrival phenomenon where particle detection is not a necessary requirement, thereby providing a direct link between time-of-arrival quantization and the outcomes of the two-slit experiment. -- Highlights: •The time-evolved position density is contained in the standard TOA distribution. •Particle may quantum mechanically arrive at a given point without being detected. •The eigenstates of the standard TOA operator are linked to the two-slit experiment.« less

Study of Exciton Hopping Transport in PbS Colloidal Quantum Dot Thin Films Using Frequency- and Temperature-Scanned Photocarrier Radiometry

NASA Astrophysics Data System (ADS)

Hu, Lilei; Mandelis, Andreas; Melnikov, Alexander; Lan, Xinzheng; Hoogland, Sjoerd; Sargent, Edward H.

2017-01-01

Solution-processed colloidal quantum dots (CQDs) are promising materials for realizing low-cost, large-area, and flexible photovoltaic devices. The study of charge carrier transport in quantum dot solids is essential for understanding energy conversion mechanisms. Recently, solution-processed two-layer oleic-acid-capped PbS CQD solar cells with one layer treated with tetrabutylammonium iodide (TBAI) serving as the main light-absorbing layer and the other treated with 1,2-ethanedithiol (EDT) acting as an electron-blocking/hole-extraction layer were reported. These solar cells demonstrated a significant improvement in power conversion efficiency of 8.55% and long-term air stability. Coupled with photocarrier radiometry measurements, this work used a new trap-state mediated exciton hopping transport model, specifically for CQD thin films, to unveil and quantify exciton transport mechanisms through the extraction of hopping transport parameters including exciton lifetimes, hopping diffusivity, exciton detrapping time, and trap-state density. It is shown that PbS-TBAI has higher trap-state density than PbS-EDT that results in higher PbS-EDT exciton lifetimes. Hopping diffusivities of both CQD thin film types show similar temperature dependence, particularly higher temperatures yield higher hopping diffusivity. The higher diffusivity of PbS-TBAI compared with PbS-EDT indicates that PbS-TBAI is a much better photovoltaic material than PbS-EDT. Furthermore, PCR temperature spectra and deep-level photothermal spectroscopy provided additional insights to CQD surface trap states: PbS-TBAI thin films exhibit a single dominant trap level, while PbS-EDT films with lower trap-state densities show multiple trap levels.

Efficient grid-based techniques for density functional theory

NASA Astrophysics Data System (ADS)

Rodriguez-Hernandez, Juan Ignacio

Understanding the chemical and physical properties of molecules and materials at a fundamental level often requires quantum-mechanical models for these substance's electronic structure. This type of many body quantum mechanics calculation is computationally demanding, hindering its application to substances with more than a few hundreds atoms. The supreme goal of many researches in quantum chemistry---and the topic of this dissertation---is to develop more efficient computational algorithms for electronic structure calculations. In particular, this dissertation develops two new numerical integration techniques for computing molecular and atomic properties within conventional Kohn-Sham-Density Functional Theory (KS-DFT) of molecular electronic structure. The first of these grid-based techniques is based on the transformed sparse grid construction. In this construction, a sparse grid is generated in the unit cube and then mapped to real space according to the pro-molecular density using the conditional distribution transformation. The transformed sparse grid was implemented in program deMon2k, where it is used as the numerical integrator for the exchange-correlation energy and potential in the KS-DFT procedure. We tested our grid by computing ground state energies, equilibrium geometries, and atomization energies. The accuracy on these test calculations shows that our grid is more efficient than some previous integration methods: our grids use fewer points to obtain the same accuracy. The transformed sparse grids were also tested for integrating, interpolating and differentiating in different dimensions (n = 1,2,3,6). The second technique is a grid-based method for computing atomic properties within QTAIM. It was also implemented in deMon2k. The performance of the method was tested by computing QTAIM atomic energies, charges, dipole moments, and quadrupole moments. For medium accuracy, our method is the fastest one we know of.

Accuracy of the adiabatic-impulse approximation for closed and open quantum systems

NASA Astrophysics Data System (ADS)

Tomka, Michael; Campos Venuti, Lorenzo; Zanardi, Paolo

2018-03-01

We study the adiabatic-impulse approximation (AIA) as a tool to approximate the time evolution of quantum states when driven through a region of small gap. Such small-gap regions are a common situation in adiabatic quantum computing and having reliable approximations is important in this context. The AIA originates from the Kibble-Zurek theory applied to continuous quantum phase transitions. The Kibble-Zurek mechanism was developed to predict the power-law scaling of the defect density across a continuous quantum phase transition. Instead, here we quantify the accuracy of the AIA via the trace norm distance with respect to the exact evolved state. As expected, we find that for short times or fast protocols, the AIA outperforms the simple adiabatic approximation. However, for large times or slow protocols, the situation is actually reversed and the AIA provides a worse approximation. Nevertheless, we found a variation of the AIA that can perform better than the adiabatic one. This counterintuitive modification consists in crossing the region of small gap twice. Our findings are illustrated by several examples of driven closed and open quantum systems.

Effects of mechanical strain on the performance of germanene sheets: Strength, failure behavior, and electronic structure

NASA Astrophysics Data System (ADS)

Ding, Ning; Wang, Huan; Liu, Long; Guo, Weimin; Chen, Xiangfeng; Wu, Chi-Man Lawrence

2018-02-01

As a two-dimensional material with a low-buckling structure, germanene has attracted considerable interest because of its excellent physical properties, such as massless Dirac fermions and quantum spin Hall effect. The mechanical characteristics of germanene are of the utmost importance when one is assessing its viability for nanodevices, especially for ones with defects. In this work, the stabilities, mechanical properties, and changes in electronic properties under mechanical strain for both pristine and defective germanene sheets were studied and analyzed with use of density functional theory. The mechanical properties of defect-free germanene exhibited obvious anisotropy along different directions. The mechanical properties of germanene sheets exhibited high sensitivity to the defect parameters, such as the linear density of vacancies, the width of the cracks, and the inflection angles caused by the grain boundaries. In addition, the applied mechanical strain changed the electronic properties of germanene to a large extent. The information obtained will be useful for the understanding and potential application of germanene.

Quantum computing without wavefunctions: time-dependent density functional theory for universal quantum computation.

PubMed

Tempel, David G; Aspuru-Guzik, Alán

2012-01-01

We prove that the theorems of TDDFT can be extended to a class of qubit Hamiltonians that are universal for quantum computation. The theorems of TDDFT applied to universal Hamiltonians imply that single-qubit expectation values can be used as the basic variables in quantum computation and information theory, rather than wavefunctions. From a practical standpoint this opens the possibility of approximating observables of interest in quantum computations directly in terms of single-qubit quantities (i.e. as density functionals). Additionally, we also demonstrate that TDDFT provides an exact prescription for simulating universal Hamiltonians with other universal Hamiltonians that have different, and possibly easier-to-realize two-qubit interactions. This establishes the foundations of TDDFT for quantum computation and opens the possibility of developing density functionals for use in quantum algorithms.

The open quantum Brownian motions

NASA Astrophysics Data System (ADS)

Bauer, Michel; Bernard, Denis; Tilloy, Antoine

2014-09-01

Using quantum parallelism on random walks as the original seed, we introduce new quantum stochastic processes, the open quantum Brownian motions. They describe the behaviors of quantum walkers—with internal degrees of freedom which serve as random gyroscopes—interacting with a series of probes which serve as quantum coins. These processes may also be viewed as the scaling limit of open quantum random walks and we develop this approach along three different lines: the quantum trajectory, the quantum dynamical map and the quantum stochastic differential equation. We also present a study of the simplest case, with a two level system as an internal gyroscope, illustrating the interplay between the ballistic and diffusive behaviors at work in these processes. Notation H_z : orbital (walker) Hilbert space, {C}^{{Z}} in the discrete, L^2({R}) in the continuum H_c : internal spin (or gyroscope) Hilbert space H_sys=H_z\\otimesH_c : system Hilbert space H_p : probe (or quantum coin) Hilbert space, H_p={C}^2 \\rho^tot_t : density matrix for the total system (walker + internal spin + quantum coins) \\bar \\rho_t : reduced density matrix on H_sys : \\bar\\rho_t=\\int dxdy\\, \\bar\\rho_t(x,y)\\otimes | x \\rangle _z\\langle y | \\hat \\rho_t : system density matrix in a quantum trajectory: \\hat\\rho_t=\\int dxdy\\, \\hat\\rho_t(x,y)\\otimes | x \\rangle _z\\langle y | . If diagonal and localized in position: \\hat \\rho_t=\\rho_t\\otimes| X_t \\rangle _z\\langle X_t | ρt: internal density matrix in a simple quantum trajectory Xt: walker position in a simple quantum trajectory Bt: normalized Brownian motion ξt, \\xi_t^\\dagger : quantum noises

Quantum dissipation theory and applications to quantum transport and quantum measurement in mesoscopic systems

NASA Astrophysics Data System (ADS)

Cui, Ping

The thesis comprises two major themes of quantum statistical dynamics. One is the development of quantum dissipation theory (QDT). It covers the establishment of some basic relations of quantum statistical dynamics, the construction of several nonequivalent complete second-order formulations, and the development of exact QDT. Another is related to the applications of quantum statistical dynamics to a variety of research fields. In particular, unconventional but novel theories of the electron transfer in Debye solvents, quantum transport, and quantum measurement are developed on the basis of QDT formulations. The thesis is organized as follows. In Chapter 1, we present some background knowledge in relation to the aforementioned two themes of this thesis. The key quantity in QDT is the reduced density operator rho(t) ≡ trBrho T(t); i.e., the partial trace of the total system and bath composite rhoT(t) over the bath degrees of freedom. QDT governs the evolution of reduced density operator, where the effects of bath are treated in a quantum statistical manner. In principle, the reduced density operator contains all dynamics information of interest. However, the conventional quantum transport theory is formulated in terms of nonequilibrium Green's function. The newly emerging field of quantum measurement in relation to quantum information and quantum computing does exploit a sort of QDT formalism. Besides the background of the relevant theoretical development, some representative experiments on molecular nanojunctions are also briefly discussed. In chapter 2, we outline some basic (including new) relations that highlight several important issues on QDT. The content includes the background of nonequilibrium quantum statistical mechanics, the general description of the total composite Hamiltonian with stochastic system-bath interaction, a novel parameterization scheme for bath correlation functions, a newly developed exact theory of driven Brownian oscillator (DBO) systems, and its closely related solvation mode transformation of system-bath coupling Hamiltonian in general. The exact QDT of DBO systems is also used to clarify the validity of conventional QDT formulations that involve Markovian approximation. In Chapter 3, we develop three nonequivalent but all complete second-order QDT (CS-QDT) formulations. Two of them are of the conventional prescriptions in terms of time-local dissipation and memory kernel, respectively. The third one is called the correlated driving-dissipation equations of motion (CODDE). This novel CS-QDT combines the merits of the former two for its advantages in both the application and numerical implementation aspects. Also highlighted is the importance of correlated driving-dissipation effects on the dynamics of the reduced system. In Chapter 4, we construct an exact QDT formalism via the calculus on path integrals. The new theory aims at the efficient evaluation of non-Markovian dissipation beyond the weak system-bath interaction regime in the presence of time-dependent external field. By adopting exponential-like expansions for bath correlation function, hierarchical equations of motion formalism and continued fraction Liouville-space Green's function formalism are established. The latter will soon be used together with the Dyson equation technique for an efficient evaluation of non-perturbative reduced density matrix dynamics. The interplay between system-bath interaction strength, non-Markovian property, and the required level of hierarchy is also studied with the aid of simple spin-boson systems, together with the three proposed schemes to truncate the infinite hierarchy. In Chapter 5, we develop a nonperturbative theory of electron transfer (ET) in Debye solvents. The resulting exact and analytical rate expression is constructed on the basis of the aforementioned continued fraction Liouville-space Green's function formalism, together with the Dyson equation technique. Not only does it recover the celebrated Marcus' inversion and Kramers' turnover behaviors, the new theory also shows some distinct quantum solvation effects that can alter the ET mechanism. Moreover, the present theory predicts further for the ET reaction thermodynamics, such as equilibrium Gibbs free-energy and entropy, some interesting solvent-dependent features that are calling for experimental verification. In Chapter 6, we discuss the constructed QDTs, in terms of their unified mathematical structure that supports a linear dynamics space, and thus facilitates their applications to various physical problems. The involving details are exemplified with the CODDE form of QDT. As the linear space is concerned, we identify the Schrodinger versus Heisenberg picture and the forward versus backward propagation of the reduced, dissipative Liouville dynamics. For applications we discuss the reduced linear response theory and the optimal control problems, in which the correlated effects of non-Markovian dissipation and field driving are shown to be important. In Chapter 7, we turn to quantum transport, i.e., electric current through molecular or mesoscopic systems under finite applied voltage. By viewing the nonequilibrium transport setup as a quantum open system, we develop a reduced-density-matrix approach to quantum transport. The resulting current is explicitly expressed in terms of the molecular reduced density matrix by tracing out the degrees of freedom of the electrodes at finite bias and temperature. We propose a conditional quantum master equation theory, which is an extension of the conventional (or unconditional) QDT by tracing out the well-defined bath subsets individually, instead of the entire bath degrees of freedom. Both the current and the noise spectrum can be conveniently analyzed in terms of the conditional reduced density matrix dynamics. By far, the QDT (including the conditional one) has only been exploited in second-order form. A self-consistent Born approximation for the system-electrode coupling is further proposed to recover all existing nonlinear current-voltage behaviors including the nonequilibrium Kondo effect. Transport theory based on the exact QDT formalism will be developed in future. In Chapter 8, we study the quantum measurement of a qubit with a quantum-point-contact detector. On the basis of a unified quantum master equation (a form of QDT), we study the measurement-induced relaxation and dephasing of the qubit. Our treatment pays particular attention on the detailed-balance relation, which is a consequence of properly accounting for the energy exchange between the qubit and detector during the measurement process. We also derive a conditional quantum master equation for quantum measurement in general, and study the readout characteristics of the qubit measurement. Our theory is applicable to the quantum measurement at arbitrary voltage and temperature. A number of remarkable new features are found and highlighted in concern with their possible relevance to future experiments. In Chapter 9, we discuss the further development of QDT, aiming at an efficient evaluation of many-electron systems. This will be carried out by reducing the many-particle (Fermion or Boson) QDT to a single-particle one by exploring, e.g. the Wick's contraction theorem. It also results in a time-dependent density functional theory (TDDFT) for transport through complex large-scale (e.g. molecules) systems. Primary results of the TDDFT-QDT are reported. In Chapter 10, we summary the thesis, and comment and remark on the future work on both the theoretical and application aspects of QDT.

Lieb-Thirring inequality for a model of particles with point interactions

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

Frank, Rupert L.; Seiringer, Robert

2012-09-15

We consider a model of quantum-mechanical particles interacting via point interactions of infinite scattering length. In the case of fermions we prove a Lieb-Thirring inequality for the energy, i.e., we show that the energy is bounded from below by a constant times the integral of the particle density to the power (5/3).

Renormalization of myoglobin–ligand binding energetics by quantum many-body effects

PubMed Central

Weber, Cédric; Cole, Daniel J.; O’Regan, David D.; Payne, Mike C.

2014-01-01

We carry out a first-principles atomistic study of the electronic mechanisms of ligand binding and discrimination in the myoglobin protein. Electronic correlation effects are taken into account using one of the most advanced methods currently available, namely a linear-scaling density functional theory (DFT) approach wherein the treatment of localized iron 3d electrons is further refined using dynamical mean-field theory. This combination of methods explicitly accounts for dynamical and multireference quantum physics, such as valence and spin fluctuations, of the 3d electrons, while treating a significant proportion of the protein (more than 1,000 atoms) with DFT. The computed electronic structure of the myoglobin complexes and the nature of the Fe–O2 bonding are validated against experimental spectroscopic observables. We elucidate and solve a long-standing problem related to the quantum-mechanical description of the respiration process, namely that DFT calculations predict a strong imbalance between O2 and CO binding, favoring the latter to an unphysically large extent. We show that the explicit inclusion of the many-body effects induced by the Hund’s coupling mechanism results in the correct prediction of similar binding energies for oxy- and carbonmonoxymyoglobin. PMID:24717844

Quantum-limited heat conduction over macroscopic distances

PubMed Central

Partanen, Matti; Tan, Kuan Yen; Govenius, Joonas; Lake, Russell E.; Mäkelä, Miika K.; Tanttu, Tuomo; Möttönen, Mikko

2016-01-01

The emerging quantum technological apparatuses1, 2, such as the quantum computer3–6, call for extreme performance in thermal engineering7. Cold distant heat sinks are needed for the quantized electric degrees of freedom due to the increasing packaging density and heat dissipation. Importantly, quantum mechanics sets a fundamental upper limit for the flow of information and heat, which is quantified by the quantum of thermal conductance8–10. However, the short distance between the heat-exchanging bodies in the previous experiments11–14 hinders their applicability in quantum technology. Here, we present experimental observations of quantum-limited heat conduction over macroscopic distances extending to a metre. We achieved this improvement of four orders of magnitude in the distance by utilizing microwave photons travelling in superconducting transmission lines. Thus, it seems that quantum-limited heat conduction has no fundamental distance cutoff. This work establishes the integration of normal-metal components into the framework of circuit quantum electrodynamics15–17 which provides a basis for the superconducting quantum computer18–21. Especially, our results facilitate remote cooling of nanoelectronic devices using far-away in-situ-tunable heat sinks22, 23. Furthermore, quantum-limited heat conduction is important in contemporary thermodynamics24, 25. Here, the long distance may lead to ultimately efficient mesoscopic heat engines with promising practical applications26. PMID:27239219

Quantum Time Evolution in a Qubit Readout Process with a Josephson Bifurcation Amplifier

NASA Astrophysics Data System (ADS)

Nakano, Hayato; Saito, Shiro; Semba, Kouichi; Takayanagi, Hideaki

2009-06-01

We analyzed the Josephson bifurcation amplifier (JBA) readout process of a superconducting qubit quantum mechanically by calculating the dynamics of the density operator of a driven nonlinear oscillator and a qubit coupled system during the measurement process. In purely quantum cases, bifurcation is impossible. Introducing decoherence enables us to reproduce the bifurcation with a finite hysteresis. When a qubit is initially in a superposition state, we have observed the qubit-probe (JBA) entangled state, and it is divided into two separable states at the moment the JBA transition begins. This corresponds to “projection.” To readout the measurement result, however, we must wait until the two JBA states are macroscopically well separated. The waiting time is determined by the strength of the decoherence in the JBA.

An unscaled quantum mechanical harmonic force field for p-benzoquinone

NASA Astrophysics Data System (ADS)

Nonella, Marco; Tavan, Paul

1995-10-01

Structure and harmonic vibrational frequencies of p-benzoquinone have been calculated using quantum chemical ab initio and density functional methods. Our calculations show that a satisfactory description of fundamentals and normal mode compositions is achieved upon consideration of correlation effects by means of Møller-Plesset perturbation expansion (MP2) or by density functional theory (DFT). Furthermore, for correct prediction of CO bondlength and force constant, basis sets augmented by polarization functions are required. Applying such basis sets, MP2 and DFT calculations both give results which are generally in reasonable agreement with experimental data. The quantitatively better agreement, however, is achieved with the computationally less demanding DFT method. This method particularly allows very precise prediction of the experimentally important absorptions in the frequency region between 1500 and 1800 cm -1 and of the isotopic shifts of these vibrations due to 13C or 18O substitution.

Relativistic self-focusing of ultra-high intensity X-ray laser beams in warm quantum plasma with upward density profile

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

Habibi, M., E-mail: habibi.physics@gmail.com; Ghamari, F.

2014-05-15

The results of a numerical study of high-intensity X-ray laser beam interaction with warm quantum plasma (WQP) are presented. By means of an upward ramp density profile combined with quantum factors specially the Fermi velocity, we have demonstrated significant relativistic self-focusing (RSF) of a Gaussian electromagnetic beam in the WQP where the Fermi temperature term in the dielectric function is important. For this purpose, we have considered the quantum hydrodynamics model that modifies refractive index of inhomogeneous WQPs with the inclusion of quantum correction through the quantum statistical and diffraction effects in the relativistic regime. Also, to better illustration ofmore » the physical difference between warm and cold quantum plasmas and their effect on the RSF, we have derived the envelope equation governing the spot size of X-ray laser beam in Q-plasmas. In addition to the upward ramp density profile, we have found that the quantum effects would be caused much higher oscillation and better focusing of X-ray laser beam in the WQP compared to that of cold quantum case. Our computational results reveal the importance of the use of electrons density profile and Fermi speed in enhancing self-focusing of laser beam.« less

Transferring elements of a density matrix

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

Allahverdyan, Armen E.; Hovhannisyan, Karen V.; Yerevan State University, A. Manoogian Street 1, Yerevan

2010-01-15

We study restrictions imposed by quantum mechanics on the process of matrix-element transfer. This problem is at the core of quantum measurements and state transfer. Given two systems A and B with initial density matrices lambda and r, respectively, we consider interactions that lead to transferring certain matrix elements of unknown lambda into those of the final state r-tilde of B. We find that this process eliminates the memory on the transferred (or certain other) matrix elements from the final state of A. If one diagonal matrix element is transferred, r(tilde sign){sub aa}=lambda{sub aa}, the memory on each nondiagonal elementmore » lambda{sub an}ot ={sub b} is completely eliminated from the final density operator of A. Consider the following three quantities, Relambda{sub an}ot ={sub b}, Imlambda{sub an}ot ={sub b}, and lambda{sub aa}-lambda{sub bb} (the real and imaginary part of a nondiagonal element and the corresponding difference between diagonal elements). Transferring one of them, e.g., Rer(tilde sign){sub an}ot ={sub b}=Relambda{sub an}ot ={sub b}, erases the memory on two others from the final state of A. Generalization of these setups to a finite-accuracy transfer brings in a trade-off between the accuracy and the amount of preserved memory. This trade-off is expressed via system-independent uncertainty relations that account for local aspects of the accuracy-disturbance trade-off in quantum measurements. Thus, the general aspect of state disturbance in quantum measurements is elimination of memory on non-diagonal elements, rather than diagonalization.« less

Biomolecular Force Field Parameterization via Atoms-in-Molecule Electron Density Partitioning.

PubMed

Cole, Daniel J; Vilseck, Jonah Z; Tirado-Rives, Julian; Payne, Mike C; Jorgensen, William L

2016-05-10

Molecular mechanics force fields, which are commonly used in biomolecular modeling and computer-aided drug design, typically treat nonbonded interactions using a limited library of empirical parameters that are developed for small molecules. This approach does not account for polarization in larger molecules or proteins, and the parametrization process is labor-intensive. Using linear-scaling density functional theory and atoms-in-molecule electron density partitioning, environment-specific charges and Lennard-Jones parameters are derived directly from quantum mechanical calculations for use in biomolecular modeling of organic and biomolecular systems. The proposed methods significantly reduce the number of empirical parameters needed to construct molecular mechanics force fields, naturally include polarization effects in charge and Lennard-Jones parameters, and scale well to systems comprised of thousands of atoms, including proteins. The feasibility and benefits of this approach are demonstrated by computing free energies of hydration, properties of pure liquids, and the relative binding free energies of indole and benzofuran to the L99A mutant of T4 lysozyme.

Simulations of defect spin qubits in piezoelectric semiconductors

NASA Astrophysics Data System (ADS)

Seo, Hosung

In recent years, remarkable advances have been reported in the development of defect spin qubits in semiconductors for solid-state quantum information science and quantum metrology. Promising spin qubits include the nitrogen-vacancy center in diamond, dopants in silicon, and the silicon vacancy and divacancy spins in silicon carbide. In this talk, I will highlight some of our recent efforts devoted to defect spin qubits in piezoelectric wide-gap semiconductors for potential applications in mechanical hybrid quantum systems. In particular, I will describe our recent combined theoretical and experimental study on remarkably robust quantum coherence found in the divancancy qubits in silicon carbide. We used a quantum bath model combined with a cluster expansion method to identify the microscopic mechanisms behind the unusually long coherence times of the divacancy spins in SiC. Our study indicates that developing spin qubits in complex crystals with multiple types of atom is a promising route to realize strongly coherent hybrid quantum systems. I will also discuss progress and challenges in computational design of new spin defects for use as qubits in piezoelectric crystals such as AlN and SiC, including a new defect design concept using large metal ion - vacancy complexes. Our first principles calculations include DFT computations using recently developed self-consistent hybrid density functional theory and large-scale many-body GW theory. This work was supported by the National Science Foundation (NSF) through the University of Chicago MRSEC under Award Number DMR-1420709.

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

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

Sirjoosingh, Andrew; Pak, Michael V.; Brorsen, Kurt R.

2015-06-07

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

Quantum mechanical study and spectroscopic (FT-IR, FT-Raman, 13C, 1H) study, first order hyperpolarizability, NBO analysis, HOMO and LUMO analysis of 2-acetoxybenzoic acid by density functional methods

NASA Astrophysics Data System (ADS)

Bhavani, K.; Renuga, S.; Muthu, S.; Sankara narayanan, K.

2015-02-01

In this work, colorless crystals of 2-acetoxybenzoic acid were grown by slow evaporation method and the FT-IR and FT-Raman spectra of the sample were recorded in the region 4000-500 cm-1 and 4000-100 cm-1 respectively. Molecular structure is optimized with the help of density functional theory method (B3LYP) with 6-31+G(d,p), 6-311++G(d,p) basis sets. Stability of the molecule arising from hyperconjugation and charge delocalization is confirmed by the natural bond orbital analysis (NBO). The results show that electron density (ED) in the σ∗ antibonding orbitals and E(2) energies confirms the occurrence of intramolecular charge transfer (ICT) within the molecule. The assignments of the vibrational spectra have been carried out with the help of normal coordinate analysis following the scaled quantum mechanical force field (SQMFF) methodology. The results of the calculations were applied to simulated spectra of the title compound, which show excellent agreement with observed spectra. The 1H and 13C nuclear magnetic resonance (NMR) chemical shifts of the molecule were calculated by GIAO method. Mulliken population analysis on atomic charges is also calculated. The calculated HOMO and LUMO energy gap shows that charge transfer occurs within the molecule.

Revealing electronic open quantum systems with subsystem TDDFT

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

Krishtal, Alisa, E-mail: alisa.krishtal@rutgers.edu; Pavanello, Michele, E-mail: m.pavanello@rutgers.edu

2016-03-28

Open quantum systems (OQSs) are perhaps the most realistic systems one can approach through simulations. In recent years, describing OQSs with Density Functional Theory (DFT) has been a prominent avenue of research with most approaches based on a density matrix partitioning in conjunction with an ad-hoc description of system-bath interactions. We propose a different theoretical approach to OQSs based on partitioning of the electron density. Employing the machinery of subsystem DFT (and its time-dependent extension), we provide a novel way of isolating and analyzing the various terms contributing to the coupling between the system and the surrounding bath. To illustratemore » the theory, we provide numerical simulations on a toy system (a molecular dimer) and on a condensed phase system (solvated excimer). The simulations show that non-Markovian dynamics in the electronic system-bath interactions are important in chemical applications. For instance, we show that the superexchange mechanism of transport in donor-bridge-acceptor systems is a non-Markovian interaction between the donor-acceptor (OQS) with the bridge (bath) which is fully characterized by real-time subsystem time-dependent DFT.« less

Revealing electronic open quantum systems with subsystem TDDFT.

PubMed

Krishtal, Alisa; Pavanello, Michele

2016-03-28

Open quantum systems (OQSs) are perhaps the most realistic systems one can approach through simulations. In recent years, describing OQSs with Density Functional Theory (DFT) has been a prominent avenue of research with most approaches based on a density matrix partitioning in conjunction with an ad-hoc description of system-bath interactions. We propose a different theoretical approach to OQSs based on partitioning of the electron density. Employing the machinery of subsystem DFT (and its time-dependent extension), we provide a novel way of isolating and analyzing the various terms contributing to the coupling between the system and the surrounding bath. To illustrate the theory, we provide numerical simulations on a toy system (a molecular dimer) and on a condensed phase system (solvated excimer). The simulations show that non-Markovian dynamics in the electronic system-bath interactions are important in chemical applications. For instance, we show that the superexchange mechanism of transport in donor-bridge-acceptor systems is a non-Markovian interaction between the donor-acceptor (OQS) with the bridge (bath) which is fully characterized by real-time subsystem time-dependent DFT.

Revealing electronic open quantum systems with subsystem TDDFT

NASA Astrophysics Data System (ADS)

Krishtal, Alisa; Pavanello, Michele

2016-03-01

Open quantum systems (OQSs) are perhaps the most realistic systems one can approach through simulations. In recent years, describing OQSs with Density Functional Theory (DFT) has been a prominent avenue of research with most approaches based on a density matrix partitioning in conjunction with an ad-hoc description of system-bath interactions. We propose a different theoretical approach to OQSs based on partitioning of the electron density. Employing the machinery of subsystem DFT (and its time-dependent extension), we provide a novel way of isolating and analyzing the various terms contributing to the coupling between the system and the surrounding bath. To illustrate the theory, we provide numerical simulations on a toy system (a molecular dimer) and on a condensed phase system (solvated excimer). The simulations show that non-Markovian dynamics in the electronic system-bath interactions are important in chemical applications. For instance, we show that the superexchange mechanism of transport in donor-bridge-acceptor systems is a non-Markovian interaction between the donor-acceptor (OQS) with the bridge (bath) which is fully characterized by real-time subsystem time-dependent DFT.

Extended Lagrangian Density Functional Tight-Binding Molecular Dynamics for Molecules and Solids

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

Aradi, Bálint; Niklasson, Anders M. N.; Frauenheim, Thomas

A computationally fast quantum mechanical molecular dynamics scheme using an extended Lagrangian density functional tight-binding formulation has been developed and implemented in the DFTB+ electronic structure program package for simulations of solids and molecular systems. The scheme combines the computational speed of self-consistent density functional tight-binding theory with the efficiency and long-term accuracy of extended Lagrangian Born–Oppenheimer molecular dynamics. Furthermore, for systems without self-consistent charge instabilities, only a single diagonalization or construction of the single-particle density matrix is required in each time step. The molecular dynamics simulation scheme can also be applied to a broad range of problems in materialsmore » science, chemistry, and biology.« less

Extended Lagrangian Density Functional Tight-Binding Molecular Dynamics for Molecules and Solids

DOE PAGES

Aradi, Bálint; Niklasson, Anders M. N.; Frauenheim, Thomas

2015-06-26

A computationally fast quantum mechanical molecular dynamics scheme using an extended Lagrangian density functional tight-binding formulation has been developed and implemented in the DFTB+ electronic structure program package for simulations of solids and molecular systems. The scheme combines the computational speed of self-consistent density functional tight-binding theory with the efficiency and long-term accuracy of extended Lagrangian Born–Oppenheimer molecular dynamics. Furthermore, for systems without self-consistent charge instabilities, only a single diagonalization or construction of the single-particle density matrix is required in each time step. The molecular dynamics simulation scheme can also be applied to a broad range of problems in materialsmore » science, chemistry, and biology.« less

Electronic field emission models beyond the Fowler-Nordheim one

NASA Astrophysics Data System (ADS)

Lepetit, Bruno

2017-12-01

We propose several quantum mechanical models to describe electronic field emission from first principles. These models allow us to correlate quantitatively the electronic emission current with the electrode surface details at the atomic scale. They all rely on electronic potential energy surfaces obtained from three dimensional density functional theory calculations. They differ by the various quantum mechanical methods (exact or perturbative, time dependent or time independent), which are used to describe tunneling through the electronic potential energy barrier. Comparison of these models between them and with the standard Fowler-Nordheim one in the context of one dimensional tunneling allows us to assess the impact on the accuracy of the computed current of the approximations made in each model. Among these methods, the time dependent perturbative one provides a well-balanced trade-off between accuracy and computational cost.

Unraveling hadron structure with generalized parton distributions

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

Andrei Belitsky; Anatoly Radyushkin

2004-10-01

The recently introduced generalized parton distributions have emerged as a universal tool to describe hadrons in terms of quark and gluonic degrees of freedom. They combine the features of form factors, parton densities and distribution amplitudes - the functions used for a long time in studies of hadronic structure. Generalized parton distributions are analogous to the phase-space Wigner quasi-probability function of non-relativistic quantum mechanics which encodes full information on a quantum-mechanical system. We give an extensive review of main achievements in the development of this formalism. We discuss physical interpretation and basic properties of generalized parton distributions, their modeling andmore » QCD evolution in the leading and next-to-leading orders. We describe how these functions enter a wide class of exclusive reactions, such as electro- and photo-production of photons, lepton pairs, or mesons.« less

Scalability of a Low-Cost Multi-Teraflop Linux Cluster for High-End Classical Atomistic and Quantum Mechanical Simulations

NASA Technical Reports Server (NTRS)

Kikuchi, Hideaki; Kalia, Rajiv K.; Nakano, Aiichiro; Vashishta, Priya; Shimojo, Fuyuki; Saini, Subhash

2003-01-01

Scalability of a low-cost, Intel Xeon-based, multi-Teraflop Linux cluster is tested for two high-end scientific applications: Classical atomistic simulation based on the molecular dynamics method and quantum mechanical calculation based on the density functional theory. These scalable parallel applications use space-time multiresolution algorithms and feature computational-space decomposition, wavelet-based adaptive load balancing, and spacefilling-curve-based data compression for scalable I/O. Comparative performance tests are performed on a 1,024-processor Linux cluster and a conventional higher-end parallel supercomputer, 1,184-processor IBM SP4. The results show that the performance of the Linux cluster is comparable to that of the SP4. We also study various effects, such as the sharing of memory and L2 cache among processors, on the performance.

Quantum electronic stress: density-functional-theory formulation and physical manifestation.

PubMed

Hu, Hao; Liu, Miao; Wang, Z F; Zhu, Junyi; Wu, Dangxin; Ding, Hepeng; Liu, Zheng; Liu, Feng

2012-08-03

The concept of quantum electronic stress (QES) is introduced and formulated within density functional theory to elucidate extrinsic electronic effects on the stress state of solids and thin films in the absence of lattice strain. A formal expression of QES (σ(QE)) is derived in relation to deformation potential of electronic states (Ξ) and variation of electron density (Δn), σ(QE) = ΞΔn as a quantum analog of classical Hooke's law. Two distinct QES manifestations are demonstrated quantitatively by density functional theory calculations: (1) in the form of bulk stress induced by charge carriers and (2) in the form of surface stress induced by quantum confinement. Implications of QES in some physical phenomena are discussed to underlie its importance.

Vapor-liquid phase equilibria of water modelled by a Kim-Gordon potential

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

Maerzke, K A; McGrath, M J; Kuo, I W

2009-03-16

Gibbs ensemble Monte Carlo simulations were carried out to investigate the properties of a frozen-electron-density (or Kim-Gordon, KG) model of water along the vapor-liquid coexistence curve. Because of its theoretical basis, such a KG model provides for seamless coupling to Kohn-Sham density functional theory for use in mixed quantum mechanics/molecular mechanics (QM/MM) implementations. The Gibbs ensemble simulations indicate rather limited transferability of such a simple KG model to other state points. Specifically, a KG model that was parameterized by Barker and Sprik to the properties of liquid water at 300 K, yields saturated vapor pressures and a critical temperature thatmore » are significantly under- and over-estimated, respectively.« less

Superradiant Decay of Cyclotron Resonance of Two-Dimensional Electron Gases

NASA Astrophysics Data System (ADS)

Zhang, Qi; Arikawa, Takashi; Kato, Eiji; Reno, John L.; Pan, Wei; Watson, John D.; Manfra, Michael J.; Zudov, Michael A.; Tokman, Mikhail; Erukhimova, Maria; Belyanin, Alexey; Kono, Junichiro

2014-07-01

We report on the observation of collective radiative decay, or superradiance, of cyclotron resonance (CR) in high-mobility two-dimensional electron gases in GaAs quantum wells using time-domain terahertz magnetospectroscopy. The decay rate of coherent CR oscillations increases linearly with the electron density in a wide range, which is a hallmark of superradiant damping. Our fully quantum mechanical theory provides a universal formula for the decay rate, which reproduces our experimental data without any adjustable parameter. These results firmly establish the many-body nature of CR decoherence in this system, despite the fact that the CR frequency is immune to electron-electron interactions due to Kohn's theorem.

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

NASA Astrophysics Data System (ADS)

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

2017-09-01

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

Irregular oscillatory patterns in the early-time region of coherent phonon generation in silicon

NASA Astrophysics Data System (ADS)

Watanabe, Yohei; Hino, Ken-ichi; Hase, Muneaki; Maeshima, Nobuya

2017-09-01

Coherent phonon (CP) generation in an undoped Si crystal is theoretically investigated to shed light on unexplored quantum-mechanical effects in the early-time region immediately after the irradiation of ultrashort laser pulses. We examine time signals attributed to an induced charge density of an ionic core, placing the focus on the effects of the Rabi frequency Ω0 c v on the signals; this frequency corresponds to the peak electric-field of the pulse. It is found that at specific Ω0 c v's, where the energy of plasmon caused by photoexcited carriers coincides with the longitudinal-optical phonon energy, the energetically resonant interaction between these two modes leads to striking anticrossings, revealing irregular oscillations with anomalously enhanced amplitudes in the observed time signals. Also, the oscillatory pattern is subject to the Rabi flopping of the excited carrier density that is controlled by Ω0 c v. These findings show that the early-time region is enriched with quantum-mechanical effects inherent in the CP generation, though experimental signals are more or less masked by the so-called coherent artifact due to nonlinear optical effects.

Generalized Reduction Formula for Discrete Wigner Functions of Multiqubit Systems

NASA Astrophysics Data System (ADS)

Srinivasan, K.; Raghavan, G.

2018-03-01

Density matrices and Discrete Wigner Functions are equally valid representations of multiqubit quantum states. For density matrices, the partial trace operation is used to obtain the quantum state of subsystems, but an analogous prescription is not available for discrete Wigner Functions. Further, the discrete Wigner function corresponding to a density matrix is not unique but depends on the choice of the quantum net used for its reconstruction. In the present work, we derive a reduction formula for discrete Wigner functions of a general multiqubit state which works for arbitrary quantum nets. These results would be useful for the analysis and classification of entangled states and the study of decoherence purely in a discrete phase space setting and also in applications to quantum computing.

Investigation of non-stationary self-focusing of intense laser pulse in cold quantum plasma using ramp density profile

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

Habibi, M.; Ghamari, F.

2012-11-15

The authors have investigated the non-stationary self-focusing of Gaussian laser pulse in cold quantum plasma. In case of high dense plasma, the nonlinearity in the dielectric constant is mainly due to relativistic high intense interactions and quantum effects. In this paper, we have introduced a ramp density profile for plasma and presented graphically the behavior of spot size oscillations of pulse at rear and front portions of the pulse. It is observed that the ramp density profile and quantum effects play a vital role in stronger and better focusing at the rear of the pulse than at the front inmore » cold quantum plasmas.« less

Systematic and Automated Development of Quantum Mechanically Derived Force Fields: The Challenging Case of Halogenated Hydrocarbons.

PubMed

Prampolini, Giacomo; Campetella, Marco; De Mitri, Nicola; Livotto, Paolo Roberto; Cacelli, Ivo

2016-11-08

A robust and automated protocol for the derivation of sound force field parameters, suitable for condensed-phase classical simulations, is here tested and validated on several halogenated hydrocarbons, a class of compounds for which standard force fields have often been reported to deliver rather inaccurate performances. The major strength of the proposed protocol is that all of the parameters are derived only from first principles because all of the information required is retrieved from quantum mechanical data, purposely computed for the investigated molecule. This a priori parametrization is carried out separately for the intra- and intermolecular contributions to the force fields, respectively exploiting the Joyce and Picky programs, previously developed in our group. To avoid high computational costs, all quantum mechanical calculations were performed exploiting the density functional theory. Because the choice of the functional is known to be crucial for the description of the intermolecular interactions, a specific procedure is proposed, which allows for a reliable benchmark of different functionals against higher-level data. The intramolecular and intermolecular contribution are eventually joined together, and the resulting quantum mechanically derived force field is thereafter employed in lengthy molecular dynamics simulations to compute several thermodynamic properties that characterize the resulting bulk phase. The accuracy of the proposed parametrization protocol is finally validated by comparing the computed macroscopic observables with the available experimental counterparts. It is found that, on average, the proposed approach is capable of yielding a consistent description of the investigated set, often outperforming the literature standard force fields, or at least delivering results of similar accuracy.

Recent developments of the quantum chemical cluster approach for modeling enzyme reactions.

PubMed

Siegbahn, Per E M; Himo, Fahmi

2009-06-01

The quantum chemical cluster approach for modeling enzyme reactions is reviewed. Recent applications have used cluster models much larger than before which have given new modeling insights. One important and rather surprising feature is the fast convergence with cluster size of the energetics of the reactions. Even for reactions with significant charge separation it has in some cases been possible to obtain full convergence in the sense that dielectric cavity effects from outside the cluster do not contribute to any significant extent. Direct comparisons between quantum mechanics (QM)-only and QM/molecular mechanics (MM) calculations for quite large clusters in a case where the results differ significantly have shown that care has to be taken when using the QM/MM approach where there is strong charge polarization. Insights from the methods used, generally hybrid density functional methods, have also led to possibilities to give reasonable error limits for the results. Examples are finally given from the most extensive study using the cluster model, the one of oxygen formation at the oxygen-evolving complex in photosystem II.

Epoxide reduction with hydrazine on graphene: a first principles study.

PubMed

Kim, Min Chan; Hwang, Gyeong S; Ruoff, Rodney S

2009-08-14

Mechanisms for epoxide reduction with hydrazine on a single-layer graphene sheet are examined using quantum mechanical calculations within the framework of gradient-corrected spin-polarized density-functional theory. We find that the reduction reaction is mainly governed by epoxide ring opening which is initiated by H transfer from hydrazine or its derivatives. In addition, our calculations suggest that the epoxide reduction by hydrazine may predominantly follow a direct Eley-Rideal mechanism rather than a Langmuir-Hinshelwood mechanism. We also discuss the generation of various hydrazine derivatives during the reduction of graphene oxide with hydrazine and their potential contribution to lowering the barrier height of epoxide ring opening.

Arbitrary amplitude nucleus-acoustic solitons in multi-ion quantum plasmas with relativistically degenerate electrons

NASA Astrophysics Data System (ADS)

Sultana, S.; Schlickeiser, R.

2018-02-01

A three component degenerate relativistic quantum plasma (consisting of relativistically degenerate electrons, nondegenerate inertial light nuclei, and stationary heavy nuclei) is considered to model the linear wave and also the electrostatic solitary waves in the light nuclei-scale length. A well-known normal mode analysis is employed to investigate the linear wave properties. A mechanical-motion analog (Sagdeev-type) pseudo-potential approach, which reveals the existence of large amplitude solitary excitations, is adopted to study the nonlinear wave properties. Only the positive potential solitary excitations are found to exist in the plasma medium under consideration. The basic properties of the arbitrary amplitude electrostatic acoustic modes in the light nuclei-scale length and their existence domain in terms of soliton speed (Mach number) are examined. The modifications of solitary wave characteristics and their existence domain with the variation of different key plasma configuration parameters (e.g., electrons degeneracy parameter, inertial light nuclei number density, and degenerate electron number density) are also analyzed. Our results, which may be helpful to explain the basic features of the nonlinear wave propagation in multi-component degenerate quantum plasmas, in connection with astrophysical compact objects (e.g., white dwarfs) are briefly discussed.

Floquet Engineering in Quantum Chains

NASA Astrophysics Data System (ADS)

Kennes, D. M.; de la Torre, A.; Ron, A.; Hsieh, D.; Millis, A. J.

2018-03-01

We consider a one-dimensional interacting spinless fermion model, which displays the well-known Luttinger liquid (LL) to charge density wave (CDW) transition as a function of the ratio between the strength of the interaction U and the hopping J . We subject this system to a spatially uniform drive which is ramped up over a finite time interval and becomes time periodic in the long-time limit. We show that by using a density matrix renormalization group approach formulated for infinite system sizes, we can access the large-time limit even when the drive induces finite heating. When both the initial and long-time states are in the gapless (LL) phase, the final state has power-law correlations for all ramp speeds. However, when the initial and final state are gapped (CDW phase), we find a pseudothermal state with an effective temperature that depends on the ramp rate, both for the Magnus regime in which the drive frequency is very large compared to other scales in the system and in the opposite limit where the drive frequency is less than the gap. Remarkably, quantum defects (instantons) appear when the drive tunes the system through the quantum critical point, in a realization of the Kibble-Zurek mechanism.

Definition of molecular structure: by choice or by appeal to observation?

PubMed

Bader, Richard F W

2010-07-22

There are two schools of thought in chemistry: one derived from the valence bond and molecular orbital models of bonding, the other appealing directly to the measurable electron density and the quantum mechanical theorems that determine its behavior, an approach embodied in the quantum theory of atoms in molecules, QTAIM. No one questions the validity of the former approach, and indeed molecular orbital models and QTAIM play complementary roles, the models finding expression in the principles of physics. However, some orbital proponents step beyond the models to impose their personal stamp on their use in interpretive chemistry, by denying the possible existence of a physical basis for the concepts of chemistry. This places them at odds with QTAIM, whose very existence stems from the discovery in the observable topology of the electron density, the definitions of atoms, of the bonding between atoms and hence of molecular structure. Relating these concepts to the electron density provides the necessary link for their ultimate quantum definition. This paper explores in depth the possible causes of the difficulties some have in accepting the quantum basis of structure beginning with the arguments associated with the acceptance of a "bond path" as a criterion for bonding. This identification is based on the finding that all classical structures may be mapped onto molecular graphs consisting of bond paths linking neighboring atoms, a mapping that has no known exceptions and one that is further bolstered by the finding that there are no examples of "missing bond paths". Difficulties arise when the quantum concept is applied to systems that are not amenable to the classical models of bonding. Thus one is faced with the recurring dilemma of science, of having to escape the constraints of a model that requires a change in the existing paradigm, a process that has been in operation since the discovery of new and novel structures necessitated the extension of the Lewis model and the octet rule. The paper reviews all facets of bonding beginning with the work of Pauling and Slater in their accounting for crystal structures, taking note of Pauling's advocating possible bonding between large anions. Many examples of nonbonded or van der Waals interactions are considered from both points of view. The final section deals with the consequences of the realization that bonded quantum atoms that share an interatomic surface do not "overlap". The time has come for entering students of chemistry to be taught that the electron density can be seen, touched, and measured and that the chemical structures they learn are in fact the tracings of "bonds" onto lines of maximum density that link bonded nuclei. Matter, as we perceive it, is bound by the electrostatic force of attraction between the nuclei and the electron density.

Imaging the He2 quantum halo state using a free electron laser

NASA Astrophysics Data System (ADS)

Zeller, Stefan; Kunitski, Maksim; Voigtsberger, Jörg; Kalinin, Anton; Schottelius, Alexander; Schober, Carl; Waitz, Markus; Sann, Hendrik; Hartung, Alexander; Bauer, Tobias; Pitzer, Martin; Trinter, Florian; Goihl, Christoph; Janke, Christian; Richter, Martin; Kastirke, Gregor; Weller, Miriam; Czasch, Achim; Kitzler, Markus; Braune, Markus; Grisenti, Robert E.; Schöllkopf, Wieland; Schmidt, Lothar Ph. H.; Schöffler, Markus S.; Williams, Joshua B.; Jahnke, Till; Dörner, Reinhard

2016-12-01

Quantum tunneling is a ubiquitous phenomenon in nature and crucial for many technological applications. It allows quantum particles to reach regions in space which are energetically not accessible according to classical mechanics. In this “tunneling region,” the particle density is known to decay exponentially. This behavior is universal across all energy scales from nuclear physics to chemistry and solid state systems. Although typically only a small fraction of a particle wavefunction extends into the tunneling region, we present here an extreme quantum system: a gigantic molecule consisting of two helium atoms, with an 80% probability that its two nuclei will be found in this classical forbidden region. This circumstance allows us to directly image the exponentially decaying density of a tunneling particle, which we achieved for over two orders of magnitude. Imaging a tunneling particle shows one of the few features of our world that is truly universal: the probability to find one of the constituents of bound matter far away is never zero but decreases exponentially. The results were obtained by Coulomb explosion imaging using a free electron laser and furthermore yielded He2’s binding energy of 151.9±13.3151.9±13.3 neV, which is in agreement with most recent calculations.

Quantum dynamics in continuum for proton transport II: Variational solvent-solute interface.

PubMed

Chen, Duan; Chen, Zhan; Wei, Guo-Wei

2012-01-01

Proton transport plays an important role in biological energy transduction and sensory systems. Therefore, it has attracted much attention in biological science and biomedical engineering in the past few decades. The present work proposes a multiscale/multiphysics model for the understanding of the molecular mechanism of proton transport in transmembrane proteins involving continuum, atomic, and quantum descriptions, assisted with the evolution, formation, and visualization of membrane channel surfaces. We describe proton dynamics quantum mechanically via a new density functional theory based on the Boltzmann statistics, while implicitly model numerous solvent molecules as a dielectric continuum to reduce the number of degrees of freedom. The density of all other ions in the solvent is assumed to obey the Boltzmann distribution in a dynamic manner. The impact of protein molecular structure and its charge polarization on the proton transport is considered explicitly at the atomic scale. A variational solute-solvent interface is designed to separate the explicit molecule and implicit solvent regions. We formulate a total free-energy functional to put proton kinetic and potential energies, the free energy of all other ions, and the polar and nonpolar energies of the whole system on an equal footing. The variational principle is employed to derive coupled governing equations for the proton transport system. Generalized Laplace-Beltrami equation, generalized Poisson-Boltzmann equation, and generalized Kohn-Sham equation are obtained from the present variational framework. The variational solvent-solute interface is generated and visualized to facilitate the multiscale discrete/continuum/quantum descriptions. Theoretical formulations for the proton density and conductance are constructed based on fundamental laws of physics. A number of mathematical algorithms, including the Dirichlet-to-Neumann mapping, matched interface and boundary method, Gummel iteration, and Krylov space techniques are utilized to implement the proposed model in a computationally efficient manner. The gramicidin A channel is used to validate the performance of the proposed proton transport model and demonstrate the efficiency of the proposed mathematical algorithms. The proton channel conductances are studied over a number of applied voltages and reference concentrations. A comparison with experimental data verifies the present model predictions and confirms the proposed model. Copyright © 2011 John Wiley & Sons, Ltd.

Transitioning NWChem to the Next Generation of Manycore Machines

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

Bylaska, Eric J.; Apra, E; Kowalski, Karol

The NorthWest chemistry (NWChem) modeling software is a popular molecular chemistry simulation software that was designed from the start to work on massively parallel processing supercomputers [1-3]. It contains an umbrella of modules that today includes self-consistent eld (SCF), second order Møller-Plesset perturbation theory (MP2), coupled cluster (CC), multiconguration self-consistent eld (MCSCF), selected conguration interaction (CI), tensor contraction engine (TCE) many body methods, density functional theory (DFT), time-dependent density functional theory (TDDFT), real-time time-dependent density functional theory, pseudopotential plane-wave density functional theory (PSPW), band structure (BAND), ab initio molecular dynamics (AIMD), Car-Parrinello molecular dynamics (MD), classical MD, hybrid quantum mechanicsmore » molecular mechanics (QM/MM), hybrid ab initio molecular dynamics molecular mechanics (AIMD/MM), gauge independent atomic orbital nuclear magnetic resonance (GIAO NMR), conductor like screening solvation model (COSMO), conductor-like screening solvation model based on density (COSMO-SMD), and reference interaction site model (RISM) solvation models, free energy simulations, reaction path optimization, parallel in time, among other capabilities [4]. Moreover, new capabilities continue to be added with each new release.« less

Cryogenic on-chip multiplexer for the study of quantum transport in 256 split-gate devices

NASA Astrophysics Data System (ADS)

Al-Taie, H.; Smith, L. W.; Xu, B.; See, P.; Griffiths, J. P.; Beere, H. E.; Jones, G. A. C.; Ritchie, D. A.; Kelly, M. J.; Smith, C. G.

2013-06-01

We present a multiplexing scheme for the measurement of large numbers of mesoscopic devices in cryogenic systems. The multiplexer is used to contact an array of 256 split gates on a GaAs/AlGaAs heterostructure, in which each split gate can be measured individually. The low-temperature conductance of split-gate devices is governed by quantum mechanics, leading to the appearance of conductance plateaux at intervals of 2e2/h. A fabrication-limited yield of 94% is achieved for the array, and a "quantum yield" is also defined, to account for disorder affecting the quantum behaviour of the devices. The quantum yield rose from 55% to 86% after illuminating the sample, explained by the corresponding increase in carrier density and mobility of the two-dimensional electron gas. The multiplexer is a scalable architecture, and can be extended to other forms of mesoscopic devices. It overcomes previous limits on the number of devices that can be fabricated on a single chip due to the number of electrical contacts available, without the need to alter existing experimental set ups.

Quantum dynamical simulation of the scattering of Ar from a frozen LiF(100) surface based on a first principles interaction potential

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

Azuri, Asaf; Pollak, Eli, E-mail: eli.pollak@weizmann.ac.il

2015-07-07

In-plane two and three dimensional diffraction patterns are computed for the vertical scattering of an Ar atom from a frozen LiF(100) surface. Suitable collimation of the incoming wavepacket serves to reveal the quantum mechanical diffraction. The interaction potential is based on a fit to an ab initio potential calculated using density functional theory with dispersion corrections. Due to the potential coupling found between the two horizontal surface directions, there are noticeable differences between the quantum angular distributions computed for two and three dimensional scattering. The quantum results are compared to analogous classical Wigner computations on the same surface and withmore » the same conditions. The classical dynamics largely provides the envelope for the quantum diffractive scattering. The classical results also show that the corrugation along the [110] direction of the surface is smaller than along the [100] direction, in qualitative agreement with experimental observations of unimodal and bimodal scattering for the [110] and [100] directions, respectively.« less

The control of electron quantum trajectories on the high-order harmonic generation of CO and N2 molecules in the presence of a low frequency field.

PubMed

Koushki, A M; Sadighi-Bonabi, R; Mohsen-Nia, M; Irani, E

2018-04-14

In the present work, an efficient method is theoretically investigated for extending high-order harmonics and ultrashort attosecond pulse generation in N 2 and CO molecules by using the time-dependent density functional theory approach. Our results show that by utilizing chirped laser field in the presence of a low frequency field, not only is the harmonic cutoff extended remarkably but also the single short quantum trajectory is selected to contribute to the harmonic spectra. When a low frequency field is added to the two-color chirped laser field, the long quantum trajectories are suppressed and only the short quantum trajectories contribute to the higher harmonic emission mechanism. As a result, the spectral modulation is significantly decreased and an intense ultrashort pulse can be generated from the supercontinuum region of high harmonics. With such a scheme, the isolated ultrashort attosecond pulses can be generated in length, velocity, and acceleration gauges. Furthermore, these results are explained by using the classical and quantum time-frequency analyses.

The control of electron quantum trajectories on the high-order harmonic generation of CO and N2 molecules in the presence of a low frequency field

NASA Astrophysics Data System (ADS)

Koushki, A. M.; Sadighi-Bonabi, R.; Mohsen-Nia, M.; Irani, E.

2018-04-01

In the present work, an efficient method is theoretically investigated for extending high-order harmonics and ultrashort attosecond pulse generation in N2 and CO molecules by using the time-dependent density functional theory approach. Our results show that by utilizing chirped laser field in the presence of a low frequency field, not only is the harmonic cutoff extended remarkably but also the single short quantum trajectory is selected to contribute to the harmonic spectra. When a low frequency field is added to the two-color chirped laser field, the long quantum trajectories are suppressed and only the short quantum trajectories contribute to the higher harmonic emission mechanism. As a result, the spectral modulation is significantly decreased and an intense ultrashort pulse can be generated from the supercontinuum region of high harmonics. With such a scheme, the isolated ultrashort attosecond pulses can be generated in length, velocity, and acceleration gauges. Furthermore, these results are explained by using the classical and quantum time-frequency analyses.

X-ray phase-contrast imaging: the quantum perspective

NASA Astrophysics Data System (ADS)

Slowik, J. M.; Santra, R.

2013-08-01

Time-resolved phase-contrast imaging using ultrafast x-ray sources is an emerging method to investigate ultrafast dynamical processes in matter. Schemes to generate attosecond x-ray pulses have been proposed, bringing electronic timescales into reach and emphasizing the demand for a quantum description. In this paper, we present a method to describe propagation-based x-ray phase-contrast imaging in nonrelativistic quantum electrodynamics. We explain why the standard scattering treatment via Fermi’s golden rule cannot be applied. Instead, the quantum electrodynamical treatment of phase-contrast imaging must be based on a different approach. It turns out that it is essential to select a suitable observable. Here, we choose the quantum-mechanical Poynting operator. We determine the expectation value of our observable and demonstrate that the leading order term describes phase-contrast imaging. It recovers the classical expression of phase-contrast imaging. Thus, it makes the instantaneous electron density of non-stationary electronic states accessible to time-resolved imaging. Interestingly, inelastic (Compton) scattering does automatically not contribute in leading order, explaining the success of the semiclassical description.

Quantum transport modeling of magnetic focusing in graphene p-n junctions

NASA Astrophysics Data System (ADS)

Lagasse, Samuel; Lee, Ji Ung

We demonstrate a new model for studying transverse magnetic focusing experiments in graphene p-n junctions, using quantum transport methods. By including a combination of dephasing edge contacts and Landauer-Büttiker multi-terminal analysis, we observe an exceptional degree of agreement with recent experimental data from Chen et al, without fitting parameters. Our model captures both the resonance and off-resonance non-local resistances from experiment. Our calculated quantum transmission functions indicate the origin of the sign of the measured resistance. Spatially resolved flow maps of local particle current density are used to explain our results and rapidly convey the mechanisms of device operation. Mode-by-mode analysis of transport shows the complex interplay between semi-classical skipping orbits and quantum effects. Quantum interference, p-n filtering, and edge scattering are clearly seen. Additionally, we are able to explain subtle features from experiment, such as the p-p- to p-p+ transition and the second p-n focusing resonance. The authors acknolwedge financial support provided by the U.S. Naval Research Laboratory (Grant Number: N00173-14-1-G017).

Photovoltaic and thermophotovoltaic devices with quantum barriers

DOEpatents

Wernsman, Bernard R [Jefferson Hills, PA

2007-04-10

A photovoltaic or thermophotovoltaic device includes a diode formed by p-type material and n-type material joined at a p-n junction and including a depletion region adjacent to said p-n junction, and a quantum barrier disposed near or in the depletion region of the p-n junction so as to decrease device reverse saturation current density while maintaining device short circuit current density. In one embodiment, the quantum barrier is disposed on the n-type material side of the p-n junction and decreases the reverse saturation current density due to electrons while in another, the barrier is disposed on the p-type material side of the p-n junction and decreases the reverse saturation current density due to holes. In another embodiment, both types of quantum barriers are used.

Dislocation-driven growth of two-dimensional lateral quantum-well superlattices

PubMed Central

Chen, Jianyi; Li, Dongdong

2018-01-01

The advent of two-dimensional (2D) materials has led to extensive studies of heterostructures for novel applications. 2D lateral multiheterojunctions and superlattices have been recently demonstrated, but the available growth methods can only produce features with widths in the micrometer or, at best, 100-nm scale and usually result in rough and defective interfaces with extensive chemical intermixing. Widths smaller than 5 nm, which are needed for quantum confinement effects and quantum-well applications, have not been achieved. We demonstrate the growth of sub–2-nm quantum-well arrays in semiconductor monolayers, driven by the climb of misfit dislocations in a lattice-mismatched sulfide/selenide heterointerface. Density functional theory calculations provide an atom-by-atom description of the growth mechanism. The calculated energy bands reveal type II alignment suitable for quantum wells, suggesting that the structure could, in principle, be turned into a “conduit” of conductive nanoribbons for interconnects in future 2D integrated circuits via n-type modulation doping. This misfit dislocation–driven growth can be applied to different combinations of 2D monolayers with lattice mismatch, paving the way to a wide range of 2D quantum-well superlattices with controllable band alignment and nanoscale width. PMID:29740600

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

PubMed

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

2018-03-31

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

A Practical Quantum Mechanics Molecular Mechanics Method for the Dynamical Study of Reactions in Biomolecules.

PubMed

Mendieta-Moreno, Jesús I; Marcos-Alcalde, Iñigo; Trabada, Daniel G; Gómez-Puertas, Paulino; Ortega, José; Mendieta, Jesús

2015-01-01

Quantum mechanics/molecular mechanics (QM/MM) methods are excellent tools for the modeling of biomolecular reactions. Recently, we have implemented a new QM/MM method (Fireball/Amber), which combines an efficient density functional theory method (Fireball) and a well-recognized molecular dynamics package (Amber), offering an excellent balance between accuracy and sampling capabilities. Here, we present a detailed explanation of the Fireball method and Fireball/Amber implementation. We also discuss how this tool can be used to analyze reactions in biomolecules using steered molecular dynamics simulations. The potential of this approach is shown by the analysis of a reaction catalyzed by the enzyme triose-phosphate isomerase (TIM). The conformational space and energetic landscape for this reaction are analyzed without a priori assumptions about the protonation states of the different residues during the reaction. The results offer a detailed description of the reaction and reveal some new features of the catalytic mechanism. In particular, we find a new reaction mechanism that is characterized by the intramolecular proton transfer from O1 to O2 and the simultaneous proton transfer from Glu 165 to C2. Copyright © 2015 Elsevier Inc. All rights reserved.

Experimental and theoretical investigation of the elastic moduli of silicate glasses and crystals

NASA Astrophysics Data System (ADS)

Philipps, Katharina; Stoffel, Ralf Peter; Dronskowski, Richard; Conradt, Reinhard

2017-02-01

A combined quantum-mechanical and thermodynamic approach to the mechanical properties of multicomponent silicate glasses is presented. Quantum chemical calculations based on density-functional theory (DFT) on various silicate systems were performed to explore the crystalline polymorphs existing for a given chemical composition. These calculations reproduced the properties of known polymorphs even in systems with extensive polymorphism, like MgSiO3. Properties resting on the atomic and electronic structure, i.e., molar volumes (densities) and bulk moduli were predicted correctly. The theoretical data (molar equilibrium volumes, bulk moduli) were then used to complement the available experimental data. In a phenomenological evaluation, experimental data of bulk moduli, a macroscopic property resting on phononic structure, were found to linearly scale with the ratios of atomic space demand to actual molar volume in a universal way. Silicates ranging from high-pressure polymorphs to glasses were represented by a single master line. This suggests that above the Debye limit (in practice: above room temperature), the elastic waves probe the short range order coordination polyhedra and their next-neighbor linkage only, while the presence or absence of an extended translational symmetry is irrelevant. As a result, glasses can be treated - with respect to the properties investigated - as commensurable members of polymorphic series. Binary glasses fit the very same line as their one-component end-members, again both in the crystalline and glassy state. Finally, it is shown that the macroscopic properties of multicomponent glasses also are linear superpositions of the properties of their constitutional phases (as determined from phase diagrams or by thermochemical calculations) taken in their respective glassy states. This is verified experimentally for heat capacities and Young’s moduli of industrial glass compositions. It can be concluded, that the combined quantum mechanical and thermochemical approach is a truly quantitative approach for the design of glasses with desired mechanical properties, e.g., for the development of high-modulus glasses.

Investigation of germanium quantum-well light sources.

PubMed

Fei, Edward T; Chen, Xiaochi; Zang, Kai; Huo, Yijie; Shambat, Gary; Miller, Gerald; Liu, Xi; Dutt, Raj; Kamins, Theodore I; Vuckovic, Jelena; Harris, James S

2015-08-24

In this paper, we report a broad investigation of the optical properties of germanium (Ge) quantum-well devices. Our simulations show a significant increase of carrier density in the Ge quantum wells. Photoluminescence (PL) measurements show the enhanced direct-bandgap radiative recombination rates due to the carrier density increase in the Ge quantum wells. Electroluminescence (EL) measurements show the temperature-dependent properties of our Ge quantum-well devices, which are in good agreement with our theoretical models. We also demonstrate the PL measurements of Ge quantum-well microdisks using tapered-fiber collection method and quantify the optical loss of the Ge quantum-well structure from the measured PL spectra for the first time.

The Shannon entropy information for mixed Manning Rosen potential in D-dimensional Schrodinger equation

NASA Astrophysics Data System (ADS)

Suparmi, A.; Cari, C.; Nur Pratiwi, Beta; Arya Nugraha, Dewanta

2017-01-01

D dimensional Schrodinger equation for the mixed Manning Rosen potential was investigated using supersymmetric quantum mechanics. We obtained the energy eigenvalues from radial part solution and wavefunctions in radial and angular parts solution. From the lowest radial wavefunctions, we evaluated the Shannon entropy information using Matlab software. Based on the entropy densities demonstrated graphically, we obtained that the wave of position information entropy density moves right when the value of potential parameter q increases, while its wave moves left with the increase of parameter α. The wave of momentum information entropy densities were expressed in graphs. We observe that its amplitude increase with increasing parameter q and α

Density functional theory for field emission from carbon nano-structures.

PubMed

Li, Zhibing

2015-12-01

Electron field emission is understood as a quantum mechanical many-body problem in which an electronic quasi-particle of the emitter is converted into an electron in vacuum. Fundamental concepts of field emission, such as the field enhancement factor, work-function, edge barrier and emission current density, will be investigated, using carbon nanotubes and graphene as examples. A multi-scale algorithm basing on density functional theory is introduced. We will argue that such a first principle approach is necessary and appropriate for field emission of nano-structures, not only for a more accurate quantitative description, but, more importantly, for deeper insight into field emission. Copyright © 2015 The Author. Published by Elsevier B.V. All rights reserved.

Noise, gain, and capture probability of p-type InAs-GaAs quantum-dot and quantum dot-in-well infrared photodetectors

NASA Astrophysics Data System (ADS)

Wolde, Seyoum; Lao, Yan-Feng; Unil Perera, A. G.; Zhang, Y. H.; Wang, T. M.; Kim, J. O.; Schuler-Sandy, Ted; Tian, Zhao-Bing; Krishna, S.

2017-06-01

We report experimental results showing how the noise in a Quantum-Dot Infrared photodetector (QDIP) and Quantum Dot-in-a-well (DWELL) varies with the electric field and temperature. At lower temperatures (below ˜100 K), the noise current of both types of detectors is dominated by generation-recombination (G-R) noise which is consistent with a mechanism of fluctuations driven by the electric field and thermal noise. The noise gain, capture probability, and carrier life time for bound-to-continuum or quasi-bound transitions in DWELL and QDIP structures are discussed. The capture probability of DWELL is found to be more than two times higher than the corresponding QDIP. Based on the analysis, structural parameters such as the numbers of active layers, the surface density of QDs, and the carrier capture or relaxation rate, type of material, and electric field are some of the optimization parameters identified to improve the gain of devices.

Quantum chemical methods for the investigation of photoinitiated processes in biological systems: theory and applications.

PubMed

Dreuw, Andreas

2006-11-13

With the advent of modern computers and advances in the development of efficient quantum chemical computer codes, the meaningful computation of large molecular systems at a quantum mechanical level became feasible. Recent experimental effort to understand photoinitiated processes in biological systems, for instance photosynthesis or vision, at a molecular level also triggered theoretical investigations in this field. In this Minireview, standard quantum chemical methods are presented that are applicable and recently used for the calculation of excited states of photoinitiated processes in biological molecular systems. These methods comprise configuration interaction singles, the complete active space self-consistent field method, and time-dependent density functional theory and its variants. Semiempirical approaches are also covered. Their basic theoretical concepts and mathematical equations are briefly outlined, and their properties and limitations are discussed. Recent successful applications of the methods to photoinitiated processes in biological systems are described and theoretical tools for the analysis of excited states are presented.

Quantum theory of spontaneous and stimulated emission of surface plasmons

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

Archambault, Alexandre; Marquier, Francois; Greffet, Jean-Jacques

2010-07-15

We introduce a quantization scheme that can be applied to surface waves propagating along a plane interface. An important result is the derivation of the energy of the surface wave for dispersive nonlossy media without invoking any specific model for the dielectric constant. Working in Coulomb's gauge, we use a modal representation of the fields. Each mode can be associated with a quantum harmonic oscillator. We have applied the formalism to derive quantum mechanically the spontaneous emission rate of surface plasmon by a two-level system. The result is in very good agreement with Green's tensor approach in the nonlossy case.more » Green's approach allows also to account for losses, so that the limitations of a quantum approach of surface plasmons are clearly defined. Finally, the issue of stimulated versus spontaneous emission has been addressed. Because of the increasing density of states near the asymptote of the dispersion relation, it is quantitatively shown that the stimulated emission probability is too small to obtain gain in this frequency region.« less

Accuracy of Protein Embedding Potentials: An Analysis in Terms of Electrostatic Potentials.

PubMed

Olsen, Jógvan Magnus Haugaard; List, Nanna Holmgaard; Kristensen, Kasper; Kongsted, Jacob

2015-04-14

Quantum-mechanical embedding methods have in recent years gained significant interest and may now be applied to predict a wide range of molecular properties calculated at different levels of theory. To reach a high level of accuracy in embedding methods, both the electronic structure model of the active region and the embedding potential need to be of sufficiently high quality. In fact, failures in quantum mechanics/molecular mechanics (QM/MM)-based embedding methods have often been associated with the QM/MM methodology itself; however, in many cases the reason for such failures is due to the use of an inaccurate embedding potential. In this paper, we investigate in detail the quality of the electronic component of embedding potentials designed for calculations on protein biostructures. We show that very accurate explicitly polarizable embedding potentials may be efficiently designed using fragmentation strategies combined with single-fragment ab initio calculations. In fact, due to the self-interaction error in Kohn-Sham density functional theory (KS-DFT), use of large full-structure quantum-mechanical calculations based on conventional (hybrid) functionals leads to less accurate embedding potentials than fragment-based approaches. We also find that standard protein force fields yield poor embedding potentials, and it is therefore not advisable to use such force fields in general QM/MM-type calculations of molecular properties other than energies and structures.

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 non-Markovian quantum dynamics are also briefly discussed.

Undergraduate quantum mechanics: lost opportunities for engaging motivated students?

NASA Astrophysics Data System (ADS)

Johansson, Anders

2018-03-01

Quantum mechanics is widely recognised as an important and difficult subject, and many studies have been published focusing on students’ conceptual difficulties. However, the sociocultural aspects of studying such an emblematic subject have not been researched to any large extent. This study explores students’ experiences of undergraduate quantum mechanics using qualitative analysis of semi-structured interview data. The results inform discussions about the teaching of quantum mechanics by adding a sociocultural dimension. Students pictured quantum mechanics as an intriguing subject that inspired them to study physics. The study environment they encountered when taking their first quantum mechanics course was however not always as inspiring as expected. Quantum mechanics instruction has commonly focused on the mathematical framework of quantum mechanics, and this kind of teaching was also what the interviewees had experienced. Two ways of handling the encounter with a traditional quantum mechanics course were identified in the interviews; either students accept the practice of studying quantum mechanics in a mathematical, exercise-centred way or they distance themselves from these practices and the subject. The students who responded by distancing themselves experienced a crisis and disappointment, where their experiences did not match the way they imagined themselves engaging with quantum mechanics. The implications of these findings are discussed in relation to efforts to reform the teaching of undergraduate quantum mechanics.

Correlations and sum rules in a half-space for a quantum two-dimensional one-component plasma

NASA Astrophysics Data System (ADS)

Jancovici, B.; Šamaj, L.

2007-05-01

This paper is the continuation of a previous one (Šamaj and Jancovici, 2007 J. Stat. Mech. P02002); for a nearly classical quantum fluid in a half-space bounded by a plain plane hard wall (no image forces), we had generalized the Wigner Kirkwood expansion of the equilibrium statistical quantities in powers of Planck's constant \\hbar . As a model system for a more detailed study, we consider the quantum two-dimensional one-component plasma: a system of charged particles of one species, interacting through the logarithmic Coulomb potential in two dimensions, in a uniformly charged background of opposite sign, such that the total charge vanishes. The corresponding classical system is exactly solvable in a variety of geometries, including the present one of a half-plane, when βe2 = 2, where β is the inverse temperature and e is the charge of a particle: all the classical n-body densities are known. In the present paper, we have calculated the expansions of the quantum density profile and truncated two-body density up to order \\hbar ^2 (instead of only to order \\hbar as in the previous paper). These expansions involve the classical n-body densities up to n = 4; thus we obtain exact expressions for these quantum expansions in this special case. For the quantum one-component plasma, two sum rules involving the truncated two-body density (and, for one of them, the density profile) have been derived, a long time ago, by using heuristic macroscopic arguments: one sum rule concerns the asymptotic form along the wall of the truncated two-body density; the other one concerns the dipole moment of the structure factor. In the two-dimensional case at βe2 = 2, we now have explicit expressions up to order \\hbar^2 for these two quantum densities; thus we can microscopically check the sum rules at this order. The checks are positive, reinforcing the idea that the sum rules are correct.

Quantum Monte Carlo Studies of Interaction-Induced Localization in Quantum Dots and Wires

NASA Astrophysics Data System (ADS)

Devrim Güçlü, A.

2009-03-01

We investigate interaction-induced localization of electrons in both quantum dots and inhomogeneous quantum wires using variational and diffusion quantum Monte Carlo methods. Quantum dots and wires are highly tunable systems that enable the study of the physics of strongly correlated electrons. With decreasing electronic density, interactions become stronger and electrons are expected to localize at their classical positions, as in Wigner crystallization in an infinite 2D system. (1) Dots: We show that the addition energy shows a clear progression from features associated with shell structure to those caused by commensurability of a Wigner crystal. This cross-over is, then, a signature of localization; it occurs near rs˜20. For higher values of rs, the configuration symmetry of the quantum dot becomes fully consistent with the classical ground state. (2) Wires: We study an inhomogeneous quasi-one-dimensional system -- a wire with two regions, one at low density and the other high. We find that strong localization occurs in the low density quantum point contact region as the gate potential is increased. The nature of the transition from high to low density depends on the density gradient -- if it is steep, a barrier develops between the two regions, causing Coulomb blockade effects. We find no evidence for ferromagnetic spin polarization for the range of parameters studied. The picture emerging here is in good agreement with the experimental measurements of tunneling between two wires. Collaborators: C. J. Umrigar (Cornell), Hong Jiang (Fritz Haber Institut), Amit Ghosal (IISER Calcutta), and H. U. Baranger (Duke).

CUGatesDensity—Quantum circuit analyser extended to density matrices

NASA Astrophysics Data System (ADS)

Loke, T.; Wang, J. B.

2013-12-01

CUGatesDensity is an extension of the original quantum circuit analyser CUGates (Loke and Wang, 2011) [7] to provide explicit support for the use of density matrices. The new package enables simulation of quantum circuits involving statistical ensemble of mixed quantum states. Such analysis is of vital importance in dealing with quantum decoherence, measurements, noise and error correction, and fault tolerant computation. Several examples involving mixed state quantum computation are presented to illustrate the use of this package. Catalogue identifier: AEPY_v1_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEPY_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.: 5368 No. of bytes in distributed program, including test data, etc.: 143994 Distribution format: tar.gz Programming language: Mathematica. Computer: Any computer installed with a copy of Mathematica 6.0 or higher. Operating system: Any system with a copy of Mathematica 6.0 or higher installed. Classification: 4.15. Nature of problem: To simulate arbitrarily complex quantum circuits comprised of single/multiple qubit and qudit quantum gates with mixed state registers. Solution method: A density matrix representation for mixed states and a state vector representation for pure states are used. The construct is based on an irreducible form of matrix decomposition, which allows a highly efficient implementation of general controlled gates with multiple conditionals. Running time: The examples provided in the notebook CUGatesDensity.nb take approximately 30 s to run on a laptop PC.

Time dependent Schrödinger equation for black hole evaporation: No information loss

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

Corda, Christian, E-mail: cordac.galilei@gmail.com

2015-02-15

In 1976 S. Hawking claimed that “Because part of the information about the state of the system is lost down the hole, the final situation is represented by a density matrix rather than a pure quantum state”. This was the starting point of the popular “black hole (BH) information paradox”. In a series of papers, together with collaborators, we naturally interpreted BH quasi-normal modes (QNMs) in terms of quantum levels discussing a model of excited BH somewhat similar to the historical semi-classical Bohr model of the structure of a hydrogen atom. Here we explicitly write down, for the same model,more » a time dependent Schrödinger equation for the system composed by Hawking radiation and BH QNMs. The physical state and the correspondent wave function are written in terms of a unitary evolution matrix instead of a density matrix. Thus, the final state results to be a pure quantum state instead of a mixed one. Hence, Hawking’s claim is falsified because BHs result to be well defined quantum mechanical systems, having ordered, discrete quantum spectra, which respect ’t Hooft’s assumption that Schrödinger equations can be used universally for all dynamics in the universe. As a consequence, information comes out in BH evaporation in terms of pure states in a unitary time dependent evolution. In Section 4 of this paper we show that the present approach permits also to solve the entanglement problem connected with the information paradox.« less

Harmonic generation in magnetized quantum plasma

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

Kumar, Punit; Singh, Abhisek Kumar; Singh, Shiv

2016-05-06

A study of second harmonic generation by propagation of a linearly polarized electromagnetic wave through homogeneous high density quantum plasma in the presence of transverse magnetic field. The nonlinear current density and dispersion relations for the fundamental and second harmonic frequencies have been obtained using the recently developed quantum hydrodynamic (QHD) model. The effect of quantum Bohm potential, Fermi pressure and the electron spin have been taken into account. The second harmonic is found to be less dispersed than the first.

Newtonian semiclassical gravity in three ontological quantum theories that solve the measurement problem: Formalisms and empirical predictions

NASA Astrophysics Data System (ADS)

Derakhshani, Maaneli

In this thesis, we consider the implications of solving the quantum measurement problem for the Newtonian description of semiclassical gravity. First we review the formalism of the Newtonian description of semiclassical gravity based on standard quantum mechanics---the Schroedinger-Newton theory---and two well-established predictions that come out of it, namely, gravitational 'cat states' and gravitationally-induced wavepacket collapse. Then we review three quantum theories with 'primitive ontologies' that are well-known known to solve the measurement problem---Schroedinger's many worlds theory, the GRW collapse theory with matter density ontology, and Nelson's stochastic mechanics. We extend the formalisms of these three quantum theories to Newtonian models of semiclassical gravity and evaluate their implications for gravitational cat states and gravitational wavepacket collapse. We find that (1) Newtonian semiclassical gravity based on Schroedinger's many worlds theory is mathematically equivalent to the Schroedinger-Newton theory and makes the same predictions; (2) Newtonian semiclassical gravity based on the GRW theory differs from Schroedinger-Newton only in the use of a stochastic collapse law, but this law allows it to suppress gravitational cat states so as not to be in contradiction with experiment, while allowing for gravitational wavepacket collapse to happen as well; (3) Newtonian semiclassical gravity based on Nelson's stochastic mechanics differs significantly from Schroedinger-Newton, and does not predict gravitational cat states nor gravitational wavepacket collapse. Considering that gravitational cat states are experimentally ruled out, but gravitational wavepacket collapse is testable in the near future, this implies that only the latter two are viable theories of Newtonian semiclassical gravity and that they can be experimentally tested against each other in future molecular interferometry experiments that are anticipated to be capable of testing the gravitational wavepacket collapse prediction.

Suppressed power saturation due to optimized optical confinement in 9xx nm high-power diode lasers that use extreme double asymmetric vertical designs

NASA Astrophysics Data System (ADS)

Kaul, T.; Erbert, G.; Maaßdorf, A.; Knigge, S.; Crump, P.

2018-03-01

Broad area lasers with novel extreme double asymmetric structure (EDAS) vertical designs featuring increased optical confinement in the quantum well, Γ, are shown to have improved temperature stability without compromising series resistance, internal efficiency or losses. Specifically, we present here vertical design considerations for the improved continuous wave (CW) performance of devices operating at 940 nm, based on systematically increasing Γ from 0.26% to 1.1%, and discuss the impact on power saturation mechanisms. The results indicate that key power saturation mechanisms at high temperatures originate in high threshold carrier densities, which arise in the quantum well at low Γ. The characteristic temperatures, T 0 and T 1, are determined under short pulse conditions and are used to clarify the thermal contribution to power limiting mechanisms. Although increased Γ reduces thermal power saturation, it is accompanied by increased optical absorption losses in the active region, which has a significant impact on the differential external quantum efficiency, {η }{{diff}}. To quantify the impact of internal optical losses contributed by the quantum well, a resonator length-dependent simulation of {η }{{diff}} is performed and compared to the experiment, which also allows the estimation of experimental values for the light absorption cross sections of electrons and holes inside the quantum well. Overall, the analysis enables vertical designs to be developed, for devices with maximized power conversion efficiency at high CW optical power and high temperatures, in a trade-off between absorption in the well and power saturation. The best balance to date is achieved in devices using EDAS designs with {{Γ }}=0.54 % , which deliver efficiencies of 50% at 14 W optical output power at an elevated junction temperature of 105 °C.

Perspective: Quantum mechanical methods in biochemistry and biophysics.

PubMed

Cui, Qiang

2016-10-14

In this perspective article, I discuss several research topics relevant to quantum mechanical (QM) methods in biophysical and biochemical applications. Due to the immense complexity of biological problems, the key is to develop methods that are able to strike the proper balance of computational efficiency and accuracy for the problem of interest. Therefore, in addition to the development of novel ab initio and density functional theory based QM methods for the study of reactive events that involve complex motifs such as transition metal clusters in metalloenzymes, it is equally important to develop inexpensive QM methods and advanced classical or quantal force fields to describe different physicochemical properties of biomolecules and their behaviors in complex environments. Maintaining a solid connection of these more approximate methods with rigorous QM methods is essential to their transferability and robustness. Comparison to diverse experimental observables helps validate computational models and mechanistic hypotheses as well as driving further development of computational methodologies.

A fully electric field driven scalable magnetoelectric switching element

NASA Astrophysics Data System (ADS)

Ahmed, R.; Victora, R. H.

2018-04-01

A technique for micromagnetic simulation of the magnetoelectric (ME) effect in Cr2O3 based structures has been developed. It has been observed that the microscopic ME susceptibility differs significantly from the experimentally measured values. The deviation between the two susceptibilities becomes more prominent near the Curie temperature, affecting the operation of the device at room temperature. A fully electric field controlled ME switching element has been proposed for use at technologically interesting densities: it employs quantum mechanical exchange at the boundaries instead of the applied magnetic field needed in traditional switching schemes. After establishing temperature dependent physics-based parameters, switching performances have been studied for different temperatures, applied electric fields, and Cr2O3 cross-sections. It has been found that our proposed use of quantum mechanical exchange favors reduced electric field operation and enhanced scalability while retaining reliable thermal stability.

State-specific tunneling lifetimes from classical trajectories: H-atom dissociation in electronically excited pyrrole

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

Xie, Weiwei; Domcke, Wolfgang; Farantos, Stavros C.

A trajectory method of calculating tunneling probabilities from phase integrals along straight line tunneling paths, originally suggested by Makri and Miller [J. Chem. Phys. 91, 4026 (1989)] and recently implemented by Truhlar and co-workers [Chem. Sci. 5, 2091 (2014)], is tested for one- and two-dimensional ab initio based potentials describing hydrogen dissociation in the {sup 1}B{sub 1} excited electronic state of pyrrole. The primary observables are the tunneling rates in a progression of bending vibrational states lying below the dissociation barrier and their isotope dependences. Several initial ensembles of classical trajectories have been considered, corresponding to the quasiclassical and themore » quantum mechanical samplings of the initial conditions. It is found that the sampling based on the fixed energy Wigner density gives the best agreement with the quantum mechanical dissociation rates.« less

Collaborative Simulation Grid: Multiscale Quantum-Mechanical/Classical Atomistic Simulations on Distributed PC Clusters in the US and Japan

NASA Technical Reports Server (NTRS)

Kikuchi, Hideaki; Kalia, Rajiv; Nakano, Aiichiro; Vashishta, Priya; Iyetomi, Hiroshi; Ogata, Shuji; Kouno, Takahisa; Shimojo, Fuyuki; Tsuruta, Kanji; Saini, Subhash;

Quantum-chemistry based calibration of the alkali metal cation series (Li(+)-Cs(+)) for large-scale polarizable molecular mechanics/dynamics simulations.

PubMed

Dudev, Todor; Devereux, Mike; Meuwly, Markus; Lim, Carmay; Piquemal, Jean-Philip; Gresh, Nohad

2015-02-15

The alkali metal cations in the series Li(+)-Cs(+) act as major partners in a diversity of biological processes and in bioinorganic chemistry. In this article, we present the results of their calibration in the context of the SIBFA polarizable molecular mechanics/dynamics procedure. It relies on quantum-chemistry (QC) energy-decomposition analyses of their monoligated complexes with representative O-, N-, S-, and Se- ligands, performed with the aug-cc-pVTZ(-f) basis set at the Hartree-Fock level. Close agreement with QC is obtained for each individual contribution, even though the calibration involves only a limited set of cation-specific parameters. This agreement is preserved in tests on polyligated complexes with four and six O- ligands, water and formamide, indicating the transferability of the procedure. Preliminary extensions to density functional theory calculations are reported. © 2014 Wiley Periodicals, Inc.

Electronic, Mechanical, and Dielectric Properties of Two-Dimensional Atomic Layers of Noble Metals

NASA Astrophysics Data System (ADS)

Kapoor, Pooja; Kumar, Jagdish; Kumar, Arun; Kumar, Ashok; Ahluwalia, P. K.

2017-01-01

We present density functional theory-based electronic, mechanical, and dielectric properties of monolayers and bilayers of noble metals (Au, Ag, Cu, and Pt) taken with graphene-like hexagonal structure. The Au, Ag, and Pt bilayers stabilize in AA-stacked configuration, while the Cu bilayer favors the AB stacking pattern. The quantum ballistic conductance of the noble-metal mono- and bilayers is remarkably increased compared with their bulk counterparts. Among the studied systems, the tensile strength is found to be highest for the Pt monolayer and bilayer. The noble metals in mono- and bilayer form show distinctly different electron energy loss spectra and reflectance spectra due to the quantum confinement effect on going from bulk to the monolayer limit. Such tunability of the electronic and dielectric properties of noble metals by reducing the degrees of freedom of electrons offers promise for their use in nanoelectronics and optoelectronics applications.

Ionocovalency and Applications 1. Ionocovalency Model and Orbital Hybrid Scales

PubMed Central

Zhang, Yonghe

2010-01-01

Ionocovalency (IC), a quantitative dual nature of the atom, is defined and correlated with quantum-mechanical potential to describe quantitatively the dual properties of the bond. Orbiotal hybrid IC model scale, IC, and IC electronegativity scale, XIC, are proposed, wherein the ionicity and the covalent radius are determined by spectroscopy. Being composed of the ionic function I and the covalent function C, the model describes quantitatively the dual properties of bond strengths, charge density and ionic potential. Based on the atomic electron configuration and the various quantum-mechanical built-up dual parameters, the model formed a Dual Method of the multiple-functional prediction, which has much more versatile and exceptional applications than traditional electronegativity scales and molecular properties. Hydrogen has unconventional values of IC and XIC, lower than that of boron. The IC model can agree fairly well with the data of bond properties and satisfactorily explain chemical observations of elements throughout the Periodic Table. PMID:21151444

A hundred years with the cosmological constant

NASA Astrophysics Data System (ADS)

Grøn, Øyvind G.

2018-07-01

The main points in the history of the cosmological constant are briefly discussed. As a conceptual background, useful for teaching of physics at an elementary college and university level, Newton’s theory formulated locally in terms of the Poisson equation is presented, and it is shown how it is modified by the introduction of the cosmological constant. The different physical interpretations of the cosmological constant, as introduced by Einstein in 1917 and interpreted by Lemaître in 1934, are presented. Energy conservation in an expanding universe dominated by vacuum energy is discussed. The connection between the cosmological constant and the quantum mechanical vacuum energy is mentioned, together with the problem that a quantum mechanical calculation of the density of the vacuum energy gives a vastly too large value of the cosmological constant. The article is concluded by reviewing a solution of this problem that was presented on May 11, 2017.

Multiscale Study of Plasmonic Scattering and Light Trapping Effect in Silicon Nanowire Array Solar Cells.

PubMed

Meng, Lingyi; Zhang, Yu; Yam, ChiYung

2017-02-02

Nanometallic structures that support surface plasmons provide new ways to confine light at deep-subwavelength scales. The effect of light scattering in nanowire array solar cells is studied by a multiscale approach combining classical electromagnetic (EM) and quantum mechanical simulations. A photovoltaic device is constructed by integrating a silicon nanowire array with a plasmonic silver nanosphere. The light scatterings by plasmonic element and nanowire array are obtained via classical EM simulations, while current-voltage characteristics and optical properties of the nanowire cells are evaluated quantum mechanically. We found that the power conversion efficiency (PCE) of photovoltaic device is substantially improved due to the local field enhancement of the plasmonic effect and light trapping by the nanowire array. In addition, we showed that there exists an optimal nanowire number density in terms of optical confinement and solar cell PCE.

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

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

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

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

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

DOE PAGES

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

2016-12-28

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

Quantum mechanical identification of quadrupolar plasmonic excited states in silver nanorods

DOE PAGES

Gieseking, Rebecca L.; Ratner, Mark A.; Schatz, George C.

2016-10-27

Quadrupolar plasmonic modes in noble metal nanoparticles have gained interest in recent years for various sensing applications. Although quantum mechanical studies have shown that dipolar plasmons can be modeled in terms of excited states where several to many excitations contribute coherently to the transition dipole moment, new approaches are needed to identify the quadrupolar plasmonic states. We show that quadrupolar states in Ag nanorods can be identified using the semiempirical INDO/SCI approach by examining the quadrupole moment of the transition density. The main longitudinal quadrupolar states occur at higher energies than the longitudinal dipolar states, in agreement with previous classicalmore » electrodynamics results, and have collective plasmonic character when the nanorods are sufficiently long. In conclusion, the ability to identify these states will make it possible to evaluate the differences between dipolar and quadrupolar plasmons that are relevant for sensing applications.« less

Quantum chemical calculation (electronic and topologic) and experimental (FT-IR, FT-Raman and UV) analysis of isonicotinic acid N-oxide

NASA Astrophysics Data System (ADS)

Karaca, Caglar; Atac, Ahmet; Karabacak, Mehmet

2015-04-01

In this work, the molecular conformation, vibrational and electronic analysis of isonicotinic acid N-oxide (iso-NANO) were presented in the ground state using experimental techniques (FT-IR, FT-Raman and UV) and density functional theory (DFT) employing B3LYP exchange correlation with the 6-311++G(d,p) basis set. The geometry optimization and energies associated possible two conformers (Rot-I and Rot-II) were computed. The vibrational spectra were calculated and fundamental vibrations were assigned on the basis of the total energy distribution (TED) of the vibrational modes, calculated with scaled quantum mechanics (SQM) method and PQS program. The obtained structures were analyzed with the Atoms in Molecules (AIMs) methodology. The computational results diagnose the most stable conformer of iso-NANO as the Rot-I form. Total density of state (TDOS) and partial density of state (PDOS) and also overlap population density of state (OPDOS) diagrams analysis for the most stable conformer (Rot-I) were calculated using the same method. Thermodynamic properties (heat capacity, entropy and enthalpy) of the title compound at different temperatures were calculated. As a result, the optimized geometry and calculated spectroscopic data show a good agreement with the experimental results.

Elastically frustrated rehybridization: Origin of chemical order and compositional limits in InGaN quantum wells

NASA Astrophysics Data System (ADS)

Lymperakis, L.; Schulz, T.; Freysoldt, C.; Anikeeva, M.; Chen, Z.; Zheng, X.; Shen, B.; Chèze, C.; Siekacz, M.; Wang, X. Q.; Albrecht, M.; Neugebauer, J.

2018-01-01

Nominal InN monolayers grown by molecular beam epitaxy on GaN(0001) are investigated combining in situ reflection high-energy electron diffraction (RHEED), transmission electron microscopy (TEM), and density functional theory (DFT). TEM reveals a chemical intraplane ordering never observed before. Employing DFT, we identify a novel surface stabilization mechanism elastically frustrated rehybridization, which is responsible for the observed chemical ordering. The mechanism also sets an incorporation barrier for indium concentrations above 25% and thus fundamentally limits the indium content in coherently strained layers.

DBI in the Sky

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

Alishahiha, M

2004-04-19

We analyze the spectrum of density perturbations generated in models of the recently discovered ''D-cceleration'' mechanism of inflation. In this scenario, strong coupling quantum field theoretic effects sum to provide a DBI-like action for the inflaton. We show that the model has a strict lower bound on the non-Gaussianity of the CMBR power spectrum at an observable level, and is thus falsifiable. This in particular observationally distinguishes this mechanism from traditional slow roll inflation generated by weakly interacting scalar fields. The model also favors a large observable tensor component to the CMBR spectrum.

Statistical Mechanics and Applications in Condensed Matter

NASA Astrophysics Data System (ADS)

Di Castro, Carlo; Raimondi, Roberto

2015-08-01

Preface; 1. Thermodynamics: a brief overview; 2. Kinetics; 3. From Boltzmann to Gibbs; 4. More ensembles; 5. The thermodynamic limit and its thermodynamic stability; 6. Density matrix and quantum statistical mechanics; 7. The quantum gases; 8. Mean-field theories and critical phenomena; 9. Second quantization and Hartree-Fock approximation; 10. Linear response and fluctuation-dissipation theorem in quantum systems: equilibrium and small deviations; 11. Brownian motion and transport in disordered systems; 12. Fermi liquids; 13. The Landau theory of the second order phase transitions; 14. The Landau-Wilson model for critical phenomena; 15. Superfluidity and superconductivity; 16. The scaling theory; 17. The renormalization group approach; 18. Thermal Green functions; 19. The microscopic foundations of Fermi liquids; 20. The Luttinger liquid; 21. Quantum interference effects in disordered electron systems; Appendix A. The central limit theorem; Appendix B. Some useful properties of the Euler Gamma function; Appendix C. Proof of the second theorem of Yang and Lee; Appendix D. The most probable distribution for the quantum gases; Appendix E. Fermi-Dirac and Bose-Einstein integrals; Appendix F. The Fermi gas in a uniform magnetic field: Landau diamagnetism; Appendix G. Ising and gas-lattice models; Appendix H. Sum over discrete Matsubara frequencies; Appendix I. Hydrodynamics of the two-fluid model of superfluidity; Appendix J. The Cooper problem in the theory of superconductivity; Appendix K. Superconductive fluctuations phenomena; Appendix L. Diagrammatic aspects of the exact solution of the Tomonaga Luttinger model; Appendix M. Details on the theory of the disordered Fermi liquid; References; Author index; Index.

Quantum coherent switch utilizing commensurate nanoelectrode and charge density periodicities

DOEpatents

Harrison,; Neil, Singleton [Santa Fe, NM; John, Migliori [Los Alamos, NM; Albert, [Santa Fe, NM

2008-08-05

A quantum coherent switch having a substrate formed from a density wave (DW) material capable of having a periodic electron density modulation or spin density modulation, a dielectric layer formed onto a surface of the substrate that is orthogonal to an intrinsic wave vector of the DW material; and structure for applying an external spatially periodic electrostatic potential over the dielectric layer.

Photonic entanglement-assisted quantum low-density parity-check encoders and decoders.

PubMed

Djordjevic, Ivan B

2010-05-01

I propose encoder and decoder architectures for entanglement-assisted (EA) quantum low-density parity-check (LDPC) codes suitable for all-optical implementation. I show that two basic gates needed for EA quantum error correction, namely, controlled-NOT (CNOT) and Hadamard gates can be implemented based on Mach-Zehnder interferometer. In addition, I show that EA quantum LDPC codes from balanced incomplete block designs of unitary index require only one entanglement qubit to be shared between source and destination.

Scaled Quantum Mechanical scale factors for vibrational calculations using alternate polarized and augmented basis sets with the B3LYP density functional calculation model

NASA Astrophysics Data System (ADS)

Legler, C. R.; Brown, N. R.; Dunbar, R. A.; Harness, M. D.; Nguyen, K.; Oyewole, O.; Collier, W. B.

2015-06-01

The Scaled Quantum Mechanical (SQM) method of scaling calculated force constants to predict theoretically calculated vibrational frequencies is expanded to include a broad array of polarized and augmented basis sets based on the split valence 6-31G and 6-311G basis sets with the B3LYP density functional. Pulay's original choice of a single polarized 6-31G(d) basis coupled with a B3LYP functional remains the most computationally economical choice for scaled frequency calculations. But it can be improved upon with additional polarization functions and added diffuse functions for complex molecular systems. The new scale factors for the B3LYP density functional and the 6-31G, 6-31G(d), 6-31G(d,p), 6-31G+(d,p), 6-31G++(d,p), 6-311G, 6-311G(d), 6-311G(d,p), 6-311G+(d,p), 6-311G++(d,p), 6-311G(2d,p), 6-311G++(2d,p), 6-311G++(df,p) basis sets are shown. The double d polarized models did not perform as well and the source of the decreased accuracy was investigated. An alternate system of generating internal coordinates that uses the out-of plane wagging coordinate whenever it is possible; makes vibrational assignments via potential energy distributions more meaningful. Automated software to produce SQM scaled vibrational calculations from different molecular orbital packages is presented.

Electron transfer in a virtual quantum state of LiBH4 induced by strong optical fields and mapped by femtosecond x-ray diffraction.

PubMed

Stingl, J; Zamponi, F; Freyer, B; Woerner, M; Elsaesser, T; Borgschulte, A

2012-10-05

Transient polarizations connected with a spatial redistribution of electronic charge in a mixed quantum state are induced by optical fields of high amplitude. We determine for the first time the related transient electron density maps, applying femtosecond x-ray powder diffraction as a structure probe. The prototype ionic material LiBH4 driven nonresonantly by an intense sub-40 fs optical pulse displays a large-amplitude fully reversible electron transfer from the BH4(-) anion to the Li+ cation during excitation. Our results establish this mechanism as the source of the strong optical polarization which agrees quantitatively with theoretical estimates.

Investigation of the CH3Cl + CN(-) reaction in water: Multilevel quantum mechanics/molecular mechanics study.

PubMed

Xu, Yulong; Zhang, Jingxue; Wang, Dunyou

2015-06-28

The CH3Cl + CN(-) reaction in water was studied using a multilevel quantum mechanics/molecular mechanics (MM) method with the multilevels, electrostatic potential, density functional theory (DFT) and coupled-cluster single double triple (CCSD(T)), for the solute region. The detailed, back-side attack SN2 reaction mechanism was mapped along the reaction pathway. The potentials of mean force were calculated under both the DFT and CCSD(T) levels for the reaction region. The CCSD(T)/MM level of theory presents a free energy activation barrier height at 20.3 kcal/mol, which agrees very well with the experiment value at 21.6 kcal/mol. The results show that the aqueous solution has a dominant role in shaping the potential of mean force. The solvation effect and the polarization effect together increase the activation barrier height by ∼11.4 kcal/mol: the solvation effect plays a major role by providing about 75% of the contribution, while polarization effect only contributes 25% to the activation barrier height. Our calculated potential of mean force under the CCSD(T)/MM also has a good agreement with the one estimated using data from previous gas-phase studies.

Investigation of the CH3Cl + CN- reaction in water: Multilevel quantum mechanics/molecular mechanics study

NASA Astrophysics Data System (ADS)

Xu, Yulong; Zhang, Jingxue; Wang, Dunyou

2015-06-01

The CH3Cl + CN- reaction in water was studied using a multilevel quantum mechanics/molecular mechanics (MM) method with the multilevels, electrostatic potential, density functional theory (DFT) and coupled-cluster single double triple (CCSD(T)), for the solute region. The detailed, back-side attack SN2 reaction mechanism was mapped along the reaction pathway. The potentials of mean force were calculated under both the DFT and CCSD(T) levels for the reaction region. The CCSD(T)/MM level of theory presents a free energy activation barrier height at 20.3 kcal/mol, which agrees very well with the experiment value at 21.6 kcal/mol. The results show that the aqueous solution has a dominant role in shaping the potential of mean force. The solvation effect and the polarization effect together increase the activation barrier height by ˜11.4 kcal/mol: the solvation effect plays a major role by providing about 75% of the contribution, while polarization effect only contributes 25% to the activation barrier height. Our calculated potential of mean force under the CCSD(T)/MM also has a good agreement with the one estimated using data from previous gas-phase studies.

Exploration of near the origin and the asymptotic behaviors of the Kohn-Sham kinetic energy density for two-dimensional quantum dot systems with parabolic confinement

NASA Astrophysics Data System (ADS)

Jana, Subrata; Samal, Prasanjit

2018-01-01

The behaviors of the positive definite Kohn-Sham kinetic energy density near the origin and at the asymptotic region play a major role in designing meta-generalized gradient approximations (meta-GGAs) for exchange in low-dimensional quantum systems. It is shown that near the origin of the parabolic quantum dot, the Kohn-Sham kinetic energy differs from its von Weizsäcker counterpart due to the p orbital contributions, whereas in the asymptotic region, the difference between the above two kinetic energy densities goes as ˜ρ/(r ) r2 . All these behaviors have been explored using the two-dimensional isotropic quantum harmonic oscillator as a test case. Several meta-GGA ingredients are then studied by making use of the above findings. Also, the asymptotic conditions for the exchange energy density and the potential at the meta-GGA level are proposed using the corresponding behaviors of the two kinetic energy densities.

Exploration of near the origin and the asymptotic behaviors of the Kohn-Sham kinetic energy density for two-dimensional quantum dot systems with parabolic confinement.

PubMed

Jana, Subrata; Samal, Prasanjit

2018-01-14

The behaviors of the positive definite Kohn-Sham kinetic energy density near the origin and at the asymptotic region play a major role in designing meta-generalized gradient approximations (meta-GGAs) for exchange in low-dimensional quantum systems. It is shown that near the origin of the parabolic quantum dot, the Kohn-Sham kinetic energy differs from its von Weizsäcker counterpart due to the p orbital contributions, whereas in the asymptotic region, the difference between the above two kinetic energy densities goes as ∼ρ(r)r 2 . All these behaviors have been explored using the two-dimensional isotropic quantum harmonic oscillator as a test case. Several meta-GGA ingredients are then studied by making use of the above findings. Also, the asymptotic conditions for the exchange energy density and the potential at the meta-GGA level are proposed using the corresponding behaviors of the two kinetic energy densities.

Time-Dependent Density Functional Theory for Open Systems and Its Applications.

PubMed

Chen, Shuguang; Kwok, YanHo; Chen, GuanHua

2018-02-20

Photovoltaic devices, electrochemical cells, catalysis processes, light emitting diodes, scanning tunneling microscopes, molecular electronics, and related devices have one thing in common: open quantum systems where energy and matter are not conserved. Traditionally quantum chemistry is confined to isolated and closed systems, while quantum dissipation theory studies open quantum systems. The key quantity in quantum dissipation theory is the reduced system density matrix. As the reduced system density matrix is an O(M! × M!) matrix, where M is the number of the particles of the system of interest, quantum dissipation theory can only be employed to simulate systems of a few particles or degrees of freedom. It is thus important to combine quantum chemistry and quantum dissipation theory so that realistic open quantum systems can be simulated from first-principles. We have developed a first-principles method to simulate the dynamics of open electronic systems, the time-dependent density functional theory for open systems (TDDFT-OS). Instead of the reduced system density matrix, the key quantity is the reduced single-electron density matrix, which is an N × N matrix where N is the number of the atomic bases of the system of interest. As the dimension of the key quantity is drastically reduced, the TDDFT-OS can thus be used to simulate the dynamics of realistic open electronic systems and efficient numerical algorithms have been developed. As an application, we apply the method to study how quantum interference develops in a molecular transistor in time domain. We include electron-phonon interaction in our simulation and show that quantum interference in the given system is robust against nuclear vibration not only in the steady state but also in the transient dynamics. As another application, by combining TDDFT-OS with Ehrenfest dynamics, we study current-induced dissociation of water molecules under scanning tunneling microscopy and follow its time dependent dynamics. Given the rapid development in ultrafast experiments with atomic resolution in recent years, time dependent simulation of open electronic systems will be useful to gain insight and understanding of such experiments. This Account will mainly focus on the practical aspects of the TDDFT-OS method, describing the numerical implementation and demonstrating the method with applications.

Quantum Mechanical Earth: Where Orbitals Become Orbits

ERIC Educational Resources Information Center

Keeports, David

2012-01-01

Macroscopic objects, although quantum mechanical by nature, conform to Newtonian mechanics under normal observation. According to the quantum mechanical correspondence principle, quantum behavior is indistinguishable from classical behavior in the limit of very large quantum numbers. The purpose of this paper is to provide an example of the…

Three pillars for achieving quantum mechanical molecular dynamics simulations of huge systems: Divide-and-conquer, density-functional tight-binding, and massively parallel computation.

PubMed

Nishizawa, Hiroaki; Nishimura, Yoshifumi; Kobayashi, Masato; Irle, Stephan; Nakai, Hiromi

2016-08-05

The linear-scaling divide-and-conquer (DC) quantum chemical methodology is applied to the density-functional tight-binding (DFTB) theory to develop a massively parallel program that achieves on-the-fly molecular reaction dynamics simulations of huge systems from scratch. The functions to perform large scale geometry optimization and molecular dynamics with DC-DFTB potential energy surface are implemented to the program called DC-DFTB-K. A novel interpolation-based algorithm is developed for parallelizing the determination of the Fermi level in the DC method. The performance of the DC-DFTB-K program is assessed using a laboratory computer and the K computer. Numerical tests show the high efficiency of the DC-DFTB-K program, a single-point energy gradient calculation of a one-million-atom system is completed within 60 s using 7290 nodes of the K computer. © 2016 Wiley Periodicals, Inc. © 2016 Wiley Periodicals, Inc.

[Effects of quantum nonlocality in the water activation process].

PubMed

Zatsepina, O V; Stekhin, A A; Yakovleva, G V

2014-01-01

The dynamic alterations of the magnetic flux density of the water volume, activated with structurally stressed calcium carbonate in micellar form have been investigated. The phase of the associated water was established to exhibit electrical and magnetic properties, recorded by in B&E meter in the frequency range of 5Hz - 2kHz. Alterations in water Eh (redox) potential and the magnetic flux density B testify to synchronous auto-oscillatory changes. This gives evidence of non-linearity of the relationship between auto-oscillatory processes excited in the water; and reflects the nonlocal in time the relationship between the states of water, manifesting in a change of water activity on the 1st and 2nd day in negative time. The mechanism of action of associated water phase is shown to be described by de Broglie concept of matter waves with taking into account delocalized in time states of phase of electron wave packet in accordance with the transactional interpretation of quantum physics.

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

NASA Astrophysics Data System (ADS)

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

2012-09-01

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

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

NASA Astrophysics Data System (ADS)

Mazzola, Guglielmo; Helled, Ravit; Sorella, Sandro

2018-01-01

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

Enhanced Solar Cell Conversion Efficiency of InGaN/GaN Multiple Quantum Wells by Piezo-Phototronic Effect.

PubMed

Jiang, Chunyan; Jing, Liang; Huang, Xin; Liu, Mengmeng; Du, Chunhua; Liu, Ting; Pu, Xiong; Hu, Weiguo; Wang, Zhong Lin

2017-09-26

The piezo-phototronic effect is the tuning of piezoelectric polarization charges at the interface to largely enhance the efficiency of optoelectronic processes related to carrier separation or recombination. Here, we demonstrated the enhanced short-circuit current density and the conversion efficiency of InGaN/GaN multiple quantum well solar cells with an external stress applied on the device. The external-stress-induced piezoelectric charges generated at the interfaces of InGaN and GaN compensate the piezoelectric charges induced by lattice mismatch stress in the InGaN wells. The energy band realignment is calculated with a self-consistent numerical model to clarify the enhancement mechanism of optical-generated carriers. This research not only theoretically and experimentally proves the piezo-phototronic effect modulated the quantum photovoltaic device but also provides a great promise to maximize the use of solar energy in the current energy revolution.

Quantum Dynamics in Continuum for Proton Transport I: Basic Formulation.

PubMed

Chen, Duan; Wei, Guo-Wei

2013-01-01

Proton transport is one of the most important and interesting phenomena in living cells. The present work proposes a multiscale/multiphysics model for the understanding of the molecular mechanism of proton transport in transmembrane proteins. We describe proton dynamics quantum mechanically via a density functional approach while implicitly model other solvent ions as a dielectric continuum to reduce the number of degrees of freedom. The densities of all other ions in the solvent are assumed to obey the Boltzmann distribution. The impact of protein molecular structure and its charge polarization on the proton transport is considered explicitly at the atomic level. We formulate a total free energy functional to put proton kinetic and potential energies as well as electrostatic energy of all ions on an equal footing. The variational principle is employed to derive nonlinear governing equations for the proton transport system. Generalized Poisson-Boltzmann equation and Kohn-Sham equation are obtained from the variational framework. Theoretical formulations for the proton density and proton conductance are constructed based on fundamental principles. The molecular surface of the channel protein is utilized to split the discrete protein domain and the continuum solvent domain, and facilitate the multiscale discrete/continuum/quantum descriptions. A number of mathematical algorithms, including the Dirichlet to Neumann mapping, matched interface and boundary method, Gummel iteration, and Krylov space techniques are utilized to implement the proposed model in a computationally efficient manner. The Gramicidin A (GA) channel is used to demonstrate the performance of the proposed proton transport model and validate the efficiency of proposed mathematical algorithms. The electrostatic characteristics of the GA channel is analyzed with a wide range of model parameters. The proton conductances are studied over a number of applied voltages and reference concentrations. A comparison with experimental data verifies the present model predictions and validates the proposed model.

Photoluminescence Spectra From The Direct Energy Gap of a-SiQDs

NASA Astrophysics Data System (ADS)

Abdul-Ameer, Nidhal M.; Abdulrida, Moafak C.; Abdul-Hakeem, Shatha M.

2018-05-01

A theoretical model for radiative recombination in amorphous silicon quantum dots (a-SiQDs) was developed. In this model, for the first time, the coexistence of both spatial and quantum confinements were considered. Also, it is found that the photoluminescence exhibits significant size dependence in the range (1-4) nm of the quantum dots. a-SiQDs show visible light emission peak energies and high radiative quantum efficiency at room temperature,in contrast to bulk a-Si structures. The quantum efficiency is sensitive to any change in defect density (the volume nonradiative centers density and/or the surface nonradiative centers density) but, with small dots sizes, the quantum efficiency is insensitive to such defects. Our analysis shows that the photoluminescence intensity increases or decreases by the effect of radiative quantum efficiency. By controlling the size of a-SiQDs, we note that the energy of emission can be tuned. The blue shift is attributed to quantum confinement effect. Meanwhile, the spatial confinement effect is clearly observed in red shift in emission spectra. we found a good agreement with the experimental published data. Therefore, we assert that a-SiQDs material is a promising candidate for visible, tunable, and high performance devices of light emitting.

Quantum entanglement and spin control in silicon nanocrystal.

PubMed

Berec, Vesna

2012-01-01

Selective coherence control and electrically mediated exchange coupling of single electron spin between triplet and singlet states using numerically derived optimal control of proton pulses is demonstrated. We obtained spatial confinement below size of the Bohr radius for proton spin chain FWHM. Precise manipulation of individual spins and polarization of electron spin states are analyzed via proton induced emission and controlled population of energy shells in pure (29)Si nanocrystal. Entangled quantum states of channeled proton trajectories are mapped in transverse and angular phase space of (29)Si <100> axial channel alignment in order to avoid transversal excitations. Proton density and proton energy as impact parameter functions are characterized in single particle density matrix via discretization of diagonal and nearest off-diagonal elements. We combined high field and low densities (1 MeV/92 nm) to create inseparable quantum state by superimposing the hyperpolarizationed proton spin chain with electron spin of (29)Si. Quantum discretization of density of states (DOS) was performed by the Monte Carlo simulation method using numerical solutions of proton equations of motion. Distribution of gaussian coherent states is obtained by continuous modulation of individual spin phase and amplitude. Obtained results allow precise engineering and faithful mapping of spin states. This would provide the effective quantum key distribution (QKD) and transmission of quantum information over remote distances between quantum memory centers for scalable quantum communication network. Furthermore, obtained results give insights in application of channeled protons subatomic microscopy as a complete versatile scanning-probe system capable of both quantum engineering of charged particle states and characterization of quantum states below diffraction limit linear and in-depth resolution.PACS NUMBERS: 03.65.Ud, 03.67.Bg, 61.85.+p, 67.30.hj.

Tunneling time in space fractional quantum mechanics

NASA Astrophysics Data System (ADS)

Hasan, Mohammad; Mandal, Bhabani Prasad

2018-02-01

We calculate the time taken by a wave packet to travel through a classically forbidden region of space in space fractional quantum mechanics. We obtain the close form expression of tunneling time from a rectangular barrier by stationary phase method. We show that tunneling time depends upon the width b of the barrier for b → ∞ and therefore Hartman effect doesn't exist in space fractional quantum mechanics. Interestingly we found that the tunneling time monotonically reduces with increasing b. The tunneling time is smaller in space fractional quantum mechanics as compared to the case of standard quantum mechanics. We recover the Hartman effect of standard quantum mechanics as a special case of space fractional quantum mechanics.

Surface Lifshits tails for random quantum Hamiltonians

NASA Astrophysics Data System (ADS)

Kirsch, Werner; Raikov, Georgi

2017-03-01

We consider Schrödinger operators on L2(ℝd) ⊗L2 (ℝℓ) of the form Hω=H⊥⊗I∥ +I⊥⊗H∥ +Vω , where H⊥ and H∥ are Schrödinger operators on L2(ℝd) and L2(ℝℓ) , respectively, and Vω(x ,y ) :=∑ξ∈ℤdλξ(ω ) v (x -ξ ,y ) ,x ∈ℝd ,y ∈ℝℓ is a random "surface potential." We investigate the behavior of the integrated density of surface states of Hω near the bottom of the spectrum and near internal band edges. The main result of the current paper is that, under suitable assumptions, the behavior of the integrated density of surface states of Hω can be read off from the integrated density of states of a reduced Hamiltonian H⊥+Wω where Wω is a quantum mechanical average of Vω with respect to y ∈ℝℓ . We are particularly interested in cases when H⊥ is a magnetic Schrödinger operator, but we also recover some of the results from Kirsch and Warzel [J. Funct. Anal. 230, 222-250 (2006)] for non-magnetic H⊥.

Twist-averaged boundary conditions for nuclear pasta Hartree-Fock calculations

DOE PAGES

Schuetrumpf, B.; Nazarewicz, W.

2015-10-21

Nuclear pasta phases, present in the inner crust of neutron stars, are associated with nucleonic matter at subsaturation densities arranged in regular shapes. Those complex phases, residing in a layer which is approximately 100-m thick, impact many features of neutron stars. Theoretical quantum-mechanical simulations of nuclear pasta are usually carried out in finite three-dimensional boxes assuming periodic boundary conditions. The resulting solutions are affected by spurious finite-size effects. To remove spurious finite-size effects, it is convenient to employ twist-averaged boundary conditions (TABC) used in condensed matter, nuclear matter, and lattice quantum chromodynamics applications. In this work, we study the effectivenessmore » of TABC in the context of pasta phase simulations within nuclear density functional theory. We demonstrated that by applying TABC reliable results can be obtained from calculations performed in relatively small volumes. By studying various contributions to the total energy, we gain insights into pasta phases in mid-density range. Future applications will include the TABC extension of the adaptive multiresolution 3D Hartree-Fock solver and Hartree-Fock-Bogoliubov TABC applications to superfluid pasta phases and complex nucleonic topologies as in fission.« less

Comparative studies of efficiency droop in polar and non-polar InGaN quantum wells

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

Davies, M. J.; Dawson, P.; Hammersley, S.

We report on a comparative study of efficiency droop in polar and non-polar InGaN quantum well structures at T = 10 K. To ensure that the experiments were carried out with identical carrier densities for any particular excitation power density, we used laser pulses of duration ∼100 fs at a repetition rate of 400 kHz. For both types of structures, efficiency droop was observed to occur for carrier densities of above 7 × 10{sup 11 }cm{sup −2 }pulse{sup −1} per quantum well; also both structures exhibited similar spectral broadening in the droop regime. These results show that efficiency droop is intrinsic in InGaN quantum wells, whether polar or non-polar,more » and is a function, specifically, of carrier density.« less

Per-Olov Löwdin - father of quantum chemistry

NASA Astrophysics Data System (ADS)

Brändas, Erkki J.

2017-09-01

During 2016, we celebrate the 100th anniversary of the birth of Per-Olov Löwdin. He was appointed to the first Lehrstuhl in quantum chemistry at Uppsala University in 1960. Löwdin introduced quantum chemistry as a field in its own right by formulating its goals, establishing fundamental concepts, like the correlation energy, the method of configuration interaction, reduced density matrices, natural spin orbitals, charge and bond order matrices, symmetric orthogonalisation, and generalised self-consistent fields. His exposition of partitioning technique and perturbation theory, wave and reaction operators and associated non-linear summation techniques, introduced mathematical rigour and deductive order in the interpretative organisation of the new field. He brought the first computer to Uppsala University and pioneered the initiation of 'electronic brains' and anticipated their significance for quantum chemistry. Perhaps his single most influential contribution to the field was his education of two generations of future faculty in quantum chemistry through Summer Schools in the Scandinavian Mountains, Winter Institutes at Sanibel Island in the Gulf of Mexico. Per-Olov Löwdin founded the book series Advances in Quantum Chemistry and the International Journal of Quantum Chemistry. The evolution of quantum chemistry is appraised, starting from a collection of cross-disciplinary applications of quantum mechanics to the technologically advanced and predominant field of today, virtually used in all branches of chemistry. The scientific work of Per-Olov Löwdin has been crucial for the development of this new important province of science.

Stabilization of the Rayleigh-Taylor instability in quantum magnetized plasmas

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

Wang, L. F.; Ye, W. H.; He, X. T.

2012-07-15

In this research, stabilization of the Rayleigh-Taylor instability (RTI) due to density gradients, magnetic fields, and quantum effects, in an ideal incompressible plasma, is studied analytically and numerically. A second-order ordinary differential equation (ODE) for the RTI including quantum corrections, with a continuous density profile, in a uniform external magnetic field, is obtained. Analytic expressions of the linear growth rate of the RTI, considering modifications of density gradients, magnetic fields, and quantum effects, are presented. Numerical approaches are performed to solve the second-order ODE. The analytical model proposed here agrees with the numerical calculation. It is found that the densitymore » gradients, the magnetic fields, and the quantum effects, respectively, have a stabilizing effect on the RTI (reduce the linear growth of the RTI). The RTI can be completely quenched by the magnetic field stabilization and/or the quantum effect stabilization in proper circumstances leading to a cutoff wavelength. The quantum effect stabilization plays a central role in systems with large Atwood number and small normalized density gradient scale length. The presence of external transverse magnetic fields beside the quantum effects will bring about more stability on the RTI. The stabilization of the linear growth of the RTI, for parameters closely related to inertial confinement fusion and white dwarfs, is discussed. Results could potentially be valuable for the RTI treatment to analyze the mixing in supernovas and other RTI-driven objects.« less

On-chip RF-to-optical transducer (Conference Presentation)

NASA Astrophysics Data System (ADS)

Simonsen, Anders; Tsaturyan, Yeghishe; Seis, Yannick; Schmid, Silvan; Schliesser, Albert; Polzik, Eugene S.

2016-04-01

Recent advances in the fabrication of nano- and micromechanical elements enable the realization of high-quality mechanical resonators with masses so small that the forces from optical photons can have a significant impact on their motion. This facilitates a strong interaction between mechanical motion and light, or phonons and photons. This interaction is the corner stone of the field of optomechanics and allows, for example, for ultrasensitive detection and manipulation of mechanical motion using laser light. Remarkably, today these techniques can be extended into the quantum regime, in which fundamental fluctuations of light and mechanics govern the system's behavior. Micromechanical elements can also interact strongly with other physical systems, which is the central aspect of many micro-electro-mechanical based sensors. Micromechanical elements can therefore act as a bridge between these diverse systems, plus technologies that utilize them, and the mature toolbox of optical techniques that routinely operates at the quantum limit. In a previous work [1], we demonstrated such a bridge by realizing simultaneous coupling between an electronic LC circuit and a quantum-noise limited optical interferometer. The coupling was mediated by a mechanical oscillator forming a mechanically compliant capacitor biased with a DC voltage. The latter enhances the electromechanical interaction all the way to the strong coupling regime. That scheme allowed optical detection of electronic signals with effective noise temperatures far below the actual temperature of the mechanical element. On-chip integration of the electrical, mechanical and optical elements is necessary for an implementation of the transduction scheme that is viable for commercial applications. Reliable assembly of a strongly coupled electromechanical device, and inclusion of an optical cavity for enhanced optical readout, are key features of the new platform. Both can be achieved with standard cleanroom fabrication techniques. We will furthermore present ongoing work to couple our transducer to an RF or microwave antenna, for low-noise detection of electromagnetic signals, including sensitive measurements of magnetic fields in an MRI detector. Suppression of thermomechanical noise is a key feature of electro-optomechanical transducers, and, more generally, hybrid systems involving mechanical degrees of freedom. We have shown that engineering of the phononic density of states allows improved isolation of the relevant mechanical modes from their thermal bath [2], enabling coherence times sufficient to realize quantum-coherent optomechanical coupling. This proves the potential of the employed platform for complex transducers all the way into the quantum regime. References: [1] Bagci et al, Nature 507, 81-85, (06 March 2014) [2] Tsaturyan, et al., Optics Express, Vol. 22, Issue 6, pp. 6810-6821 (2014)

Pulsed quantum optomechanics

PubMed Central

Vanner, M. R.; Pikovski, I.; Cole, G. D.; Kim, M. S.; Brukner, Č.; Hammerer, K.; Milburn, G. J.; Aspelmeyer, M.

2011-01-01

Studying mechanical resonators via radiation pressure offers a rich avenue for the exploration of quantum mechanical behavior in a macroscopic regime. However, quantum state preparation and especially quantum state reconstruction of mechanical oscillators remains a significant challenge. Here we propose a scheme to realize quantum state tomography, squeezing, and state purification of a mechanical resonator using short optical pulses. The scheme presented allows observation of mechanical quantum features despite preparation from a thermal state and is shown to be experimentally feasible using optical microcavities. Our framework thus provides a promising means to explore the quantum nature of massive mechanical oscillators and can be applied to other systems such as trapped ions. PMID:21900608

Adiabatic Quantum Search in Open Systems.

PubMed

Wild, Dominik S; Gopalakrishnan, Sarang; Knap, Michael; Yao, Norman Y; Lukin, Mikhail D

2016-10-07

Adiabatic quantum algorithms represent a promising approach to universal quantum computation. In isolated systems, a key limitation to such algorithms is the presence of avoided level crossings, where gaps become extremely small. In open quantum systems, the fundamental robustness of adiabatic algorithms remains unresolved. Here, we study the dynamics near an avoided level crossing associated with the adiabatic quantum search algorithm, when the system is coupled to a generic environment. At zero temperature, we find that the algorithm remains scalable provided the noise spectral density of the environment decays sufficiently fast at low frequencies. By contrast, higher order scattering processes render the algorithm inefficient at any finite temperature regardless of the spectral density, implying that no quantum speedup can be achieved. Extensions and implications for other adiabatic quantum algorithms will be discussed.

An Estimation of Hybrid Quantum Mechanical Molecular Mechanical Polarization Energies for Small Molecules Using Polarizable Force-Field Approaches

DOE PAGES

Huang, Jing; Mei, Ye; König, Gerhard; ...

2017-01-24

Here in this work, we report two polarizable molecular mechanics (polMM) force field models for estimating the polarization energy in hybrid quantum mechanical molecular mechanical (QM/MM) calculations. These two models, named the potential of atomic charges (PAC) and potential of atomic dipoles (PAD), are formulated from the ab initio quantum mechanical (QM) response kernels for the prediction of the QM density response to an external molecular mechanical (MM) environment (as described by external point charges). The PAC model is similar to fluctuating charge (FQ) models because the energy depends on external electrostatic potential values at QM atomic sites; the PADmore » energy depends on external electrostatic field values at QM atomic sites, resembling induced dipole (ID) models. To demonstrate their uses, we apply the PAC and PAD models to 12 small molecules, which are solvated by TIP3P water. The PAC model reproduces the QM/MM polarization energy with a R 2 value of 0.71 for aniline (in 10,000 TIP3P water configurations) and 0.87 or higher for other eleven solute molecules, while the PAD model has a much better performance with R 2 values of 0.98 or higher. The PAC model reproduces reference QM/MM hydration free energies for 12 solute molecules with a RMSD of 0.59 kcal/mol. The PAD model is even more accurate, with a much smaller RMSD of 0.12 kcal/mol, with respect to the reference. Lastly, this suggests that polarization effects, including both local charge distortion and intramolecular charge transfer, can be well captured by induced dipole type models with proper parametrization.« less

An Estimation of Hybrid Quantum Mechanical Molecular Mechanical Polarization Energies for Small Molecules Using Polarizable Force-Field Approaches.

PubMed

Huang, Jing; Mei, Ye; König, Gerhard; Simmonett, Andrew C; Pickard, Frank C; Wu, Qin; Wang, Lee-Ping; MacKerell, Alexander D; Brooks, Bernard R; Shao, Yihan

2017-02-14

In this work, we report two polarizable molecular mechanics (polMM) force field models for estimating the polarization energy in hybrid quantum mechanical molecular mechanical (QM/MM) calculations. These two models, named the potential of atomic charges (PAC) and potential of atomic dipoles (PAD), are formulated from the ab initio quantum mechanical (QM) response kernels for the prediction of the QM density response to an external molecular mechanical (MM) environment (as described by external point charges). The PAC model is similar to fluctuating charge (FQ) models because the energy depends on external electrostatic potential values at QM atomic sites; the PAD energy depends on external electrostatic field values at QM atomic sites, resembling induced dipole (ID) models. To demonstrate their uses, we apply the PAC and PAD models to 12 small molecules, which are solvated by TIP3P water. The PAC model reproduces the QM/MM polarization energy with a R 2 value of 0.71 for aniline (in 10,000 TIP3P water configurations) and 0.87 or higher for other 11 solute molecules, while the PAD model has a much better performance with R 2 values of 0.98 or higher. The PAC model reproduces reference QM/MM hydration free energies for 12 solute molecules with a RMSD of 0.59 kcal/mol. The PAD model is even more accurate, with a much smaller RMSD of 0.12 kcal/mol, with respect to the reference. This suggests that polarization effects, including both local charge distortion and intramolecular charge transfer, can be well captured by induced dipole type models with proper parametrization.

An Estimation of Hybrid Quantum Mechanical Molecular Mechanical Polarization Energies for Small Molecules Using Polarizable Force-Field Approaches

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

Huang, Jing; Mei, Ye; König, Gerhard

Here in this work, we report two polarizable molecular mechanics (polMM) force field models for estimating the polarization energy in hybrid quantum mechanical molecular mechanical (QM/MM) calculations. These two models, named the potential of atomic charges (PAC) and potential of atomic dipoles (PAD), are formulated from the ab initio quantum mechanical (QM) response kernels for the prediction of the QM density response to an external molecular mechanical (MM) environment (as described by external point charges). The PAC model is similar to fluctuating charge (FQ) models because the energy depends on external electrostatic potential values at QM atomic sites; the PADmore » energy depends on external electrostatic field values at QM atomic sites, resembling induced dipole (ID) models. To demonstrate their uses, we apply the PAC and PAD models to 12 small molecules, which are solvated by TIP3P water. The PAC model reproduces the QM/MM polarization energy with a R 2 value of 0.71 for aniline (in 10,000 TIP3P water configurations) and 0.87 or higher for other eleven solute molecules, while the PAD model has a much better performance with R 2 values of 0.98 or higher. The PAC model reproduces reference QM/MM hydration free energies for 12 solute molecules with a RMSD of 0.59 kcal/mol. The PAD model is even more accurate, with a much smaller RMSD of 0.12 kcal/mol, with respect to the reference. Lastly, this suggests that polarization effects, including both local charge distortion and intramolecular charge transfer, can be well captured by induced dipole type models with proper parametrization.« less

Quantum oscillations in a biaxial pair density wave state.

PubMed

Norman, M R; Davis, J C Séamus

2018-05-22

There has been growing speculation that a pair density wave state is a key component of the phenomenology of the pseudogap phase in the cuprates. Recently, direct evidence for such a state has emerged from an analysis of scanning tunneling microscopy data in halos around the vortex cores. By extrapolation, these vortex halos would then overlap at a magnetic-field scale where quantum oscillations have been observed. Here, we show that a biaxial pair density wave state gives a unique description of the quantum oscillation data, bolstering the case that the pseudogap phase in the cuprates may be a pair density wave state. Copyright © 2018 the Author(s). Published by PNAS.

Vapor-liquid phase equilibria of water modelled by a Kim-Gordon potential

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

Maerzke, Katie A.; McGrath, M. J.; Kuo, I-F W.

2009-09-07

Gibbs ensemble Monte Carlo simulations were carried out to investigate the properties of a frozen-electron-density (or Kim-Gordon, KG) model of water along the vapor-liquid coexistence curve. Because of its theoretical basis, such a KG model provides for seamless coupling to Kohn-Sham density functional theory for use in mixed quantum mechanics/molecular mechanics (QM/MM) implementations. The Gibbs ensemble simulations indicate rather limited transferability of such a simple KG model to other state points. Specifically, a KG model that was parameterized by Barker and Sprik to the properties of liquid water at 300 K, yields saturated vapor pressures and a critical temperature thatmore » are significantly under- and overestimated, respectively. We present a comprehensive density functional theory study to asses the accuracy of two popular exchange correlation functionals on the structure and density of liquid water at ambient conditions This work was supported by the US Department of Energy Office of Basic Energy Science Chemical Sciences Program. Battelle operates Pacific Northwest National Laboratory for the US Department of Energy.« less

Complexity Reduction in Large Quantum Systems: Fragment Identification and Population Analysis via a Local Optimized Minimal Basis

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

Mohr, Stephan; Masella, Michel; Ratcliff, Laura E.

We present, within Kohn-Sham Density Functional Theory calculations, a quantitative method to identify and assess the partitioning of a large quantum mechanical system into fragments. We then introduce a simple and efficient formalism (which can be written as generalization of other well-known population analyses) to extract, from first principles, electrostatic multipoles for these fragments. The corresponding fragment multipoles can in this way be seen as reliable (pseudo-) observables. By applying our formalism within the code BigDFT, we show that the usage of a minimal set of in-situ optimized basis functions is of utmost importance for having at the same timemore » a proper fragment definition and an accurate description of the electronic structure. With this approach it becomes possible to simplify the modeling of environmental fragments by a set of multipoles, without notable loss of precision in the description of the active quantum mechanical region. Furthermore, this leads to a considerable reduction of the degrees of freedom by an effective coarsegraining approach, eventually also paving the way towards efficient QM/QM and QM/MM methods coupling together different levels of accuracy.« less

Tuning the photoluminescence of graphene quantum dots through the charge transfer effect of functional groups.

PubMed

Jin, Sung Hwan; Kim, Da Hye; Jun, Gwang Hoon; Hong, Soon Hyung; Jeon, Seokwoo

2013-02-26

The band gap properties of graphene quantum dots (GQDs) arise from quantum confinement effects and differ from those in semimetallic graphene sheets. Tailoring the size of the band gap and understanding the band gap tuning mechanism are essential for the applications of GQDs in opto-electronics. In this study, we observe that the photoluminescence (PL) of the GQDs shifts due to charge transfers between functional groups and GQDs. GQDs that are functionalized with amine groups and are 1-3 layers thick and less than 5 nm in diameter were successfully fabricated using a two-step cutting process from graphene oxides (GOs). The functionalized GQDs exhibit a redshift of PL emission (ca. 30 nm) compared to the unfunctionalized GQDs. Furthermore, the PL emissions of the GQDs and the amine-functionalized GQDs were also shifted by changes in the pH due to the protonation or deprotonation of the functional groups. The PL shifts resulted from charge transfers between the functional groups and GQDs, which can tune the band gap of the GQDs. Calculations from density functional theory (DFT) are in good agreement with our proposed mechanism for band gap tuning in the GQDs through the use of functionalization.

Complexity Reduction in Large Quantum Systems: Fragment Identification and Population Analysis via a Local Optimized Minimal Basis

DOE PAGES

Mohr, Stephan; Masella, Michel; Ratcliff, Laura E.; ...

2017-07-21

We present, within Kohn-Sham Density Functional Theory calculations, a quantitative method to identify and assess the partitioning of a large quantum mechanical system into fragments. We then introduce a simple and efficient formalism (which can be written as generalization of other well-known population analyses) to extract, from first principles, electrostatic multipoles for these fragments. The corresponding fragment multipoles can in this way be seen as reliable (pseudo-) observables. By applying our formalism within the code BigDFT, we show that the usage of a minimal set of in-situ optimized basis functions is of utmost importance for having at the same timemore » a proper fragment definition and an accurate description of the electronic structure. With this approach it becomes possible to simplify the modeling of environmental fragments by a set of multipoles, without notable loss of precision in the description of the active quantum mechanical region. Furthermore, this leads to a considerable reduction of the degrees of freedom by an effective coarsegraining approach, eventually also paving the way towards efficient QM/QM and QM/MM methods coupling together different levels of accuracy.« less

Exploring the Interaction Natures in Plutonyl (VI) Complexes with Topological Analyses of Electron Density

PubMed Central

Du, Jiguang; Sun, Xiyuan; Jiang, Gang

2016-01-01

The interaction natures between Pu and different ligands in several plutonyl (VI) complexes are investigated by performing topological analyses of electron density. The geometrical structures in both gaseous and aqueous phases are obtained with B3LYP functional, and are generally in agreement with available theoretical and experimental results when combined with all-electron segmented all-electron relativistic contracted (SARC) basis set. The Pu–Oyl bond orders show significant linear dependence on bond length and the charge of oxygen atoms in plutonyl moiety. The closed-shell interactions were identified for Pu-Ligand bonds in most complexes with quantum theory of atoms in molecules (QTAIM) analyses. Meanwhile, we found that some Pu–Ligand bonds, like Pu–OH−, show weak covalent. The interactive nature of Pu–ligand bonds were revealed based on the interaction quantum atom (IQA) energy decomposition approach, and our results indicate that all Pu–Ligand interactions is dominated by the electrostatic attraction interaction as expected. Meanwhile it is also important to note that the quantum mechanical exchange-correlation contributions can not be ignored. By means of the non-covalent interaction (NCI) approach it has been found that some weak and repulsion interactions existed in plutonyl(VI) complexes, which can not be distinguished by QTAIM, can be successfully identified. PMID:27077844

Possible role of interference, protein noise, and sink effects in nonphotochemical quenching in photosynthetic complexes.

PubMed

Berman, Gennady P; Nesterov, Alexander I; Gurvitz, Shmuel; Sayre, Richard T

2017-01-01

We analyze theoretically a simple and consistent quantum mechanical model that reveals the possible role of quantum interference, protein noise, and sink effects in the nonphotochemical quenching (NPQ) in light-harvesting complexes (LHCs). The model consists of a network of five interconnected sites (excitonic states of light-sensitive molecules) responsible for the NPQ mechanism. The model also includes the "damaging" and the dissipative channels. The damaging channel is responsible for production of singlet oxygen and other destructive outcomes. In our model, both damaging and "dissipative" charge transfer channels are described by discrete electron energy levels attached to their sinks, that mimic the continuum part of electron energy spectrum. All five excitonic sites interact with the protein environment that is modeled using a stochastic process. Our approach allowed us to derive the exact and closed system of linear ordinary differential equations for the reduced density matrix and its first momentums. These equations are solved numerically including for strong interactions between the light-sensitive molecules and protein environment. As an example, we apply our model to demonstrate possible contributions of quantum interference, protein noise, and sink effects in the NPQ mechanism in the CP29 minor LHC. The numerical simulations show that using proper combination of quantum interference effects, properties of noise, and sinks, one can significantly suppress the damaging channel. Our findings demonstrate the possible role of interference, protein noise, and sink effects for modeling, engineering, and optimizing the performance of the NPQ processes in both natural and artificial light-harvesting complexes.

Possible role of interference, protein noise, and sink effects in nonphotochemical quenching in photosynthetic complexes

DOE PAGES

Berman, Gennady P.; Nesterov, Alexander I.; Gurvitz, Shmuel; ...

2016-04-30

Here, we analyze theoretically a simple and consistent quantum mechanical model that reveals the possible role of quantum interference, protein noise, and sink effects in the nonphotochemical quenching (NPQ) in light-harvesting complexes (LHCs). The model consists of a network of five interconnected sites (excitonic states of light-sensitive molecules) responsible for the NPQ mechanism. The model also includes the “damaging” and the dissipative channels. The damaging channel is responsible for production of singlet oxygen and other destructive outcomes. In this model, both damaging and “dissipative” charge transfer channels are described by discrete electron energy levels attached to their sinks, that mimicmore » the continuum part of electron energy spectrum. All five excitonic sites interact with the protein environment that is modeled using a stochastic process. Our approach allowed us to derive the exact and closed system of linear ordinary differential equations for the reduced density matrix and its first momentums. Moreover, these equations are solved numerically including for strong interactions between the light-sensitive molecules and protein environment. As an example, we apply our model to demonstrate possible contributions of quantum interference, protein noise, and sink effects in the NPQ mechanism in the CP29 minor LHC. The numerical simulations show that using proper combination of quantum interference effects, properties of noise, and sinks, one can significantly suppress the damaging channel. Finally, our findings demonstrate the possible role of interference, protein noise, and sink effects for modeling, engineering, and optimizing the performance of the NPQ processes in both natural and artificial light-harvesting complexes.« less

Novel Principles and the Charge-Symmetric Design of Dirac's Quantum Mechanics: I. Enhanced Eriksen's Theorem and the Universal Charge-Index Formalism for Dirac's Equation in (Strong) External Static Fields

NASA Astrophysics Data System (ADS)

Kononets, Yu. V.

2016-12-01

The presented enhanced version of Eriksen's theorem defines an universal transform of the Foldy-Wouthuysen type and in any external static electromagnetic field (ESEMF) reveals a discrete symmetry of Dirac's equation (DE), responsible for existence of a highly influential conserved quantum number—the charge index distinguishing two branches of DE spectrum. It launches the charge-index formalism (CIF) obeying the charge-index conservation law (CICL). Via its unique ability to manipulate each spectrum branch independently, the CIF creates a perfect charge-symmetric architecture of Dirac's quantum mechanics (DQM), which resolves all the riddles of the standard DE theory (SDET). Besides the abstract CIF algebra, the paper discusses: (1) the novel accurate charge-symmetric definition of the electric-current density; (2) DE in the true-particle representation, where electrons and positrons coexist on equal footing; (3) flawless "natural" scheme of second quantization; and (4) new physical grounds for the Fermi-Dirac statistics. As a fundamental quantum law, the CICL originates from the kinetic-energy sign conservation and leads to a novel single-particle physics in strong-field situations. Prohibiting Klein's tunneling (KT) in Klein's zone via the CICL, the precise CIF algebra defines a new class of weakly singular DE solutions, strictly confined in the coordinate space and experiencing the total reflection from the potential barrier.

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.

Positive spaces, generalized semi-densities, and quantum interactions

NASA Astrophysics Data System (ADS)

Canarutto, Daniel

2012-03-01

The basics of quantum particle physics on a curved Lorentzian background are expressed in a formulation which has original aspects and exploits some non-standard mathematical notions. In particular, positive spaces and generalized semi-densities (in a distributional sense) are shown to link, in a natural way, discrete multi-particle spaces to distributional bundles of quantum states. The treatment of spinor and boson fields is partly original also from an algebraic point of view and suggests a non-standard approach to quantum interactions. The case of electroweak interactions provides examples.

Minimized open-circuit voltage reduction in GaAs/InGaAs quantum well solar cells with bandgap-engineered graded quantum well depths

NASA Astrophysics Data System (ADS)

Li, Xiaohan; Dasika, Vaishno D.; Li, Ping-Chun; Ji, Li; Bank, Seth R.; Yu, Edward T.

2014-09-01

The use of InGaAs quantum wells with composition graded across the intrinsic region to increase open-circuit voltage in p-i-n GaAs/InGaAs quantum well solar cells is demonstrated and analyzed. By engineering the band-edge energy profile to reduce photo-generated carrier concentration in the quantum wells at high forward bias, simultaneous increases in both open-circuit voltage and short-circuit current density are achieved, compared to those for a structure with the same average In concentration, but constant rather than graded quantum well composition across the intrinsic region. This approach is combined with light trapping to further increase short-circuit current density.

A wave function for stock market returns

NASA Astrophysics Data System (ADS)

Ataullah, Ali; Davidson, Ian; Tippett, Mark

2009-02-01

The instantaneous return on the Financial Times-Stock Exchange (FTSE) All Share Index is viewed as a frictionless particle moving in a one-dimensional square well but where there is a non-trivial probability of the particle tunneling into the well’s retaining walls. Our analysis demonstrates how the complementarity principle from quantum mechanics applies to stock market prices and of how the wave function presented by it leads to a probability density which exhibits strong compatibility with returns earned on the FTSE All Share Index. In particular, our analysis shows that the probability density for stock market returns is highly leptokurtic with slight (though not significant) negative skewness. Moreover, the moments of the probability density determined under the complementarity principle employed here are all convergent - in contrast to many of the probability density functions on which the received theory of finance is based.

Nuclear magnetic resonance studies of quadrupolar nuclei and dipolar field effects

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

Urban, Jeffry Todd

Experimental and theoretical research conducted in two areas in the field of nuclear magnetic resonance (NMR) spectroscopy is presented: (1) studies of the coherent quantum-mechanical control of the angular momentum dynamics of quadrupolar (spin I > 1/2) nuclei and its application to the determination of molecular structure; and (2) applications of the long-range nuclear dipolar field to novel NMR detection methodologies.The dissertation is organized into six chapters. The first two chapters and associated appendices are intended to be pedagogical and include an introduction to the quantum mechanical theory of pulsed NMR spectroscopy and the time dependent theory of quantum mechanics.more » The third chapter describes investigations of the solid-state multiple-quantum magic angle spinning (MQMAS) NMR experiment applied to I = 5/2 quadrupolar nuclei. This work reports the use of rotary resonance-matched radiofrequency irradiation for sensitivity enhancement of the I = 5/2 MQMAS experiment. These experiments exhibited certain selective line narrowing effects which were investigated theoretically.The fourth chapter extends the discussion of multiple quantum spectroscopy of quadrupolar nuclei to a mostly theoretical study of the feasibility of enhancing the resolution of nitrogen-14 NMR of large biomolecules in solution via double-quantum spectroscopy. The fifth chapter continues to extend the principles of multiple quantum NMR spectroscopy of quadrupolar nuclei to make analogies between experiments in NMR/nuclear quadrupolar resonance (NQR) and experiments in atomic/molecular optics (AMO). These analogies are made through the Hamiltonian and density operator formalism of angular momentum dynamics in the presence of electric and magnetic fields.The sixth chapter investigates the use of the macroscopic nuclear dipolar field to encode the NMR spectrum of an analyte nucleus indirectly in the magnetization of a sensor nucleus. This technique could potentially serve as an encoding module for the recently developed NMR remote detection experiment. The feasibility of using hyperpolarized xenon-129 gas as a sensor is discussed. This work also reports the use of an optical atomic magnetometer to detect the nuclear magnetization of Xe-129 gas, which has potential applicability as a detection module for NMR remote detection experiments.« less

Reaction mechanism of Ru(II) piano-stool complexes: umbrella sampling QM/MM MD study.

PubMed

Futera, Zdeněk; Burda, Jaroslav V

2014-07-15

Biologically relevant interactions of piano-stool ruthenium(II) complexes with ds-DNA are studied in this article by hybrid quantum mechanics-molecular mechanics (QM/MM) computational technique. The whole reaction mechanism is divided into three phases: (i) hydration of the [Ru(II) (η(6) -benzene)(en)Cl](+) complex, (ii) monoadduct formation between the resulting aqua-Ru(II) complex and N7 position of one of the guanines in the ds-DNA oligomer, and (iii) formation of the intrastrand Ru(II) bridge (cross-link) between two adjacent guanines. Free energy profiles of all the reactions are explored by QM/MM MD umbrella sampling approach where the Ru(II) complex and two guanines represent a quantum core, which is described by density functional theory methods. The combined QM/MM scheme is realized by our own software, which was developed to couple several quantum chemical programs (in this study Gaussian 09) and Amber 11 package. Calculated free energy barriers of the both ruthenium hydration and Ru(II)-N7(G) DNA binding process are in good agreement with experimentally measured rate constants. Then, this method was used to study the possibility of cross-link formation. One feasible pathway leading to Ru(II) guanine-guanine cross-link with synchronous releasing of the benzene ligand is predicted. The cross-linking is an exergonic process with the energy barrier lower than for the monoadduct reaction of Ru(II) complex with ds-DNA. Copyright © 2014 Wiley Periodicals, Inc.

Emerging interpretations of quantum mechanics and recent progress in quantum measurement

NASA Astrophysics Data System (ADS)

Clarke, M. L.

2014-01-01

The focus of this paper is to provide a brief discussion on the quantum measurement process, by reviewing select examples highlighting recent progress towards its understanding. The areas explored include an outline of the measurement problem, the standard interpretation of quantum mechanics, quantum to classical transition, types of measurement (including weak and projective measurements) and newly emerging interpretations of quantum mechanics (decoherence theory, objective reality, quantum Darwinism and quantum Bayesianism).

Ab initio Computations of the Electronic, Mechanical, and Thermal Properties of Ultra High Temperature Ceramics (UHTC) ZrB2 and HfB2

NASA Technical Reports Server (NTRS)

Lawson, John W.; Bauschlicher, Charles W.; Daw, Murray

2011-01-01

Refractory materials such as metallic borides, often considered as ultra high temperature ceramics (UHTC), are characterized by high melting point, high hardness, and good chemical inertness. These materials have many applications which require high temperature materials that can operate with no or limited oxidation. Ab initio, first principles methods are the most accurate modeling approaches available and represent a parameter free description of the material based on the quantum mechanical equations. Using these methods, many of the intrinsic properties of these material can be obtained. We performed ab initio calculations based on density functional theory for the UHTC materials ZrB2 and HfB2. Computational results are presented for structural information (lattice constants, bond lengths, etc), electronic structure (bonding motifs, densities of states, band structure, etc), thermal quantities (phonon spectra, phonon densities of states, specific heat), as well as information about point defects such as vacancy and antisite formation energies.

Transfer of Learning in Quantum Mechanics

NASA Astrophysics Data System (ADS)

Singh, Chandralekha

2005-09-01

We investigate the difficulties that undergraduate students in quantum mechanics courses have in transferring learning from previous courses or within the same course from one context to another by administering written tests and conducting individual interviews. Quantum mechanics is abstract and its paradigm is very different from the classical one. A good grasp of the principles of quantum mechanics requires creating and organizing a knowledge structure consistent with the quantum postulates. Previously learned concepts such as the principle of superposition and probability can be useful in quantum mechanics if students are given opportunity to build associations between new and prior knowledge. We also discuss the need for better alignment between quantum mechanics and modern physics courses taken previously because semi-classical models can impede internalization of the quantum paradigm in more advanced courses.

Dimensionality of nanoscale TiO 2 determines the mechanism of photoinduced electron injection from a CdSe nanoparticle

DOE PAGES

Tafen, De Nyago; Long, Run; Prezhdo, Oleg V.

2014-03-10

Assumptions about electron transfer (ET) mechanisms guide design of catalytic, photovoltaic, and electronic systems. We demonstrate that the mechanism of ET from a CdSe quantum dot (QD) into nanoscale TiO 2 depends on TiO 2 dimensionality. The injection into a TiO 2 QD is adiabatic due to strong donor–acceptor coupling, arising from unsaturated chemical bonds on the QD surface, and low density of acceptor states. In contrast, the injection into a TiO 2 nanobelt (NB) is nonadiabatic, because the state density is high, the donor–acceptor coupling is weak, and multiple phonons accommodate changes in the electronic energy. The CdSe adsorbantmore » breaks symmetry of delocalized TiO 2 NB states, relaxing coupling selection rules, and generating more ET channels. Both mechanisms can give efficient ultrafast injection. Furthermore, the dependence on system properties is very different for the two mechanisms, demonstrating that the fundamental principles leading to efficient charge separation depend strongly on the type of nanoscale material.« less

Dimensionality of nanoscale TiO 2 determines the mechanism of photoinduced electron injection from a CdSe nanoparticle

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

Tafen, De Nyago; Long, Run; Prezhdo, Oleg V.

Assumptions about electron transfer (ET) mechanisms guide design of catalytic, photovoltaic, and electronic systems. We demonstrate that the mechanism of ET from a CdSe quantum dot (QD) into nanoscale TiO 2 depends on TiO 2 dimensionality. The injection into a TiO 2 QD is adiabatic due to strong donor–acceptor coupling, arising from unsaturated chemical bonds on the QD surface, and low density of acceptor states. In contrast, the injection into a TiO 2 nanobelt (NB) is nonadiabatic, because the state density is high, the donor–acceptor coupling is weak, and multiple phonons accommodate changes in the electronic energy. The CdSe adsorbantmore » breaks symmetry of delocalized TiO 2 NB states, relaxing coupling selection rules, and generating more ET channels. Both mechanisms can give efficient ultrafast injection. Furthermore, the dependence on system properties is very different for the two mechanisms, demonstrating that the fundamental principles leading to efficient charge separation depend strongly on the type of nanoscale material.« less

Spectral density of mixtures of random density matrices for qubits

NASA Astrophysics Data System (ADS)

Zhang, Lin; Wang, Jiamei; Chen, Zhihua

2018-06-01

We derive the spectral density of the equiprobable mixture of two random density matrices of a two-level quantum system. We also work out the spectral density of mixture under the so-called quantum addition rule. We use the spectral densities to calculate the average entropy of mixtures of random density matrices, and show that the average entropy of the arithmetic-mean-state of n qubit density matrices randomly chosen from the Hilbert-Schmidt ensemble is never decreasing with the number n. We also get the exact value of the average squared fidelity. Some conjectures and open problems related to von Neumann entropy are also proposed.

Quantum thermodynamic cycles and quantum heat engines. II.

PubMed

Quan, H T

2009-04-01

We study the quantum-mechanical generalization of force or pressure, and then we extend the classical thermodynamic isobaric process to quantum-mechanical systems. Based on these efforts, we are able to study the quantum version of thermodynamic cycles that consist of quantum isobaric processes, such as the quantum Brayton cycle and quantum Diesel cycle. We also consider the implementation of the quantum Brayton cycle and quantum Diesel cycle with some model systems, such as single particle in a one-dimensional box and single-mode radiation field in a cavity. These studies lay the microscopic (quantum-mechanical) foundation for Szilard-Zurek single-molecule engine.

Hybrid reconstruction of quantum density matrix: when low-rank meets sparsity

NASA Astrophysics Data System (ADS)

Li, Kezhi; Zheng, Kai; Yang, Jingbei; Cong, Shuang; Liu, Xiaomei; Li, Zhaokai

2017-12-01

Both the mathematical theory and experiments have verified that the quantum state tomography based on compressive sensing is an efficient framework for the reconstruction of quantum density states. In recent physical experiments, we found that many unknown density matrices in which people are interested in are low-rank as well as sparse. Bearing this information in mind, in this paper we propose a reconstruction algorithm that combines the low-rank and the sparsity property of density matrices and further theoretically prove that the solution of the optimization function can be, and only be, the true density matrix satisfying the model with overwhelming probability, as long as a necessary number of measurements are allowed. The solver leverages the fixed-point equation technique in which a step-by-step strategy is developed by utilizing an extended soft threshold operator that copes with complex values. Numerical experiments of the density matrix estimation for real nuclear magnetic resonance devices reveal that the proposed method achieves a better accuracy compared to some existing methods. We believe that the proposed method could be leveraged as a generalized approach and widely implemented in the quantum state estimation.

Atomic quantum corrals for Bose-Einstein condensates

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

Xiong Hongwei; Kavli Institute for Theoretical Physics China, Chinese Academy of Sciences, Beijing 100190; Wu Biao

2010-11-15

We consider the dynamics of Bose-Einstein condensates in a corral-like potential. Compared to the electronic quantum corrals, the atomic quantum corrals have the advantages of allowing direct and convenient observation of the wave dynamics, together with adjustable interaction strength. Our numerical study shows that these advantages not only allow exploration of the rich dynamical structures in the density distribution but also make the corrals useful in many other aspects. In particular, the corrals for atoms can be arranged into a stadium shape for the experimental visualization of quantum chaos, which has been elusive with electronic quantum corrals. The density correlationmore » is used to describe quantitatively the dynamical quantum chaos. Furthermore, we find that the interatomic interaction can greatly enhance the dynamical quantum chaos, for example, inducing a chaotic behavior even in circle-shaped corrals.« less

Quantum State Tomography via Reduced Density Matrices.

PubMed

Xin, Tao; Lu, Dawei; Klassen, Joel; Yu, Nengkun; Ji, Zhengfeng; Chen, Jianxin; Ma, Xian; Long, Guilu; Zeng, Bei; Laflamme, Raymond

2017-01-13

Quantum state tomography via local measurements is an efficient tool for characterizing quantum states. However, it requires that the original global state be uniquely determined (UD) by its local reduced density matrices (RDMs). In this work, we demonstrate for the first time a class of states that are UD by their RDMs under the assumption that the global state is pure, but fail to be UD in the absence of that assumption. This discovery allows us to classify quantum states according to their UD properties, with the requirement that each class be treated distinctly in the practice of simplifying quantum state tomography. Additionally, we experimentally test the feasibility and stability of performing quantum state tomography via the measurement of local RDMs for each class. These theoretical and experimental results demonstrate the advantages and possible pitfalls of quantum state tomography with local measurements.

Probability and Locality: Determinism Versus Indeterminism in Quantum Mechanics

NASA Astrophysics Data System (ADS)

Dickson, William Michael

1995-01-01

Quantum mechanics is often taken to be necessarily probabilistic. However, this view of quantum mechanics appears to be more the result of historical accident than of careful analysis. Moreover, quantum mechanics in its usual form faces serious problems. Although the mathematical core of quantum mechanics--quantum probability theory- -does not face conceptual difficulties, the application of quantum probability to the physical world leads to problems. In particular, quantum mechanics seems incapable of describing our everyday macroscopic experience. Therefore, several authors have proposed new interpretations --including (but not limited to) modal interpretations, spontaneous localization interpretations, the consistent histories approach, and the Bohm theory--each of which deals with quantum-mechanical probabilities differently. Each of these interpretations promises to describe our macroscopic experience and, arguably, each succeeds. Is there any way to compare them? Perhaps, if we turn to another troubling aspect of quantum mechanics, non-locality. Non -locality is troubling because prima facie it threatens the compatibility of quantum mechanics with special relativity. This prima facie threat is mitigated by the no-signalling theorems in quantum mechanics, but nonetheless one may find a 'conflict of spirit' between nonlocality in quantum mechanics and special relativity. Do any of these interpretations resolve this conflict of spirit?. There is a strong relation between how an interpretation deals with quantum-mechanical probabilities and how it deals with non-locality. The main argument here is that only a completely deterministic interpretation can be completely local. That is, locality together with the empirical predictions of quantum mechanics (specifically, its strict correlations) entails determinism. But even with this entailment in hand, comparison of the various interpretations requires a look at each, to see how non-locality arises, or in the case of deterministic interpretations, whether it arises. The result of this investigation is that, at the least, deterministic interpretations are no worse off with respect to special relativity than indeterministic interpretations. This conclusion runs against a common view that deterministic interpretations, specifically the Bohm theory, have more difficulty with special relativity than other interpretations.

Conceptual Foundations of Quantum Mechanics:. the Role of Evidence Theory, Quantum Sets, and Modal Logic

NASA Astrophysics Data System (ADS)

Resconi, Germano; Klir, George J.; Pessa, Eliano

Recognizing that syntactic and semantic structures of classical logic are not sufficient to understand the meaning of quantum phenomena, we propose in this paper a new interpretation of quantum mechanics based on evidence theory. The connection between these two theories is obtained through a new language, quantum set theory, built on a suggestion by J. Bell. Further, we give a modal logic interpretation of quantum mechanics and quantum set theory by using Kripke's semantics of modal logic based on the concept of possible worlds. This is grounded on previous work of a number of researchers (Resconi, Klir, Harmanec) who showed how to represent evidence theory and other uncertainty theories in terms of modal logic. Moreover, we also propose a reformulation of the many-worlds interpretation of quantum mechanics in terms of Kripke's semantics. We thus show how three different theories — quantum mechanics, evidence theory, and modal logic — are interrelated. This opens, on one hand, the way to new applications of quantum mechanics within domains different from the traditional ones, and, on the other hand, the possibility of building new generalizations of quantum mechanics itself.

Plasticity and Kinky Chemistry of Carbon Nanotubes

NASA Technical Reports Server (NTRS)

Srivastava, Deepak; Dzegilenko, Fedor

2000-01-01

Since their discovery in 1991, carbon nanotubes have been the subject of intense research interest based on early predictions of their unique mechanical, electronic, and chemical properties. Materials with the predicted unique properties of carbon nanotubes are of great interest for use in future generations of aerospace vehicles. For their structural properties, carbon nanotubes could be used as reinforcing fibers in ultralight multifunctional composites. For their electronic properties, carbon nanotubes offer the potential of very high-speed, low-power computing elements, high-density data storage, and unique sensors. In a continuing effort to model and predict the properties of carbon nanotubes, Ames accomplished three significant results during FY99. First, accurate values of the nanomechanics and plasticity of carbon nanotubes based on quantum molecular dynamics simulations were computed. Second, the concept of mechanical deformation catalyzed-kinky-chemistry as a means to control local chemistry of nanotubes was discovered. Third, the ease of nano-indentation of silicon surfaces with carbon nanotubes was established. The elastic response and plastic failure mechanisms of single-wall nanotubes were investigated by means of quantum molecular dynamics simulations.

Surface Morphology Evolution Mechanisms of InGaN/GaN Multiple Quantum Wells with Mixture N2/H2-Grown GaN Barrier.

PubMed

Zhou, Xiaorun; Lu, Taiping; Zhu, Yadan; Zhao, Guangzhou; Dong, Hailiang; Jia, Zhigang; Yang, Yongzhen; Chen, Yongkang; Xu, Bingshe

2017-12-01

Surface morphology evolution mechanisms of InGaN/GaN multiple quantum wells (MQWs) during GaN barrier growth with different hydrogen (H 2 ) percentages have been systematically studied. Ga surface-diffusion rate, stress relaxation, and H 2 etching effect are found to be the main affecting factors of the surface evolution. As the percentage of H 2 increases from 0 to 6.25%, Ga surface-diffusion rate and the etch effect are gradually enhanced, which is beneficial to obtaining a smooth surface with low pits density. As the H 2 proportion further increases, stress relaxation and H 2 over- etching effect begin to be the dominant factors, which degrade surface quality. Furthermore, the effects of surface evolution on the interface and optical properties of InGaN/GaN MQWs are also profoundly discussed. The comprehensive study on the surface evolution mechanisms herein provides both technical and theoretical support for the fabrication of high-quality InGaN/GaN heterostructures.

Mechanism of nuclear spin initiated para-H2 to ortho-H2 conversion.

PubMed

Buntkowsky, G; Walaszek, B; Adamczyk, A; Xu, Y; Limbach, H-H; Chaudret, B

2006-04-28

In this paper a quantitative explanation for a diamagnetic ortho/para H2 conversion is given. The description is based on the quantum-mechanical density matrix formalism originally developed by Alexander and Binsch for studies of exchange processes in NMR spectra. Only the nuclear spin system is treated quantum-mechanically. Employing the model of a three spin system, the reactions of the hydrogen gas with the catalysts are treated as a phenomenological rate process, described by a rate constant. Numerical calculations reveal that for nearly all possible geometrical arrangements of the three spin system an efficient spin conversion is obtained. Only in the chemically improbable case of a linear group H-X-H no spin conversion is obtained. The efficiency of the spin conversion depends strongly on the lifetime of the H-X-H complex and on the presence of exchange interactions between the two hydrogens. Even moderate exchange couplings cause a quench of the spin conversion. Thus a sufficiently strong binding of the dihydrogen to the S spin is necessary to render the quenching by the exchange interaction ineffective.

Trapped Inflation

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

Green, Daniel; Horn, Bart; /SLAC /Stanford U., Phys. Dept.

2009-06-19

We analyze a distinctive mechanism for inflation in which particle production slows down a scalar field on a steep potential, and show how it descends from angular moduli in string compactifications. The analysis of density perturbations - taking into account the integrated effect of the produced particles and their quantum fluctuations - requires somewhat new techniques that we develop. We then determine the conditions for this effect to produce sixty e-foldings of inflation with the correct amplitude of density perturbations at the Gaussian level, and show that these requirements can be straightforwardly satisfied. Finally, we estimate the amplitude of themore » non-Gaussianity in the power spectrum and find a significant equilateral contribution.« less

Auger heating of carriers in {GaAs}/{AlAs} heterostructures

NASA Astrophysics Data System (ADS)

Borri, P.; Ceccherini, S.; Gurioli, M.; Bogani, F.

1997-07-01

The photoluminescence of {GaAs}/{AlAs} multiple quantum wells structures under optical ps excitation is investigated for carrier densities in the range 10 18-4 × 10 19 cm -3 with frequency and time-resolved spectroscopic techniques. The measurements give a direct evidence of the occurrence in the sample of carrier heating. This energy up-conversion gives rise to photoluminescence from the states near the Fermi level whose intensity and time evolution depend on the carrier density in a strongly non-linear way. The observed behaviour can be explained introducing in the carrier dynamics an up-conversion mechanism due to Auger-like processes.

Quantum description of a field in macroscopic electrodynamics and photon properties in transparent media

NASA Astrophysics Data System (ADS)

Toptygin, I. N.

2017-12-01

Applying a quantum mechanical treatment to a high-frequency macroscopic electromagnetic field and radiative phenomena in a medium, we construct quantum operators for energy-momentum tensor components in dispersive media and find their eigenvalues, which are different in the Minkowski and Abraham representations. It is shown that the photon momentum in a medium resulting from the quantization of the vector potential differs from that defined from Abraham’s symmetric energy-momentum-tensor but is equal to the momentum defined from the Minkowski tensor. A similar result is obtained by calculating the intrinsic angular momentum (spin) of an electro-magnetic field in the medium. Only the Minkowski tensor leads to the experimentally confirmed spin values that are multiples of ħ, providing the grounds for choosing the Minkowski representation as the proper form for the momentum density of a transverse electromagnetic field in a transparent medium, in both classical and quantum descriptions of the field. The Abraham representation is unsuitable for this purpose and leads to contradictions. The conclusion drawn does not apply to quasistatic and static fields.

One-Step Synthesis of Boron Nitride Quantum Dots: Simple Chemistry Meets Delicate Nanotechnology.

PubMed

Liu, Bingping; Yan, Shihai; Song, Zhongqian; Liu, Mengli; Ji, Xuqiang; Yang, Wenrong; Liu, Jingquan

2016-12-23

Herein, a conceptually new and straightforward aqueous route is described for the synthesis of hydroxyl- and amino-functionalized boron nitride quantum dots (BNQDs) with quantum yields (QY) as high as 18.3 % by using a facile bottom-up approach, in which a mixture of boric acid and ammonia solution was hydrothermally treated in one pot at 200 °C for 12 h. The functionalized BNQDs, with excellent photoluminescence properties, could be easily dispersed in an aqueous medium and applied as fluorescent probes for the detection of ferrous (Fe 2+ ) and ferric (Fe 3+ ) ions with excellent selectivity and low detection limits. The mechanisms for the hydrothermal reaction and fluorescence quenching were also simulated by using density functional theory (DFT), which confirmed the feasibility and advantages of this strategy. It provides a scalable and eco-friendly method for preparation of BNQDs with good dispersability and could also be generalized to the synthesis of other 2D quantum dots and nanoplates. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Exotic ferromagnetism in the two-dimensional quantum material C3N

NASA Astrophysics Data System (ADS)

Huang, Wen-Cheng; Li, Wei; Liu, Xiaosong

2018-04-01

The search for and study of exotic quantum states in novel low-dimensional quantum materials have triggered extensive research in recent years. Here, we systematically study the electronic and magnetic structures in the newly discovered two-dimensional quantum material C3N within the framework of density functional theory. The calculations demonstrate that C3N is an indirect-band semiconductor with an energy gap of 0.38 eV, which is in good agreement with experimental observations. Interestingly, we find van Hove singularities located at energies near the Fermi level, which is half that of graphene. Thus, the Fermi energy easily approaches that of the singularities, driving the system to ferromagnetism, under charge carrier injection, such as electric field gating or hydrogen doping. These findings not only demonstrate that the emergence of magnetism stems from the itinerant electron mechanism rather than the effects of local magnetic impurities, but also open a new avenue to designing field-effect transistor devices for possible realization of an insulator-ferromagnet transition by tuning an external electric field.

Terahertz response in the quantum-Hall-effect regime of a quantum-well-based charge-sensitive infrared phototransistor

NASA Astrophysics Data System (ADS)

Nakagawa, Daisuke; Takizawa, Kazuhiro; Ikushima, Kenji; Kim, Sunmi; Patrashin, Mikhail; Hosako, Iwao; Komiyama, Susumu

2018-04-01

The characteristics of a charge-sensitive infrared phototransistor (CSIP) based on a GaAs/AlGaAs multiple quantum-well (QW) structure are studied under a magnetic field. In the CSIP, the upper QWs serve as a floating gate that is charged by photoexcitation. The photoinduced charges are detected using the resistance of the lowest QW conducting channel. The conducting channel exhibits the integer quantum Hall effect (QHE) in a perpendicular high magnetic field, yielding the magnetic field dependence of the terahertz (THz) response ΔR. We found two different features of ΔR. One is that ΔR switches sign across the QHE plateau, which is explained simply by an increased electron density in the conducting channel. The other feature is observed as an enhanced positive ΔR when a potential barrier is formed in the conducting channel. The latter mechanism can be interpreted as the promotion of edge/bulk scattering due to photoinduced charges. These findings suggest ways to enhance the THz response by using magnetic fields and potential barriers.

A New Ontological View of the Quantum Measurement Problem

DTIC Science & Technology

2005-06-13

broader issues in the foundations of quantum mechanics as well. In this scenario, a quantum measurement is a nonequilibrium phase transition in a...the foundations of quantum mechan - ics as well. In this scenario a quantum measurement is a non-equilibrium phase transition in a “resonant cavity...ontology, and the probabilistic element is removed from the foundations of quantum mechanics , its apparent presence in the quantum measurement being solely

Exciton and intracenter radiative recombination in ZnMnTe and CdMnTe quantum wells with optically active manganese ions

NASA Astrophysics Data System (ADS)

Agekyan, V. F.; Akai, I.; Vasil'Ev, N. N.; Karasawa, T.; Karczewski, G.; Serov, A. Yu.; Filosofov, N. G.

2007-06-01

The emission spectra of Zn1-x Mn x Te/Zn0.6Mg0.4Te and Cd1-x Mn x Te/Cd0.5Mg0.5Te quantum-well structures with different manganese concentrations and quantum-well widths are studied at excitation power densities ranging from 105 to 107 W cm-2. Under strong optical pumping, intracenter luminescence of Mn2+ ions degrades as a result of the interaction of excited managanese ions with high-density excitons. This process is accompanied by a strong broadening of the emission band of quantum-well excitons due to the exciton-exciton interaction and saturation of the exciton ground state. Under pumping at a power density of 105 W cm-2, stimulated emission of quantum-well excitons arises in CdTe/Cd0.5Mg0.5Te. The luminescence kinetics of the quantum-well and barrier excitons is investigated with a high temporal resolution. The effect of the quantum-well width and the managanese concentration on the kinetics and band shape of the Mn2+ intracenter luminescence characterized by the contribution of the manganese interface ions is determined.

Anisotropy-driven transition from the Moore-Read state to quantum Hall stripes

NASA Astrophysics Data System (ADS)

Zhu, Zheng; Sodemann, Inti; Sheng, D. N.; Fu, Liang

2017-05-01

We investigate the nature of the quantum Hall liquid in a half-filled second Landau level (n =1 ) as a function of band mass anisotropy using numerical exact diagonalization and density matrix renormalization group methods. We find increasing the mass anisotropy induces a quantum phase transition from the Moore-Read state to a charge density wave state. By analyzing the energy spectrum, guiding center structure factors, and by adding weak pinning potentials, we show that this charge density wave is a unidirectional quantum Hall stripe, which has a periodicity of a few magnetic lengths and survives in the thermodynamic limit. We find smooth profiles for the guiding center occupation function that reveal the strong coupling nature of the array of chiral Luttinger liquids residing at the stripe edges.

Quantum Stress: Density Functional Theory Formulation and Physical Manifestation

NASA Astrophysics Data System (ADS)

Hu, Hao; Liu, Feng

2012-02-01

The concept of ``quantum stress (QS)'' is introduced and formulated within density functional theory (DFT), to underlie extrinsic electronic effects on the stress state of solids and thin films in the absence of lattice strain. An explicit expression of QS (σ^Q) is derived in relation to the deformation potential of electronic states (ξ) and the variation of electron density (δn), σ^Q=ξ(δn), as a quantum analog of classical Hook's law. Two distinct QS manifestations are demonstrated quantitatively by DFT calculations: (1) in the form of bulk stress induced by charge carriers; and (2) in the form of surface stress induced by quantum confinement. QS has broad implications in physical phenomena and technological applications that are based on coupling of electronic structure with lattice strain.

A multilayered-representation quantum mechanical/molecular mechanics study of the SN2 reaction of CH3Br + OH- in aqueous solution

NASA Astrophysics Data System (ADS)

Xu, Yulong; Wang, Tingting; Wang, Dunyou

2012-11-01

The bimolecular nucleophilic substitution (SN2) reaction of CH3Br and OH- in aqueous solution was investigated using a multilayered-representation quantum mechanical and molecular mechanics methodology. Reactant complex, transition state, and product complex are identified and characterized in aqueous solution. The potentials of mean force are computed under both the density function theory and coupled-cluster single double (triple) (CCSD(T)) levels of theory for the reaction region. The results show that the aqueous environment has a significant impact on the reaction process. The solvation effect and the polarization effect combined raise the activation barrier height by ˜16.2 kcal/mol and the solvation effect is the dominant contribution to the potential of mean force. The CCSD(T)/MM representation presents a free energy activation barrier height of 22.8 kcal/mol and the rate constant at 298 K of 3.7 × 10-25 cm3 molecule-1 s-1 which agree very well with the experiment values at 23.0 kcal/mol and 2.6 × 10-25 cm3 molecule-1 s-1, respectively.

Quantum-coherent coupling of a mechanical oscillator to an optical cavity mode.

PubMed

Verhagen, E; Deléglise, S; Weis, S; Schliesser, A; Kippenberg, T J

2012-02-01

Optical laser fields have been widely used to achieve quantum control over the motional and internal degrees of freedom of atoms and ions, molecules and atomic gases. A route to controlling the quantum states of macroscopic mechanical oscillators in a similar fashion is to exploit the parametric coupling between optical and mechanical degrees of freedom through radiation pressure in suitably engineered optical cavities. If the optomechanical coupling is 'quantum coherent'--that is, if the coherent coupling rate exceeds both the optical and the mechanical decoherence rate--quantum states are transferred from the optical field to the mechanical oscillator and vice versa. This transfer allows control of the mechanical oscillator state using the wide range of available quantum optical techniques. So far, however, quantum-coherent coupling of micromechanical oscillators has only been achieved using microwave fields at millikelvin temperatures. Optical experiments have not attained this regime owing to the large mechanical decoherence rates and the difficulty of overcoming optical dissipation. Here we achieve quantum-coherent coupling between optical photons and a micromechanical oscillator. Simultaneously, coupling to the cold photon bath cools the mechanical oscillator to an average occupancy of 1.7 ± 0.1 motional quanta. Excitation with weak classical light pulses reveals the exchange of energy between the optical light field and the micromechanical oscillator in the time domain at the level of less than one quantum on average. This optomechanical system establishes an efficient quantum interface between mechanical oscillators and optical photons, which can provide decoherence-free transport of quantum states through optical fibres. Our results offer a route towards the use of mechanical oscillators as quantum transducers or in microwave-to-optical quantum links.

Existence of dark matter with observed properties of cosmic microwave background radiation substantiates three conservation laws of classical physics and all principles of quantum mechanics as creates the value of Planck’s constant

NASA Astrophysics Data System (ADS)

Boriev, I. A.

2018-03-01

Astronomical data indicate a presence of dark matter (DM) in the space, what is necessary for explanation of observed dynamics of the galaxies within Newtonian mechanics. DM, at its very low density (∼10-26kg/m3), constitutes main part of the matter in the Universe, 10 times the mass of all visible cosmic bodies. No doubt, namely properties of DM, which fills space, must determine its physical properties and fundamental physical laws. Taking into account observed properties of cosmic microwave background radiation (CMBR), whose energy is ∼90% of all cosmic radiation, and understanding that this radiation is produced by DM motion, conservation laws of classical physics and principles of quantum mechanics receive their materialistic substantiation. Thus, CMBR high homogeneity and isotropy (∼10-4), and hence the same properties of DM (and space) justify momentum and angular momentum conservation laws, respectively, according to E. Noether's theorems. CMBR has black body spectrum at ∼2.7K with maximum wavelength ∼1.9·10-3m, what allows calculate the value of mechanical action produced by DM thermal motion (∼7·10-34 J·s). This value corresponds well to the Planck’s constant, which is the mechanical action too, what gives materialistic basis for all principles of quantum mechanics. Obtained results directly confirm the reality of DM existence, and show that CMBR is an observed display of DM thermal motion. Understanding that namely from DM occur known creation of electron-positron pairs as contrarily rotating material vortexes (according to their spins) let substantiate positron nature of ball lightning what first explains all its observed specific properties.

Quantum Information in Non-physics Departments at Liberal Arts Colleges

NASA Astrophysics Data System (ADS)

Westmoreland, Michael

2012-02-01

Quantum information and quantum computing have changed our thinking about the basic concepts of quantum physics. These fields have also introduced exciting new applications of quantum mechanics such as quantum cryptography and non-interactive measurement. It is standard to teach such topics only to advanced physics majors who have completed coursework in quantum mechanics. Recent encounters with teaching quantum cryptography to non-majors and a bout of textbook-writing suggest strategies for teaching this interesting material to those without the standard quantum mechanics background. This talk will share some of those strategies.

Synthesis of photochromic nanoparticles and determination of the mechanism of photochromism

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

Inoue, Shuhei, E-mail: shu18@hiroshima-u.ac.jp; Matsumura, Yukihiko; Kawamoto, Takahiro

2016-05-15

Photochromic nanoparticles of zinc-silicon oxide were synthesized using plasma enhanced chemical vapor deposition. These particles turned black upon irradiating with ultraviolet light. We investigated this phenomenon using density functional theory calculations. Silicon inclusions create trap levels and oxygen defects that reduce the ionization potential of ZnO. This forms a quantum potential between ZnO and zinc-silicon oxide, and the excited electron is stable. Because oxygen defects also increase the bond overlap population between the zinc atoms in a ZnO crystal, they introduce further defects and help in the formation of quantum potentials. Growth of a perfect crystal of ZnO prevents themore » formation of oxygen defects, which is not desirable for photochromism.« less

Development and validation of an achievement test in introductory quantum mechanics: The Quantum Mechanics Visualization Instrument (QMVI)

NASA Astrophysics Data System (ADS)

Cataloglu, Erdat

The purpose of this study was to construct a valid and reliable multiple-choice achievement test to assess students' understanding of core concepts of introductory quantum mechanics. Development of the Quantum Mechanics Visualization Instrument (QMVI) occurred across four successive semesters in 1999--2001. During this time 213 undergraduate and graduate students attending the Pennsylvania State University (PSU) at University Park and Arizona State University (ASU) participated in this development and validation study. Participating students were enrolled in four distinct groups of courses: Modern Physics, Undergraduate Quantum Mechanics, Graduate Quantum Mechanics, and Chemistry Quantum Mechanics. Expert panels of professors of physics experienced in teaching quantum mechanics courses and graduate students in physics and science education established the core content and assisted in the validating of successive versions of the 24-question QMVI. Instrument development was guided by procedures outlined in the Standards for Educational and Psychological Testing (AERA-APA-NCME, 1999). Data gathered in this study provided information used in the development of successive versions of the QMVI. Data gathered in the final phase of administration of the QMVI also provided evidence that the intended score interpretation of the QMVI achievement test is valid and reliable. A moderate positive correlation coefficient of 0.49 was observed between the students' QMVI scores and their confidence levels. Analyses of variance indicated that students' scores in Graduate Quantum Mechanics and Undergraduate Quantum Mechanics courses were significantly higher than the mean scores of students in Modern Physics and Chemistry Quantum Mechanics courses (p < 0.05). That finding is consistent with the additional understanding and experience that should be anticipated in graduate students and junior-senior level students over sophomore physics majors and majors in another field. The moderate positive correlation coefficient of 0.42 observed between students' QMVI scores and their final course grades was also consistent with expectations in a valid instrument. In addition, the Cronbach-alpha reliability coefficient of the QMVI was found to be 0.82. Limited findings were drawn on students' understanding of introductory quantum mechanics concepts. Data suggested that the construct of quantum mechanics understanding is most likely multidimensional and the Main Topic defined as "Quantum Mechanics Postulates" may be an especially important factor for students in acquiring a successful understanding of quantum mechanics.

Enhancing multi-step quantum state tomography by PhaseLift

NASA Astrophysics Data System (ADS)

Lu, Yiping; Zhao, Qing

2017-09-01

Multi-photon system has been studied by many groups, however the biggest challenge faced is the number of copies of an unknown state are limited and far from detecting quantum entanglement. The difficulty to prepare copies of the state is even more serious for the quantum state tomography. One possible way to solve this problem is to use adaptive quantum state tomography, which means to get a preliminary density matrix in the first step and revise it in the second step. In order to improve the performance of adaptive quantum state tomography, we develop a new distribution scheme of samples and extend it to three steps, that is to correct it once again based on the density matrix obtained in the traditional adaptive quantum state tomography. Our numerical results show that the mean square error of the reconstructed density matrix by our new method is improved to the level from 10-4 to 10-9 for several tested states. In addition, PhaseLift is also applied to reduce the required storage space of measurement operator.

Theory of the Decoherence Effect in Finite and Infinite Open Quantum Systems Using the Algebraic Approach

NASA Astrophysics Data System (ADS)

Blanchard, Philippe; Hellmich, Mario; Ługiewicz, Piotr; Olkiewicz, Robert

Quantum mechanics is the greatest revision of our conception of the character of the physical world since Newton. Consequently, David Hilbert was very interested in quantum mechanics. He and John von Neumann discussed it frequently during von Neumann's residence in Göttingen. He published in 1932 his book Mathematical Foundations of Quantum Mechanics. In Hilbert's opinion it was the first exposition of quantum mechanics in a mathematically rigorous way. The pioneers of quantum mechanics, Heisenberg and Dirac, neither had use for rigorous mathematics nor much interest in it. Conceptually, quantum theory as developed by Bohr and Heisenberg is based on the positivism of Mach as it describes only observable quantities. It first emerged as a result of experimental data in the form of statistical observations of quantum noise, the basic concept of quantum probability.

Formulation of state projected centroid molecular dynamics: Microcanonical ensemble and connection to the Wigner distribution.

PubMed

Orr, Lindsay; Hernández de la Peña, Lisandro; Roy, Pierre-Nicholas

2017-06-07

A derivation of quantum statistical mechanics based on the concept of a Feynman path centroid is presented for the case of generalized density operators using the projected density operator formalism of Blinov and Roy [J. Chem. Phys. 115, 7822-7831 (2001)]. The resulting centroid densities, centroid symbols, and centroid correlation functions are formulated and analyzed in the context of the canonical equilibrium picture of Jang and Voth [J. Chem. Phys. 111, 2357-2370 (1999)]. The case where the density operator projects onto a particular energy eigenstate of the system is discussed, and it is shown that one can extract microcanonical dynamical information from double Kubo transformed correlation functions. It is also shown that the proposed projection operator approach can be used to formally connect the centroid and Wigner phase-space distributions in the zero reciprocal temperature β limit. A Centroid Molecular Dynamics (CMD) approximation to the state-projected exact quantum dynamics is proposed and proven to be exact in the harmonic limit. The state projected CMD method is also tested numerically for a quartic oscillator and a double-well potential and found to be more accurate than canonical CMD. In the case of a ground state projection, this method can resolve tunnelling splittings of the double well problem in the higher barrier regime where canonical CMD fails. Finally, the state-projected CMD framework is cast in a path integral form.

Formulation of state projected centroid molecular dynamics: Microcanonical ensemble and connection to the Wigner distribution

NASA Astrophysics Data System (ADS)

Orr, Lindsay; Hernández de la Peña, Lisandro; Roy, Pierre-Nicholas

2017-06-01

A derivation of quantum statistical mechanics based on the concept of a Feynman path centroid is presented for the case of generalized density operators using the projected density operator formalism of Blinov and Roy [J. Chem. Phys. 115, 7822-7831 (2001)]. The resulting centroid densities, centroid symbols, and centroid correlation functions are formulated and analyzed in the context of the canonical equilibrium picture of Jang and Voth [J. Chem. Phys. 111, 2357-2370 (1999)]. The case where the density operator projects onto a particular energy eigenstate of the system is discussed, and it is shown that one can extract microcanonical dynamical information from double Kubo transformed correlation functions. It is also shown that the proposed projection operator approach can be used to formally connect the centroid and Wigner phase-space distributions in the zero reciprocal temperature β limit. A Centroid Molecular Dynamics (CMD) approximation to the state-projected exact quantum dynamics is proposed and proven to be exact in the harmonic limit. The state projected CMD method is also tested numerically for a quartic oscillator and a double-well potential and found to be more accurate than canonical CMD. In the case of a ground state projection, this method can resolve tunnelling splittings of the double well problem in the higher barrier regime where canonical CMD fails. Finally, the state-projected CMD framework is cast in a path integral form.

From classical to quantum mechanics: ``How to translate physical ideas into mathematical language''

NASA Astrophysics Data System (ADS)

Bergeron, H.

2001-09-01

Following previous works by E. Prugovečki [Physica A 91A, 202 (1978) and Stochastic Quantum Mechanics and Quantum Space-time (Reidel, Dordrecht, 1986)] on common features of classical and quantum mechanics, we develop a unified mathematical framework for classical and quantum mechanics (based on L2-spaces over classical phase space), in order to investigate to what extent quantum mechanics can be obtained as a simple modification of classical mechanics (on both logical and analytical levels). To obtain this unified framework, we split quantum theory in two parts: (i) general quantum axiomatics (a system is described by a state in a Hilbert space, observables are self-adjoints operators, and so on) and (ii) quantum mechanics proper that specifies the Hilbert space as L2(Rn); the Heisenberg rule [pi,qj]=-iℏδij with p=-iℏ∇, the free Hamiltonian H=-ℏ2Δ/2m and so on. We show that general quantum axiomatics (up to a supplementary "axiom of classicity") can be used as a nonstandard mathematical ground to formulate physical ideas and equations of ordinary classical statistical mechanics. So, the question of a "true quantization" with "ℏ" must be seen as an independent physical problem not directly related with quantum formalism. At this stage, we show that this nonstandard formulation of classical mechanics exhibits a new kind of operation that has no classical counterpart: this operation is related to the "quantization process," and we show why quantization physically depends on group theory (the Galilei group). This analytical procedure of quantization replaces the "correspondence principle" (or canonical quantization) and allows us to map classical mechanics into quantum mechanics, giving all operators of quantum dynamics and the Schrödinger equation. The great advantage of this point of view is that quantization is based on concrete physical arguments and not derived from some "pure algebraic rule" (we exhibit also some limit of the correspondence principle). Moreover spins for particles are naturally generated, including an approximation of their interaction with magnetic fields. We also recover by this approach the semi-classical formalism developed by E. Prugovečki [Stochastic Quantum Mechanics and Quantum Space-time (Reidel, Dordrecht, 1986)].

Advanced Concepts in Quantum Mechanics

NASA Astrophysics Data System (ADS)

Esposito, Giampiero; Marmo, Giuseppe; Miele, Gennaro; Sudarshan, George

2014-11-01

Preface; 1. Introduction: the need for a quantum theory; 2. Experimental foundations of quantum theory; 3. Waves and particles; 4. Schrödinger picture, Heisenberg picture and probabilistic aspects; 5. Integrating the equations of motion; 6. Elementary applications: 1-dimensional problems; 7. Elementary applications: multidimensional problems; 8. Coherent states and related formalism; 9. Introduction to spin; 10. Symmetries in quantum mechanics; 11. Approximation methods; 12. Modern pictures of quantum mechanics; 13. Formulations of quantum mechanics and their physical implications; 14. Exam problems; Glossary of geometric concepts; References; Index.

The dissociative recombination of O2(+) - The quantum yield of O(1S) and O(1D)

NASA Technical Reports Server (NTRS)

Abreu, V. J.; Solomon, S. C.; Sharp, W. E.; Hays, P. B.

1983-01-01

Data from the visible airglow experiment on the Atmosphere Explorer-E satellite have been used to determine the quantum yield of O(1S) and O(1D) from the dissociative recombination of O2(+). A range of values between 0.09 and 0.23 has been obtained for the quantum yield of O(1S). It is shown that the quantum yield of O(1S) depends on the ratio of electron density to atomic oxygen density. This suggests that the quantum yield of O(1S) may depend on the degree of vibrational excitation of the recombining O2(+). The quantum yield of O(1D) has been measured to be 1.23 + or - 0.42, with no dependence on the electron-oxygen ratio.

A photoemission moments model using density functional and transfer matrix methods applied to coating layers on surfaces: Theory

NASA Astrophysics Data System (ADS)

Jensen, Kevin L.; Finkenstadt, Daniel; Shabaev, Andrew; Lambrakos, Samuel G.; Moody, Nathan A.; Petillo, John J.; Yamaguchi, Hisato; Liu, Fangze

2018-01-01

Recent experimental measurements of a bulk material covered with a small number of graphene layers reported by Yamaguchi et al. [NPJ 2D Mater. Appl. 1, 12 (2017)] (on bialkali) and Liu et al. [Appl. Phys. Lett. 110, 041607 (2017)] (on copper) and the needs of emission models in beam optics codes have lead to substantial changes in a Moments model of photoemission. The changes account for (i) a barrier profile and density of states factor based on density functional theory (DFT) evaluations, (ii) a Drude-Lorentz model of the optical constants and laser penetration depth, and (iii) a transmission probability evaluated by an Airy Transfer Matrix Approach. Importantly, the DFT results lead to a surface barrier profile of a shape similar to both resonant barriers and reflectionless wells: the associated quantum mechanical transmission probabilities are shown to be comparable to those recently required to enable the Moments (and Three Step) model to match experimental data but for reasons very different than the assumption by conventional wisdom that a barrier is responsible. The substantial modifications of the Moments model components, motivated by computational materials methods, are developed. The results prepare the Moments model for use in treating heterostructures and discrete energy level systems (e.g., quantum dots) proposed for decoupling the opposing metrics of performance that undermine the performance of advanced light sources like the x-ray Free Electron Laser. The consequences of the modified components on quantum yield, emittance, and emission models needed by beam optics codes are discussed.

Nonadiabatic one-electron transfer mechanism for the O-O bond formation in the oxygen-evolving complex of photosystem II

NASA Astrophysics Data System (ADS)

Shoji, Mitsuo; Isobe, Hiroshi; Shigeta, Yasuteru; Nakajima, Takahito; Yamaguchi, Kizashi

2018-04-01

The reaction mechanism of the O2 formation in the S4 state of the oxygen-evolving complex of photosystem II was clarified at the quantum mechanics/molecular mechanics (QM/MM) level. After the Yz (Y161) oxidation and the following proton transfer in the S3 state, five reaction steps are required to produce the molecular dioxygen. The highest barrier step is the first proton transfer reaction (0 → 1). The following reactions involving electron transfers were precisely analyzed in terms of their energies, structures and spin densities. We found that the one-electron transfer from the Mn4Ca cluster to Y161 triggers the O-O sigma bond formation.

Magneto-transport of an electron bilayer system in an undoped Si/SiGe double-quantum-well heterostructure

DOE PAGES

Laroche, Dominique; Huang, ShiHsien; Nielsen, Erik; ...

2015-04-08

We report the design, the fabrication, and the magneto-transport study of an electron bilayer system embedded in an undoped Si/SiGe double-quantum-well heterostructure. Additionally, the combined Hall densities (n Hall ) ranging from 2.6 × 10 10 cm -2 to 2.7 × 10 11 cm -2 were achieved, yielding a maximal combined Hall mobility (μ Hall ) of 7.7 × 10 5 cm 2/(V • s) at the highest density. Simultaneous electron population of both quantum wells is clearly observed through a Hall mobility drop as the Hall density is increased to n Hall > 3.3 × 10 10 cm -2,more » consistent with Schrödinger-Poisson simulations. Furthermore, the integer and fractional quantum Hall effects are observed in the device, and single-layer behavior is observed when both layers have comparable densities, either due to spontaneous interlayer coherence or to the symmetric-antisymmetric gap.« less

Quantum mechanical study of the structure and spectroscopic (FT-IR, FT-Raman, 13C, 1H and UV), first order hyperpolarizabilities, NBO and TD-DFT analysis of the 4-methyl-2-cyanobiphenyl

NASA Astrophysics Data System (ADS)

Sebastian, S.; Sundaraganesan, N.; Karthikeiyan, B.; Srinivasan, V.

2011-02-01

The Fourier transform infrared (FT-IR) and FT-Raman of 4-methyl-2-cyanobiphenyl (4M2CBP) have been recorded and analyzed. The equilibrium geometry, bonding features and harmonic vibrational frequencies have been investigated with the help of density functional theory (DFT) method. The assignments of the vibrational spectra have been carried out with the help of normal coordinate analysis (NCA) following the scaled quantum mechanical force field methodology (SQMFF). The 1H and 13C nuclear magnetic resonance (NMR) chemical shifts of the molecule were calculated by the Gauge including atomic orbital (GIAO) method. The first order hyperpolarizability ( β0) of this novel molecular system and related properties ( β, α0 and Δ α) of 4M2CBP are calculated using HF/6-311G(d,p) method on the finite-field approach. Stability of the molecule arising from hyperconjugative interactions, charge delocalization have been analyzed using natural bond orbital (NBO) analysis. The results show that charge in electron density (ED) in the σ* and π* antibonding orbitals and second order delocalization energies ( E2) confirms the occurrence of intramolecular charge transfer (ICT) within the molecule. UV-vis spectrum of the compound was recorded and the electronic properties, such as HOMO and LUMO energies, were performed by time-dependent density functional theory (TD-DFT) approach. Finally the calculations results were applied to simulated infrared and Raman spectra of the title compound which show good agreement with observed spectra.

Synthesis, spectroscopic and TD-DFT quantum mechanical study of azo-azomethine dyes. A laser induced trans-cis-trans photoisomerization cycle

NASA Astrophysics Data System (ADS)

Georgiev, Anton; Kostadinov, Anton; Ivanov, Deyan; Dimov, Deyan; Stoyanov, Simeon; Nedelchev, Lian; Nazarova, Dimana; Yancheva, Denitsa

2018-03-01

This paper describes the synthesis, spectroscopic characterization and quantum mechanical calculations of three azo-azomethine dyes. The dyes were synthesized via condensation reaction between 4-(dimethylamino)benzaldehyde and three different 4-aminobenzene azo dyes. Quantum chemical calculations on the optimized molecular geometry and electron densities of the trans (E) and cis (Z) isomers and their vibrational frequencies have been computed by using DFT/B3LYP density-functional theory with 6-311 ++G(d,p) basis set in vacuo. The thermodynamic parameters such as total electronic energy E (RB3LYP), enthalpy H298 (sum of electronic and thermal enthalpies), free Gibbs energy G298 (sum of electronic and thermal free Gibbs energies) and dipole moment μ were computed for trans (E) and cis (Z) isomers in order to estimate the ΔEtrans → cis, Δμtrans → cis,ΔHtrans → cis, ΔGtrans → cis and ΔStrans → cis values. After molecular geometry optimization the electronic spectra have been obtained by TD-DFT calculations at same basis set and correlated with the spectra of vapour deposited nanosized films of the dyes. The NBO analysis was performed in order to understand the intramolecular charge transfer and energy of resonance stabilization. Solvatochromism was investigated by UV-VIS spectroscopy in five different organic solvents with increasing polarity. The dynamic photoisomerization experiments have been performed in DMF by pump lasers λ = 355 nm (mostly E → Z) and λ = 491 nm (mostly Z → E) in spectral region 300 nm - 800 nm at equal concentrations and times of illumination in order to investigate the photodynamical trans-cis-trans properties of the sbnd CHdbnd Nsbnd and sbnd Ndbnd Nsbnd chromophore groups of the dyes.

Quantum Mechanics From the Cradle?

ERIC Educational Resources Information Center

Martin, John L.

1974-01-01

States that the major problem in learning quantum mechanics is often the student's ignorance of classical mechanics and that one conceptual hurdle in quantum mechanics is its statistical nature, in contrast to the determinism of classical mechanics. (MLH)

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

Influence of template properties and quantum well number on stimulated emission from Al0.7Ga0.3N/Al0.8Ga0.2N quantum wells

NASA Astrophysics Data System (ADS)

Jeschke, J.; Martens, M.; Hagedorn, S.; Knauer, A.; Mogilatenko, A.; Wenzel, H.; Zeimer, U.; Enslin, J.; Wernicke, T.; Kneissl, M.; Weyers, M.

2018-03-01

AlGaN multiple quantum well laser heterostructures for emission around 240 nm have been grown by metalorganic vapor phase epitaxy on epitaxially laterally overgrown (ELO) AlN/sapphire templates. The edge emitting laser structures showed optically pumped lasing with threshold power densities in the range of 2 MW cm-2. The offcut angle of the sapphire substrates as well as the number and the width of the quantum wells were varied while keeping the total thickness of the gain region constant. A larger offcut angle of 0.2° leads to step bunching on the surface as well as Ga accumulation at the steps, but also to an increased inclination of threading dislocations and coalescence boundaries resulting in a reduced dislocation density and thus a reduced laser threshold in comparison to lasers grown on ELO with an offcut of 0.1°. For low losses, samples with fewer QWs exhibited a lower lasing threshold due to a reduced transparency pump power density while for high losses, caused by a higher threading dislocation density, the quadruple quantum well was favorable due to its higher maximum gain.

Information measures for a local quantum phase transition: Lattice fermions in a one-dimensional harmonic trap

NASA Astrophysics Data System (ADS)

Zhang, Yicheng; Vidmar, Lev; Rigol, Marcos

2018-02-01

We use quantum information measures to study the local quantum phase transition that occurs for trapped spinless fermions in one-dimensional lattices. We focus on the case of a harmonic confinement. The transition occurs upon increasing the characteristic density and results in the formation of a band-insulating domain in the center of the trap. We show that the ground-state bipartite entanglement entropy can be used as an order parameter to characterize this local quantum phase transition. We also study excited eigenstates by calculating the average von Neumann and second Renyi eigenstate entanglement entropies, and compare the results with the thermodynamic entropy and the mutual information of thermal states at the same energy density. While at low temperatures we observe a linear increase of the thermodynamic entropy with temperature at all characteristic densities, the average eigenstate entanglement entropies exhibit a strikingly different behavior as functions of temperature below and above the transition. They are linear in temperature below the transition but exhibit activated behavior above it. Hence, at nonvanishing energy densities above the ground state, the average eigenstate entanglement entropies carry fingerprints of the local quantum phase transition.

Quantum Optical Implementations of Current Quantum Computing Paradigms

DTIC Science & Technology

2005-05-01

Conferences and Proceedings: The results were presented at several conferences. These include: 1. M. O. Scully, " Foundations of Quantum Mechanics ", in...applications have revealed a strong connection between the fundamental aspects of quantum mechanics that governs physical systems and the informational...could be solved in polynomial time using quantum computers. Another set of problems where quantum mechanics can carry out computations substantially

Axioms for quantum mechanics: relativistic causality, retrocausality, and the existence of a classical limit

NASA Astrophysics Data System (ADS)

Rohrlich, Daniel

Y. Aharonov and A. Shimony both conjectured that two axioms - relativistic causality (``no superluminal signalling'') and nonlocality - so nearly contradict each other that only quantum mechanics reconciles them. Can we indeed derive quantum mechanics, at least in part, from these two axioms? No: ``PR-box'' correlations show that quantum correlations are not the most nonlocal correlations consistent with relativistic causality. Here we replace ``nonlocality'' with ``retrocausality'' and supplement the axioms of relativistic causality and retrocausality with a natural and minimal third axiom: the existence of a classical limit, in which macroscopic observables commute. That is, just as quantum mechanics has a classical limit, so must any generalization of quantum mechanics. In this limit, PR-box correlations violaterelativistic causality. Generalized to all stronger-than-quantum bipartite correlations, this result is a derivation of Tsirelson's bound (a theorem of quantum mechanics) from the three axioms of relativistic causality, retrocausality and the existence of a classical limit. Although the derivation does not assume quantum mechanics, it points to the Hilbert space structure that underlies quantum correlations. I thank the John Templeton Foundation (Project ID 43297) and the Israel Science Foundation (Grant No. 1190/13) for support.

Elimination of Bimodal Size in InAs/GaAs Quantum Dots for Preparation of 1.3-μm Quantum Dot Lasers

NASA Astrophysics Data System (ADS)

Su, Xiang-Bin; Ding, Ying; Ma, Ben; Zhang, Ke-Lu; Chen, Ze-Sheng; Li, Jing-Lun; Cui, Xiao-Ran; Xu, Ying-Qiang; Ni, Hai-Qiao; Niu, Zhi-Chuan

2018-02-01

The device characteristics of semiconductor quantum dot lasers have been improved with progress in active layer structures. Self-assembly formed InAs quantum dots grown on GaAs had been intensively promoted in order to achieve quantum dot lasers with superior device performances. In the process of growing high-density InAs/GaAs quantum dots, bimodal size occurs due to large mismatch and other factors. The bimodal size in the InAs/GaAs quantum dot system is eliminated by the method of high-temperature annealing and optimized the in situ annealing temperature. The annealing temperature is taken as the key optimization parameters, and the optimal annealing temperature of 680 °C was obtained. In this process, quantum dot growth temperature, InAs deposition, and arsenic (As) pressure are optimized to improve quantum dot quality and emission wavelength. A 1.3-μm high-performance F-P quantum dot laser with a threshold current density of 110 A/cm2 was demonstrated.

Elimination of Bimodal Size in InAs/GaAs Quantum Dots for Preparation of 1.3-μm Quantum Dot Lasers.

PubMed

Su, Xiang-Bin; Ding, Ying; Ma, Ben; Zhang, Ke-Lu; Chen, Ze-Sheng; Li, Jing-Lun; Cui, Xiao-Ran; Xu, Ying-Qiang; Ni, Hai-Qiao; Niu, Zhi-Chuan

2018-02-21

The device characteristics of semiconductor quantum dot lasers have been improved with progress in active layer structures. Self-assembly formed InAs quantum dots grown on GaAs had been intensively promoted in order to achieve quantum dot lasers with superior device performances. In the process of growing high-density InAs/GaAs quantum dots, bimodal size occurs due to large mismatch and other factors. The bimodal size in the InAs/GaAs quantum dot system is eliminated by the method of high-temperature annealing and optimized the in situ annealing temperature. The annealing temperature is taken as the key optimization parameters, and the optimal annealing temperature of 680 °C was obtained. In this process, quantum dot growth temperature, InAs deposition, and arsenic (As) pressure are optimized to improve quantum dot quality and emission wavelength. A 1.3-μm high-performance F-P quantum dot laser with a threshold current density of 110 A/cm 2 was demonstrated.

Tuning Surface Energy Landscapes in Metallic Quantum Films using Alkali Adsorbates

NASA Astrophysics Data System (ADS)

Khajetoorians, Alexander; Qin, Shengyong; Zhu, Wenguang; Eisele, Holger; Zhang, Zhenyu; Shih, Chih-Kang

2008-03-01

Quantum confinement shows a strong interplay with growth and kinetics in thin metal systems where the Fermi wavelength has a special relationship to the surface normal lattice constant. In the case of Pb/Si(111) systems, this relationship reveals an interesting thickness-dependent bilayer oscillation in the density of states and surface energy up to a phase. In this paper, we report on a novel effect: tuning of the energy landscape of a flat-top quantum Pb mesa using Cs adsorbates. Using STM/STS, we show that depositing Cs adsorbates on a thin Pb mesa promotes quantum stable Pb nanoislands on preferentially unstable thicknesses. Thickness-dependent nanoisland densities show a strong bilayer oscillation correlating with quantum stability. By modifying the Cs coverage on the mesa surface, we can tune the lateral size distribution of the nanoislands and the overall amplitude of the island density oscillation. Nanoisland formation is linked to a step decoration of Cs adatoms along the step edge of the nanoisland.

Density-functional theory simulation of large quantum dots

NASA Astrophysics Data System (ADS)

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

2003-10-01

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

Anomaly detection in reconstructed quantum states using a machine-learning technique

NASA Astrophysics Data System (ADS)

Hara, Satoshi; Ono, Takafumi; Okamoto, Ryo; Washio, Takashi; Takeuchi, Shigeki

2014-02-01

The accurate detection of small deviations in given density matrices is important for quantum information processing. Here we propose a method based on the concept of data mining. We demonstrate that the proposed method can more accurately detect small erroneous deviations in reconstructed density matrices, which contain intrinsic fluctuations due to the limited number of samples, than a naive method of checking the trace distance from the average of the given density matrices. This method has the potential to be a key tool in broad areas of physics where the detection of small deviations of quantum states reconstructed using a limited number of samples is essential.

Influence of Molecular Oxygen on Ortho-Para Conversion of Water Molecules

NASA Astrophysics Data System (ADS)

Valiev, R. R.; Minaev, B. F.

2017-07-01

The mechanism of influence of molecular oxygen on the probability of ortho-para conversion of water molecules and its relation to water magnetization are considered within the framework of the concept of paramagnetic spin catalysis. Matrix elements of the hyperfine ortho-para interaction via the Fermi contact mechanism are calculated, as well as the Maliken spin densities on water protons in H2O and O2 collisional complexes. The mechanism of penetration of the electron spin density into the water molecule due to partial spin transfer from paramagnetic oxygen is considered. The probability of ortho-para conversion of the water molecules is estimated by the quantum chemistry methods. The results obtained show that effective ortho-para conversion of the water molecules is possible during the existence of water-oxygen dimers. An external magnetic field affects the ortho-para conversion rate given that the wave functions of nuclear spin sublevels of the water protons are mixed in the complex with oxygen.

Time of arrival in quantum and Bohmian mechanics

NASA Astrophysics Data System (ADS)

Leavens, C. R.

1998-08-01

In a recent paper Grot, Rovelli, and Tate (GRT) [Phys. Rev. A 54, 4676 (1996)] derived an expression for the probability distribution π(TX) of intrinsic arrival times T(X) at position x=X for a quantum particle with initial wave function ψ(x,t=0) freely evolving in one dimension. This was done by quantizing the classical expression for the time of arrival of a free particle at X, assuming a particular choice of operator ordering, and then regulating the resulting time of arrival operator. For the special case of a minimum-uncertainty-product wave packet at t=0 with average wave number and variance Δk they showed that their analytical expression for π(TX) agreed with the probability current density J(x=X,t=T) only to terms of order Δk/. They dismissed the probability current density as a viable candidate for the exact arrival time distribution on the grounds that it can sometimes be negative. This fact is not a problem within Bohmian mechanics where the arrival time distribution for a particle, either free or in the presence of a potential, is rigorously given by \\|J(X,T)\\| (suitably normalized) [W. R. McKinnon and C. R. Leavens, Phys. Rev. A 51, 2748 (1995); C. R. Leavens, Phys. Lett. A 178, 27 (1993); M. Daumer et al., in On Three Levels: The Mathematical Physics of Micro-, Meso-, and Macro-Approaches to Physics, edited by M. Fannes et al. (Plenum, New York, 1994); M. Daumer, in Bohmian Mechanics and Quantum Theory: An Appraisal, edited by J. T. Cushing et al. (Kluwer Academic, Dordrecht, 1996)]. The two theories are compared in this paper and a case presented for which the results could not differ more: According to GRT's theory, every particle in the ensemble reaches a point x=X, where ψ(x,t) and J(x,t) are both zero for all t, while no particle ever reaches X according to the theory based on Bohmian mechanics. Some possible implications are discussed.

Ultrafast electronic dynamics in unipolar n-doped indium gallium arsenide/gallium arsenide self-assembled quantum dots

NASA Astrophysics Data System (ADS)

Wu, Zong-Kwei J.

2006-12-01

Photodetectors based on intraband infrared absorption in the quantum dots have demonstrated improved performance over its quantum well counterpart by lower dark current, relative temperature insensitivity, and its ability for normal incidence operation. Various scattering processes, including phonon emission/absorption and carrier-carrier scattering, are critical in understanding device operation on the fundamental level. In previous studies, our group has investigated carrier dynamics in both low- and high-density regime. Ultrafast electron-hole scattering and the predicted phonon bottleneck effect in intrinsic quantum dots have been observed. Further examination on electron dynamics in unipolar structures is presented in this thesis. We used n-doped quantum dot in mid-infrared photodetector device structure to study the electron dynamics in unipolar structure. Differential transmission spectroscopy with mid-infrared intraband pump and optical interband probe was implemented to measure the electron dynamics directly without creating extra electron-hole pair, Electron relaxation after excitation was measured under various density and temperature conditions. Rapid capture into quantum dot within ˜ 10 ps was observed due to Auger-type electron-electron scattering. Intradot relaxation from the quantum dot excited state to the ground state was also observed on the time scale of 100 ps. With highly doped electron density in the structure, the inter-sublevel relaxation is dominated by Auger-type electron-electron scattering and the phonon bottleneck effect is circumvented. Nanosecond-scale recovery in larger-sized quantum dots was observed, not intrinsic to electron dynamics but due to band-bending and built-in voltage drift. An ensemble Monte Carlo simulation was also established to model the dynamics in quantum dots and in goad agreement with the experimental results. We presented a comprehensive picture of electron dynamics in the unipolar quantum dot structure. Although the phonon bottleneck is circumvented with high doped electron density, relaxation processes in unipolar quantum dots have been measured with time scales longer than that of bipolar systems. The results explain the operation principles of the quantum dot infrared photodetector on a microscopic level and provide basic understanding for future applications and designs.

Investigation of the CH{sub 3}Cl + CN{sup −} reaction in water: Multilevel quantum mechanics/molecular mechanics study

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

Xu, Yulong; College of Physics and Electronics, Shandong Normal University, Jinan 250014; Zhang, Jingxue

2015-06-28

The CH{sub 3}Cl + CN{sup −} reaction in water was studied using a multilevel quantum mechanics/molecular mechanics (MM) method with the multilevels, electrostatic potential, density functional theory (DFT) and coupled-cluster single double triple (CCSD(T)), for the solute region. The detailed, back-side attack S{sub N}2 reaction mechanism was mapped along the reaction pathway. The potentials of mean force were calculated under both the DFT and CCSD(T) levels for the reaction region. The CCSD(T)/MM level of theory presents a free energy activation barrier height at 20.3 kcal/mol, which agrees very well with the experiment value at 21.6 kcal/mol. The results show thatmore » the aqueous solution has a dominant role in shaping the potential of mean force. The solvation effect and the polarization effect together increase the activation barrier height by ∼11.4 kcal/mol: the solvation effect plays a major role by providing about 75% of the contribution, while polarization effect only contributes 25% to the activation barrier height. Our calculated potential of mean force under the CCSD(T)/MM also has a good agreement with the one estimated using data from previous gas-phase studies.« less

The keto-enol equilibrium and thermal conversion kinetics of 2- and 4-hydroxyacetophenone in the gas phase: a DFT study

NASA Astrophysics Data System (ADS)

Monascal, Yeljair; Gallardo, Eliana; Cartaya, Loriett; Maldonado, Alexis; Bentarcurt, Yenner; Chuchani, Gabriel

2018-01-01

Keto-enol tautomeric equilibrium and the mechanism of thermal conversion of 2- and 4-hydroxyacetophenone in gas phase have been studied by means of electronic structure calculations using density functional theory (DFT). A topological analysis of electron density evidence that the structure of keto and enol forms of 2-hydroxyacetophenone are stabilised by a relatively strong intramolecular hydrogen bond. 2- and 4-hydroxyacetophenone undergo deacetylation reactions yielding phenol and ketene. Two possible mechanisms are considered for these eliminations: the process takes place from the keto form (mechanism A), or occurs from the enolic form of the substrate (mechanism B). Quantum chemical calculations support the mechanism B, being found a good agreement with the experimental activation parameters. These results suggest that the rate-limiting step is the reaction of the enol through a concerted, non-synchronous, semi-polar, four-membered cyclic transition state (TS). The most advanced reaction coordinate in the TS is the rupture of O1...H1 bond, with an evolution in the order of 79.7%-80.9%. Theoretical results also suggest a three-step mechanism for the phenyl acetate formation from 2-hydroxyacetophenone.

Quantum Jeffreys prior for displaced squeezed thermal states

NASA Astrophysics Data System (ADS)

Kwek, L. C.; Oh, C. H.; Wang, Xiang-Bin

1999-09-01

It is known that, by extending the equivalence of the Fisher information matrix to its quantum version, the Bures metric, the quantum Jeffreys prior can be determined from the volume element of the Bures metric. We compute the Bures metric for the displaced squeezed thermal state and analyse the quantum Jeffreys prior and its marginal probability distributions. To normalize the marginal probability density function, it is necessary to provide a range of values of the squeezing parameter or the inverse temperature. We find that if the range of the squeezing parameter is kept narrow, there are significant differences in the marginal probability density functions in terms of the squeezing parameters for the displaced and undisplaced situations. However, these differences disappear as the range increases. Furthermore, marginal probability density functions against temperature are very different in the two cases.

Direct Measurement of the Density Matrix of a Quantum System

NASA Astrophysics Data System (ADS)

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

2016-09-01

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

Direct Measurement of the Density Matrix of a Quantum System.

PubMed

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

2016-09-16

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

Insights into Teaching Quantum Mechanics in Secondary and Lower Undergraduate Education

ERIC Educational Resources Information Center

Krijtenburg-Lewerissa, K.; Pol, H. J.; Brinkman, A.; van Joolingen, W. R.

2017-01-01

This study presents a review of the current state of research on teaching quantum mechanics in secondary and lower undergraduate education. A conceptual approach to quantum mechanics is being implemented in more and more introductory physics courses around the world. Because of the differences between the conceptual nature of quantum mechanics and…

Metal Ion Modeling Using Classical Mechanics

PubMed Central

2017-01-01

Metal ions play significant roles in numerous fields including chemistry, geochemistry, biochemistry, and materials science. With computational tools increasingly becoming important in chemical research, methods have emerged to effectively face the challenge of modeling metal ions in the gas, aqueous, and solid phases. Herein, we review both quantum and classical modeling strategies for metal ion-containing systems that have been developed over the past few decades. This Review focuses on classical metal ion modeling based on unpolarized models (including the nonbonded, bonded, cationic dummy atom, and combined models), polarizable models (e.g., the fluctuating charge, Drude oscillator, and the induced dipole models), the angular overlap model, and valence bond-based models. Quantum mechanical studies of metal ion-containing systems at the semiempirical, ab initio, and density functional levels of theory are reviewed as well with a particular focus on how these methods inform classical modeling efforts. Finally, conclusions and future prospects and directions are offered that will further enhance the classical modeling of metal ion-containing systems. PMID:28045509

Frequency-domain multiscale quantum mechanics/electromagnetics simulation method

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

Meng, Lingyi; Yin, Zhenyu; Yam, ChiYung, E-mail: yamcy@yangtze.hku.hk, E-mail: ghc@everest.hku.hk

A frequency-domain quantum mechanics and electromagnetics (QM/EM) method is developed. Compared with the time-domain QM/EM method [Meng et al., J. Chem. Theory Comput. 8, 1190–1199 (2012)], the newly developed frequency-domain QM/EM method could effectively capture the dynamic properties of electronic devices over a broader range of operating frequencies. The system is divided into QM and EM regions and solved in a self-consistent manner via updating the boundary conditions at the QM and EM interface. The calculated potential distributions and current densities at the interface are taken as the boundary conditions for the QM and EM calculations, respectively, which facilitate themore » information exchange between the QM and EM calculations and ensure that the potential, charge, and current distributions are continuous across the QM/EM interface. Via Fourier transformation, the dynamic admittance calculated from the time-domain and frequency-domain QM/EM methods is compared for a carbon nanotube based molecular device.« less

A priori calculations of the free energy of formation from solution of polymorphic self-assembled monolayers.

PubMed

Reimers, Jeffrey R; Panduwinata, Dwi; Visser, Johan; Chin, Yiing; Tang, Chunguang; Goerigk, Lars; Ford, Michael J; Sintic, Maxine; Sum, Tze-Jing; Coenen, Michiel J J; Hendriksen, Bas L M; Elemans, Johannes A A W; Hush, Noel S; Crossley, Maxwell J

2015-11-10

Modern quantum chemical electronic structure methods typically applied to localized chemical bonding are developed to predict atomic structures and free energies for meso-tetraalkylporphyrin self-assembled monolayer (SAM) polymorph formation from organic solution on highly ordered pyrolytic graphite surfaces. Large polymorph-dependent dispersion-induced substrate-molecule interactions (e.g., -100 kcal mol(-1) to -150 kcal mol(-1) for tetratrisdecylporphyrin) are found to drive SAM formation, opposed nearly completely by large polymorph-dependent dispersion-induced solvent interactions (70-110 kcal mol(-1)) and entropy effects (25-40 kcal mol(-1) at 298 K) favoring dissolution. Dielectric continuum models of the solvent are used, facilitating consideration of many possible SAM polymorphs, along with quantum mechanical/molecular mechanical and dispersion-corrected density functional theory calculations. These predict and interpret newly measured and existing high-resolution scanning tunnelling microscopy images of SAM structure, rationalizing polymorph formation conditions. A wide range of molecular condensed matter properties at room temperature now appear suitable for prediction and analysis using electronic structure calculations.

Quantum Mechanical Calculations of Free Energy and Open-Circuit Voltage in Lattice Modeled Organic Photovoltaic Devices

NASA Astrophysics Data System (ADS)

Lankevich, Vladimir; Bittner, Eric

In organic photovoltaic devices (OPVs), initially bound electron and hole can take many different paths to dissociate and become free charge carriers. This leads to the increase in their density of states and therefore increase in the entropy of the system. Accurate description of the energy barriers that charges have to overcome, therefore requires calculation of the free energy. Free energy of an OPV is directly related to its open-circuit voltage and depends only on few important parameters such as average life-time of a charge-transfer state, average energy of the charge-transfer state and energetic disorder in the system. We extend these ideas to the quantum mechanical simulations of the dissociation in the lattice modeled bulk-heterojunction system. We observe average excitonic and free energies that agree with theoretical predictions and the number of experimental results from previous studies. We study effects of the energy disorder and importance of the dimensionality and morphology in materials such as polymer-fullerene blends.

Molecular origin of differences in hole and electron mobility in amorphous Alq3--a multiscale simulation study.

PubMed

Fuchs, Andreas; Steinbrecher, Thomas; Mommer, Mario S; Nagata, Yuki; Elstner, Marcus; Lennartz, Christian

2012-03-28

In order to determine the molecular origin of the difference in electron and hole mobilities of amorphous thin films of Alq(3) (meridional Alq(3) (tris(8-hydroxyquinoline) aluminium)) we performed multiscale simulations covering quantum mechanics, molecular mechanics and lattice models. The study includes realistic disordered morphologies, polarized site energies to describe diagonal disorder, quantum chemically calculated transfer integrals for the off-diagonal disorder, inner sphere reorganization energies and an approximative scheme for outer sphere reorganization energies. Intermolecular transfer rates were calculated via Marcus-theory and mobilities were simulated via kinetic Monte Carlo simulations and by a Master Equation approach. The difference in electron and hole mobility originates from the different localization of charge density in the radical anion (more delocalized) compared to the radical cation (more confined). This results in higher diagonal disorder for holes and less favourable overlap properties for the hole transfer integrals leading to an overall higher electron mobility.

Theoretical and Experimental Study of Inclusion Complexes of β-Cyclodextrins with Chalcone and 2',4'-Dihydroxychalcone.

PubMed

Sancho, Matias I; Andujar, Sebastian; Porasso, Rodolfo D; Enriz, Ricardo D

2016-03-31

The inclusion complexes formed by chalcone and 2',4'-dihydroxychalcone with β-cyclodextrin have been studied combining experimental (phase solubility diagrams, Fourier transform infrared spectroscopy) and molecular modeling (molecular dynamics, quantum mechanics/molecular mechanics calculations) techniques. The formation constants of the complexes were determined at different temperatures, and the thermodynamic parameters of the process were obtained. The inclusion of chalcone in β-cyclodextrin is an exothermic process, while the inclusion of 2',4'-dihydroxychalcone is endothermic. Free energy profiles, derived from umbrella sampling using molecular dynamics simulations, were constructed to analyze the binding affinity and the complexation reaction at a molecular level. Hybrid QM/MM calculations were also employed to obtain a better description of the energetic and structural aspects of the complexes. The intermolecular interactions that stabilize both inclusion complexes were characterized by means of quantum atoms in molecules theory and reduce density gradient method. The calculated interactions were experimentally observed using FTIR.

Quantum chemical modeling of the inhibition mechanism of monoamine oxidase by oxazolidinone and analogous heterocyclic compounds.

PubMed

Erdem, Safiye Sağ; Özpınar, Gül Altınbaş; Boz, Ümüt

2014-02-01

Monoamine oxidase (MAO, EC 1.4.3.4) is responsible from the oxidation of a variety of amine neurotransmitters. MAO inhibitors are used for the treatment of depression or Parkinson's disease. They also inhibit the catabolism of dietary amines. According to one hypothesis, inactivation results from the formation of a covalent adduct to a cysteine residue in the enzyme. If the adduct is stable enough, the enzyme is inhibited for a long time. After a while, enzyme can turn to its active form as a result of adduct breakdown by β-elimination. In this study, the proposed inactivation mechanism was modeled and tested by quantum chemical calculations. Eight heterocyclic methylthioamine derivatives were selected to represent the proposed covalent adducts. Activation energies related to their β-elimination reactions were calculated using ab initio and density functional theory methods. Calculated activation energies were in good agreement with the relative stabilities of the hypothetical adducts predicted in the literature by enzyme inactivation measurements.

Condensed Matter Theories: Volume 25

NASA Astrophysics Data System (ADS)

Ludeña, Eduardo V.; Bishop, Raymond F.; Iza, Peter

2011-03-01

pt. A. Fermi and Bose fluids, exotic systems. Reemergence of the collective mode in [symbol]He and electron layers / H. M. Bohm ... [et al.]. Dissecting and testing collective and topological scenarios for the quantum critical point / J. W. Clark, V. A. Khodel and M. V. Zverev. Helium on nanopatterned surfaces at finite temperature / E. S. Hernandez ... [et al.]. Towards DFT calculations of metal clusters in quantum fluid matrices / S. A. Chin ... [et al.]. Acoustic band gap formation in metamaterials / D. P. Elford ... [et al.]. Dissipative processes in low density strongly interacting 2D electron systems / D. Neilson. Dynamical spatially resolved response function of finite 1-D nano plasmas / T. Raitza, H. Reinholz and G. Ropke. Renormalized bosons and fermions / K. A. Gernoth and M. L. Ristig. Light clusters in nuclear matter / G. Ropke -- pt. B. Quantum magnets, quantum dynamics and phase transitions. Magnetic ordering of antiferromagnets on a spatially anisotropic triangular lattice / R. F. Bishop ... [et al.]. Thermodynamic detection of quantum phase transitions / M. K. G. Kruse ... [et al.]. The SU(2) semi quantum systems dynamics and thermodynamics / C. M. Sarris and A. N. Proto -- pt. C. Physics of nanosystems and nanotechnology. Quasi-one dimensional fluids that exhibit higher dimensional behavior / S. M. Gatica ... [et al.]. Spectral properties of molecular oligomers. A non-Markovian quantum state diffusion approach / J. Roden, W. T. Strunz and A. Eisfeld. Quantum properties in transport through nanoscopic rings: Charge-spin separation and interference effects / K. Hallberg, J. Rincon and S. Ramasesha. Cooperative localization-delocalization in the high T[symbol] cuprates / J. Ranninger. Thermodynamically stable vortex states in superconducting nanowires / W. M. Wu, M. B. Sobnack and F. V. Kusmartsev.pt. D. Quantum information. Quantum information in optical lattices / A. M. Guzman and M. A. Duenas E. -- pt. E. Theory and applications of molecular dynamics and density functional theory. Exchange-correlation functionals from the identical-particle Ornstein-Zernike equation: Basic formulation and numerical algorithms / R. Cuevas-Saavedra and P. W. Ayers. Features and catalytic properties of RhCu: A review / S. Gonzalez, C. Sousa and F. Illas. Kinetic energy functionals: Exact ones from analytic model wave functions and approximate ones in orbital-free molecular dynamics / V. V. Karasiev ... [et al.]. Numerical analysis of hydrogen storage in carbon nanopores / C. Wexler ... [et al.] -- pt. F. Superconductivity. Generalized Bose-Einstein condensation in superconductivity / M. de Llano. Kohn anomaly energy in conventional superconductors equals twice the energy of the superconducting gap: How and why? / R. Chaudhury and M. P. Das. Collective excitations in superconductors and semiconductors in the presence of a condensed phase / Z. Koinov. Thermal expansion of ferromagnetic superconductors: Possible application to UGe[symbol] / N. Hatayama and R. Konno. Generalized superconducting gap in a Boson-Fermion model / T. A. Mamedov and M. de Llano. Influence of domain walls in the superconductor/ferromagnet proximity effect / E. J. Patino. Spin singlet and triplet superconductivity induced by correlated hopping interactions / L. A. Perez, J. S. Millan and C. Wang -- pt. G. Statistical mechanics, relativistic quantum mechanics. Boltzmann's ergodic hypothesis: A meeting place for two cultures / M. H. Lee. Electron-electron interaction in the non-relativistic limit / F. B. Malik.

Tripolar vortex formation in dense quantum plasma with ion-temperature-gradients

NASA Astrophysics Data System (ADS)

Qamar, Anisa; Ata-ur-Rahman, Mirza, Arshad M.

2012-05-01

We have derived system of nonlinear equations governing the dynamics of low-frequency electrostatic toroidal ion-temperature-gradient mode for dense quantum magnetoplasma. For some specific profiles of the equilibrium density, temperature, and ion velocity gradients, the nonlinear equations admit a stationary solution in the form of a tripolar vortex. These results are relevant to understand nonlinear structure formation in dense quantum plasmas in the presence of equilibrium ion-temperature and density gradients.

Investigating and Improving Student Understanding of Key Ideas in Quantum Mechanics throughout Instruction

NASA Astrophysics Data System (ADS)

Emigh, Paul Jeffrey

This dissertation describes research on student understanding of quantum mechanics across multiple levels of instruction. The primary focus has been to identify patterns in student reasoning related to key concepts in quantum mechanics. The specific topics include quantum measurements, time dependence, vector spaces, and angular momentum. The research has spanned a variety of different quantum courses intended for introductory physics students, upper-division physics majors, and graduate students in physics. The results of this research have been used to develop a set of curriculum, Tutorials in Physics: Quantum Mechanics, for addressing the most persistent student difficulties. We document both the development of this curriculum and how it has impacted and improved student understanding of quantum mechanics.

Quantum mechanics: The Bayesian theory generalized to the space of Hermitian matrices

NASA Astrophysics Data System (ADS)

Benavoli, Alessio; Facchini, Alessandro; Zaffalon, Marco

2016-10-01

We consider the problem of gambling on a quantum experiment and enforce rational behavior by a few rules. These rules yield, in the classical case, the Bayesian theory of probability via duality theorems. In our quantum setting, they yield the Bayesian theory generalized to the space of Hermitian matrices. This very theory is quantum mechanics: in fact, we derive all its four postulates from the generalized Bayesian theory. This implies that quantum mechanics is self-consistent. It also leads us to reinterpret the main operations in quantum mechanics as probability rules: Bayes' rule (measurement), marginalization (partial tracing), independence (tensor product). To say it with a slogan, we obtain that quantum mechanics is the Bayesian theory in the complex numbers.

Teaching Quantum Mechanics on an Introductory Level.

ERIC Educational Resources Information Center

Muller, Rainer; Wiesner, Hartmut

2002-01-01

Presents a new research-based course on quantum mechanics in which the conceptual issues of quantum mechanics are taught at an introductory level. Involves students in the discovery of how quantum phenomena deviate from classical everyday experiences. (Contains 31 references.) (Author/YDS)

Gaussian effective potential: Quantum mechanics

NASA Astrophysics Data System (ADS)

Stevenson, P. M.

1984-10-01

We advertise the virtues of the Gaussian effective potential (GEP) as a guide to the behavior of quantum field theories. Much superior to the usual one-loop effective potential, the GEP is a natural extension of intuitive notions familiar from quantum mechanics. A variety of quantum-mechanical examples are studied here, with an eye to field-theoretic analogies. Quantum restoration of symmetry, dynamical mass generation, and "quantum-mechanical resuscitation" are among the phenomena discussed. We suggest how the GEP could become the basis of a systematic approximation procedure. A companion paper will deal with scalar field theory.

Polarization effects on quantum levels in InN/GaN quantum wells.

PubMed

Lin, Wei; Li, Shuping; Kang, Junyong

2009-12-02

Polarization effects on quantum states in InN/GaN quantum wells have been investigated by means of ab initio calculation and spectroscopic ellipsometry. Through the position-dependent partial densities of states, our results show that the polarization modified by the strain with different well thickness leads to an asymmetry band bending of the quantum well. The quantum levels are identified via the band structures and their square wave function distributions are analyzed by the partial charge densities. Further theoretical and experimental comparison of the imaginary part of the dielectric function show that the overall transition probability increases under larger polarization fields, which can be attributable to the fact that the excited quantum states of 2h have a greater overlap with 1e states and enhance other hole quantum states in the well by a hybridization. These results would provide a new approach to improve the transition probability and light emission by enhancing the polarization fields in a proper way.

Facets of contextual realism in quantum mechanics

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

Pan, Alok Kumar; Home, Dipankar

2011-09-23

In recent times, there is an upsurge of interest in demonstrating the quantum contextuality. In this proceedings, we explore the two different forms of arguments that have been used for showing the contextual character of quantum mechanics. First line of study concerns the violations of the noncontextual realist models by quantum mechanics, where second line of study that is qualitatively distinct from the earlier one, demonstrates the contextuality within the formalism of quantum mechanics.

Density-Gradient Theory: A Macroscopic Approach to Quantum Confinement and Tunneling in Semiconductor Devices

DTIC Science & Technology

2011-01-01

that are attractive as luminescent biolabels, and possibly also for optoelectronic devices and solar cells . The equilibrium nature of such situations...The boundary layers as- sociated with the diffusion and Debye lengths are familiar, while that of LQ defines the layer in which the quantum in...circuits, transmission lines Diffusion -drift, density-gradient Semi-classical electron dynamics, Boltzmann transport Schrödinger, density- matrix, Wigner

Local quantum measurement and no-signaling imply quantum correlations.

PubMed

Barnum, H; Beigi, S; Boixo, S; Elliott, M B; Wehner, S

2010-04-09

We show that, assuming that quantum mechanics holds locally, the finite speed of information is the principle that limits all possible correlations between distant parties to be quantum mechanical as well. Local quantum mechanics means that a Hilbert space is assigned to each party, and then all local positive-operator-valued measurements are (in principle) available; however, the joint system is not necessarily described by a Hilbert space. In particular, we do not assume the tensor product formalism between the joint systems. Our result shows that if any experiment would give nonlocal correlations beyond quantum mechanics, quantum theory would be invalidated even locally.

Probing quantum effects in lithium

NASA Astrophysics Data System (ADS)

Deemyad, Shanti; Zhang, Rong

2018-05-01

In periodic table lithium is the first element immediately after helium and the lightest metal. While fascinating quantum nature of condensed helium is suppressed at high densities, lithium is expected to adapt more quantum solid behavior under compression. This is due to the presence of long range interactions in metallic systems for which an increase in the de-Boer parameter (λ/σ, where σ is the minimum interatomic distance and λ is the de-Broglie wavelength) is predicted at higher densities [1,2]. Physics of dense lithium offers a rich playground to look for new emergent quantum phenomena in condensed matter and has been subject of many theoretical and experimental investigations. In this article recent progress in studying the quantum nature of dense lithium will be discussed.

Sensitivity to perturbations and quantum phase transitions.

PubMed

Wisniacki, D A; Roncaglia, A J

2013-05-01

The local density of states or its Fourier transform, usually called fidelity amplitude, are important measures of quantum irreversibility due to imperfect evolution. In this Rapid Communication we study both quantities in a paradigmatic many body system, the Dicke Hamiltonian, where a single-mode bosonic field interacts with an ensemble of N two-level atoms. This model exhibits a quantum phase transition in the thermodynamic limit, while for finite instances the system undergoes a transition from quasi-integrability to quantum chaotic. We show that the width of the local density of states clearly points out the imprints of the transition from integrability to chaos but no trace remains of the quantum phase transition. The connection with the decay of the fidelity amplitude is also established.

Strained-layer InGaAs/GaAs/AlGaAs single quantum well lasers with high internal quantum efficiency

NASA Technical Reports Server (NTRS)

Larsson, Anders; Cody, Jeffrey; Lang, Robert J.

1989-01-01

Low threshold current density strained-layer In(0.2)Ga(0.8)As/GaAs/AlGaAs single quantum well lasers, emitting at 980 nm, have been grown by molecular beam epitaxy. Contrary to what has been reported for broad-area lasers with pseudomorphic InGaAs active layers grown by metalorganic chemical vapor deposition, these layers exhibit a high internal quantum efficiency (about 90 percent). The maximum external differential quantum efficiency is 70 percent, limited by an anomalously high internal loss possibly caused by a large lateral spreading of the optical mode. In addition, experimental results supporting the theoretically predicted strain-induced reduction of the valence-band nonparabolicity and density of states are presented.

Molecular structure, spectroscopic studies and first-order molecular hyperpolarizabilities of ferulic acid by density functional study

NASA Astrophysics Data System (ADS)

Sebastian, S.; Sundaraganesan, N.; Manoharan, S.

2009-10-01

Quantum chemical calculations of energies, geometrical structure and vibrational wavenumbers of ferulic acid (FA) (4-hydroxy-3-methoxycinnamic acid) were carried out by using density functional (DFT/B3LYP/BLYP) method with 6-31G(d,p) as basis set. The optimized geometrical parameters obtained by DFT calculations are in good agreement with single crystal XRD data. The vibrational spectral data obtained from solid phase FT-IR and FT-Raman spectra are assigned based on the results of the theoretical calculations. The observed spectra are found to be in good agreement with calculated values. The electric dipole moment ( μ) and the first hyperpolarizability ( β) values of the investigated molecule have been computed using ab initio quantum mechanical calculations. The calculation results also show that the FA molecule might have microscopic nonlinear optical (NLO) behavior with non-zero values. A detailed interpretation of the infrared and Raman spectra of FA was also reported. The energy and oscillator strength calculated by time-dependent density functional theory (TD-DFT) results complements with the experimental findings. The calculated HOMO and LUMO energies shows that charge transfer occur within the molecule. The theoretical FT-IR and FT-Raman spectra for the title molecule have been constructed.

Induced Superconductivity in the Quantum Spin Hall Edge

NASA Astrophysics Data System (ADS)

Ren, Hechen; Hart, Sean; Wagner, Timo; Leubner, Philipp; Muehlbauer, Mathias; Bruene, Christoph; Buhmann, Hartmut; Molenkamp, Laurens; Yacoby, Amir

2014-03-01

Two-dimensional topological insulators have a gapped bulk and helical edge states, making it a quantum spin Hall insulator. Combining such edge states with superconductivity can be an excellent platform for observing and manipulating localized Majorana fermions. In the context of condensed matter, these are emergent electronic states that obey non-Abelian statistics and hence support fault-tolerant quantum computing. To realize such theoretical constructions, an essential step is to show these edge channels are capable of carrying coherent supercurrent. In our experiment, we fabricate Josephson junctions with HgTe/HgCdTe quantum wells, a two-dimensional material that becomes a quantum spin Hall insulator when the quantum well is thicker than 6.3 nm and the bulk density is depleted. In this regime, we observe supercurrents whose densities are confined to the edges of the junctions, with edge widths ranging from 180 nm to 408 nm. To verify the topological nature of these edges, we measure identical junctions with HgTe/HgCdTe quantum wells thinner than 6.3 nm and observe only uniform supercurrent density across the junctions. This research is supported by Microsoft Corporation Project Q, the NSF DMR-1206016, the DOE SCGF Program, the German Research Foundation, and EU ERC-AG program.

Quantum dot-polymer conjugates for stable luminescent displays.

PubMed

Ghimire, Sushant; Sivadas, Anjaly; Yuyama, Ken-Ichi; Takano, Yuta; Francis, Raju; Biju, Vasudevanpillai

2018-05-23

The broad absorption of light in the UV-Vis-NIR region and the size-based tunable photoluminescence color of semiconductor quantum dots make these tiny crystals one of the most attractive antennae in solar cells and phosphors in electrooptical devices. One of the primary requirements for such real-world applications of quantum dots is their stable and uniform distribution in optically transparent matrices. In this work, we prepare transparent thin films of polymer-quantum dot conjugates, where CdSe/ZnS quantum dots are uniformly distributed at high densities in a chitosan-polystyrene copolymer (CS-g-PS) matrix. Here, quantum dots in an aqueous solution are conjugated to the copolymer by a phase transfer reaction. With the stable conjugation of quantum dots to the copolymer, we prevent undesired phase separation between the two and aggregation of quantum dots. Furthermore, the conjugate allows us to prepare transparent thin films in which quantum dots are uniformly distributed at high densities. The CS-g-PS copolymer helps us in not only preserving the photoluminescence properties of quantum dots in the film but also rendering excellent photostability to quantum dots at the ensemble and single particle levels, making the conjugate a promising material for photoluminescence-based devices.

Symmetry-broken states in a system of interacting bosons on a two-leg ladder with a uniform Abelian gauge field

NASA Astrophysics Data System (ADS)

Greschner, S.; Piraud, M.; Heidrich-Meisner, F.; McCulloch, I. P.; Schollwöck, U.; Vekua, T.

2016-12-01

We study the quantum phases of bosons with repulsive contact interactions on a two-leg ladder in the presence of a uniform Abelian gauge field. The model realizes many interesting states, including Meissner phases, vortex fluids, vortex lattices, charge density waves, and the biased-ladder phase. Our work focuses on the subset of these states that breaks a discrete symmetry. We use density matrix renormalization group simulations to demonstrate the existence of three vortex-lattice states at different vortex densities and we characterize the phase transitions from these phases into neighboring states. Furthermore, we provide an intuitive explanation of the chiral-current reversal effect that is tied to some of these vortex lattices. We also study a charge-density-wave state that exists at 1/4 particle filling at large interaction strengths and flux values close to half a flux quantum. By changing the system parameters, this state can transition into a completely gapped vortex-lattice Mott-insulating state. We elucidate the stability of these phases against nearest-neighbor interactions on the rungs of the ladder relevant for experimental realizations with a synthetic lattice dimension. A charge-density-wave state at 1/3 particle filling can be stabilized for flux values close to half a flux quantum and for very strong on-site interactions in the presence of strong repulsion on the rungs. Finally, we analytically describe the emergence of these phases in the low-density regime, and, in particular, we obtain the boundaries of the biased-ladder phase, i.e., the phase that features a density imbalance between the legs. We make contact with recent quantum-gas experiments that realized related models and discuss signatures of these quantum states in experimentally accessible observables.

Understanding quantum measurement from the solution of dynamical models

NASA Astrophysics Data System (ADS)

Allahverdyan, Armen E.; Balian, Roger; Nieuwenhuizen, Theo M.

2013-04-01

The quantum measurement problem, to wit, understanding why a unique outcome is obtained in each individual experiment, is currently tackled by solving models. After an introduction we review the many dynamical models proposed over the years for elucidating quantum measurements. The approaches range from standard quantum theory, relying for instance on quantum statistical mechanics or on decoherence, to quantum-classical methods, to consistent histories and to modifications of the theory. Next, a flexible and rather realistic quantum model is introduced, describing the measurement of the z-component of a spin through interaction with a magnetic memory simulated by a Curie-Weiss magnet, including N≫1 spins weakly coupled to a phonon bath. Initially prepared in a metastable paramagnetic state, it may transit to its up or down ferromagnetic state, triggered by its coupling with the tested spin, so that its magnetization acts as a pointer. A detailed solution of the dynamical equations is worked out, exhibiting several time scales. Conditions on the parameters of the model are found, which ensure that the process satisfies all the features of ideal measurements. Various imperfections of the measurement are discussed, as well as attempts of incompatible measurements. The first steps consist in the solution of the Hamiltonian dynamics for the spin-apparatus density matrix Dˆ(t). Its off-diagonal blocks in a basis selected by the spin-pointer coupling, rapidly decay owing to the many degrees of freedom of the pointer. Recurrences are ruled out either by some randomness of that coupling, or by the interaction with the bath. On a longer time scale, the trend towards equilibrium of the magnet produces a final state Dˆ(t) that involves correlations between the system and the indications of the pointer, thus ensuring registration. Although Dˆ(t) has the form expected for ideal measurements, it only describes a large set of runs. Individual runs are approached by analyzing the final states associated with all possible subensembles of runs, within a specified version of the statistical interpretation. There the difficulty lies in a quantum ambiguity: There exist many incompatible decompositions of the density matrix Dˆ(t) into a sum of sub-matrices, so that one cannot infer from its sole determination the states that would describe small subsets of runs. This difficulty is overcome by dynamics due to suitable interactions within the apparatus, which produce a special combination of relaxation and decoherence associated with the broken invariance of the pointer. Any subset of runs thus reaches over a brief delay a stable state which satisfies the same hierarchic property as in classical probability theory; the reduction of the state for each individual run follows. Standard quantum statistical mechanics alone appears sufficient to explain the occurrence of a unique answer in each run and the emergence of classicality in a measurement process. Finally, pedagogical exercises are proposed and lessons for future works on models are suggested, while the statistical interpretation is promoted for teaching.

Cognitive Issues in Learning Advanced Physics: An Example from Quantum Mechanics

NASA Astrophysics Data System (ADS)

Singh, Chandralekha; Zhu, Guangtian

2009-11-01

We are investigating cognitive issues in learning quantum mechanics in order to develop effective teaching and learning tools. The analysis of cognitive issues is particularly important for bridging the gap between the quantitative and conceptual aspects of quantum mechanics and for ensuring that the learning tools help students build a robust knowledge structure. We discuss the cognitive aspects of quantum mechanics that are similar or different from those of introductory physics and their implications for developing strategies to help students develop a good grasp of quantum mechanics.

Heats of Segregation of BCC Metals Using Ab Initio and Quantum Approximate Methods

NASA Technical Reports Server (NTRS)

Good, Brian; Chaka, Anne; Bozzolo, Guillermo

2003-01-01

Many multicomponent alloys exhibit surface segregation, in which the composition at or near a surface may be substantially different from that of the bulk. A number of phenomenological explanations for this tendency have been suggested, involving, among other things, differences among the components' surface energies, molar volumes, and heats of solution. From a theoretical standpoint, the complexity of the problem has precluded a simple, unified explanation, thus preventing the development of computational tools that would enable the identification of the driving mechanisms for segregation. In that context, we investigate the problem of surface segregation in a variety of bcc metal alloys by computing dilute-limit heats of segregation using both the quantum-approximate energy method of Bozzolo, Ferrante and Smith (BFS), and all-electron density functional theory. In addition, the composition dependence of the heats of segregation is investigated using a BFS-based Monte Carlo procedure, and, for selected cases of interest, density functional calculations. Results are discussed in the context of a simple picture that describes segregation behavior as the result of a competition between size mismatch and alloying effects

Electronic decoherence of two-level systems in a Josephson junction

NASA Astrophysics Data System (ADS)

Bilmes, Alexander; Zanker, Sebastian; Heimes, Andreas; Marthaler, Michael; Schön, Gerd; Weiss, Georg; Ustinov, Alexey V.; Lisenfeld, Jürgen

2017-08-01

The sensitivity of superconducting qubits allows for spectroscopy and coherence measurements on individual two-level systems present in the disordered tunnel barrier of an Al /AlOx /Al Josephson junction. We report experimental evidence for the decoherence of two-level systems by Bogoliubov quasiparticles leaking into the insulating AlOx barrier. We control the density of quasiparticles in the junction electrodes either by the sample temperature or by injecting them using an on-chip dc superconducting quantum interference device driven to its resistive state. The decoherence rates were measured by observing the two-level system's quantum state evolving under application of resonant microwave pulses and were found to increase linearly with quasiparticle density, in agreement with theory. This interaction with electronic states provides a noise and decoherence mechanism that is relevant for various microfabricated devices such as qubits, single-electron transistors, and field-effect transistors. The presented experiments also offer a possibility to determine the location of the probed two-level systems across the tunnel barrier, providing clues about the fabrication step in which they emerge.

Extending density functional embedding theory for covalently bonded systems.

PubMed

Yu, Kuang; Carter, Emily A

2017-12-19

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

Electrical tuning of a quantum plasmonic resonance

DOE PAGES

Liu, Xiaoge; Kang, Ju -Hyung; Yuan, Hongtao; ...

2017-06-12

Surface plasmon (SP) excitations in metals facilitate confinement of light into deep-subwavelength volumes and can induce strong light–matter interaction. Generally, the SP resonances supported by noble metal nanostructures are explained well by classical models, at least until the nanostructure size is decreased to a few nanometres, approaching the Fermi wavelength λ F of the electrons. Although there is a long history of reports on quantum size effects in the plasmonic response of nanometre-sized metal particles systematic experimental studies have been hindered by inhomogeneous broadening in ensemble measurements, as well as imperfect control over size, shape, faceting, surface reconstructions, contamination, chargingmore » effects and surface roughness in single-particle measurements. In particular, observation of the quantum size effect in metallic films and its tuning with thickness has been challenging as they only confine carriers in one direction. Here, we show active tuning of quantum size effects in SP resonances supported by a 20-nm-thick metallic film of indium tin oxide (ITO), a plasmonic material serving as a low-carrier-density Drude metal. An ionic liquid (IL) is used to electrically gate and partially deplete the ITO layer. The experiment shows a controllable and reversible blue-shift in the SP resonance above a critical voltage. As a result, a quantum-mechanical model including the quantum size effect reproduces the experimental results, whereas a classical model only predicts a red shift.« less

Electrical tuning of a quantum plasmonic resonance

NASA Astrophysics Data System (ADS)

Liu, Xiaoge; Kang, Ju-Hyung; Yuan, Hongtao; Park, Junghyun; Kim, Soo Jin; Cui, Yi; Hwang, Harold Y.; Brongersma, Mark L.

2017-09-01

Surface plasmon (SP) excitations in metals facilitate confinement of light into deep-subwavelength volumes and can induce strong light-matter interaction. Generally, the SP resonances supported by noble metal nanostructures are explained well by classical models, at least until the nanostructure size is decreased to a few nanometres, approaching the Fermi wavelength λF of the electrons. Although there is a long history of reports on quantum size effects in the plasmonic response of nanometre-sized metal particles, systematic experimental studies have been hindered by inhomogeneous broadening in ensemble measurements, as well as imperfect control over size, shape, faceting, surface reconstructions, contamination, charging effects and surface roughness in single-particle measurements. In particular, observation of the quantum size effect in metallic films and its tuning with thickness has been challenging as they only confine carriers in one direction. Here, we show active tuning of quantum size effects in SP resonances supported by a 20-nm-thick metallic film of indium tin oxide (ITO), a plasmonic material serving as a low-carrier-density Drude metal. An ionic liquid (IL) is used to electrically gate and partially deplete the ITO layer. The experiment shows a controllable and reversible blue-shift in the SP resonance above a critical voltage. A quantum-mechanical model including the quantum size effect reproduces the experimental results, whereas a classical model only predicts a red shift.

Quantum optics, cavity QED, and quantum optomechanics

NASA Astrophysics Data System (ADS)

Meystre, Pierre

2013-05-01

Quantum optomechanics provides a universal tool to achieve the quantum control of mechanical motion. It does that in devices spanning a vast range of parameters, with mechanical frequencies from a few Hertz to GHz, and with masses from 10-20 g to several kilos. Its underlying ideas can be traced back to the study of gravitational wave antennas, quantum optics, cavity QED and laser cooling which, when combined with the recent availability of advanced micromechanical and nanomechanical devices, opens a path to the realization of macroscopic mechanical systems that operate deep in the quantum regime. At the fundamental level this development paves the way to experiments that will lead to a more profound understanding of quantum mechanics; and from the point of view of applications, quantum optomechanical techniques will provide motion and force sensing near the fundamental limit imposed by quantum mechanics (quantum metrology) and significantly expand the toolbox of quantum information science. After a brief summary of key historical developments, the talk will give a broad overview of the current state of the art of quantum optomechanics, and comment on future prospects both in applied and in fundamental science. Work supported by NSF, ARO and the DARPA QuASAR and ORCHID programs.

Testing Nonassociative Quantum Mechanics.

PubMed

Bojowald, Martin; Brahma, Suddhasattwa; Büyükçam, Umut

2015-11-27

The familiar concepts of state vectors and operators in quantum mechanics rely on associative products of observables. However, these notions do not apply to some exotic systems such as magnetic monopoles, which have long been known to lead to nonassociative algebras. Their quantum physics has remained obscure. This Letter presents the first derivation of potentially testable physical results in nonassociative quantum mechanics, based on effective potentials. They imply new effects which cannot be mimicked in usual quantum mechanics with standard magnetic fields.

From Einstein-Podolsky-Rosen paradox to quantum nonlocality: experimental investigation of quantum correlations

NASA Astrophysics Data System (ADS)

Xu, Jin-Shi; Li, Chuan-Feng; Guo, Guang-Can

2016-11-01

In 1935, Einstein, Podolsky and Rosen published their influential paper proposing a now famous paradox (the EPR paradox) that threw doubt on the completeness of quantum mechanics. Two fundamental concepts: entanglement and steering, were given in the response to the EPR paper by Schrodinger, which both reflect the nonlocal nature of quantum mechanics. In 1964, John Bell obtained an experimentally testable inequality, in which its violation contradicts the prediction of local hidden variable models and agrees with that of quantum mechanics. Since then, great efforts have been made to experimentally investigate the nonlocal feature of quantum mechanics and many distinguished quantum properties were observed. In this work, along with the discussion of the development of quantum nonlocality, we would focus on our recent experimental efforts in investigating quantum correlations and their applications with optical systems, including the study of entanglement-assisted entropic uncertainty principle, Einstein-Podolsky-Rosen steering and the dynamics of quantum correlations.

Bose-Einstein condensation in an ultra-hot gas of pumped magnons.

PubMed

Serga, Alexander A; Tiberkevich, Vasil S; Sandweg, Christian W; Vasyuchka, Vitaliy I; Bozhko, Dmytro A; Chumak, Andrii V; Neumann, Timo; Obry, Björn; Melkov, Gennadii A; Slavin, Andrei N; Hillebrands, Burkard

2014-03-11

Bose-Einstein condensation of quasi-particles such as excitons, polaritons, magnons and photons is a fascinating quantum mechanical phenomenon. Unlike the Bose-Einstein condensation of real particles (like atoms), these processes do not require low temperatures, since the high densities of low-energy quasi-particles needed for the condensate to form can be produced via external pumping. Here we demonstrate that such a pumping can create remarkably high effective temperatures in a narrow spectral region of the lowest energy states in a magnon gas, resulting in strikingly unexpected transitional dynamics of Bose-Einstein magnon condensate: the density of the condensate increases immediately after the external magnon flow is switched off and initially decreases if it is switched on again. This behaviour finds explanation in a nonlinear 'evaporative supercooling' mechanism that couples the low-energy magnons overheated by pumping with all the other thermal magnons, removing the excess heat, and allowing Bose-Einstein condensate formation.

Efficiency enhancement of blue light emitting diodes by eliminating V-defects from InGaN/GaN multiple quantum well structures through GaN capping layer control

NASA Astrophysics Data System (ADS)

Tsai, Sheng-Chieh; Li, Ming-Jui; Fang, Hsin-Chiao; Tu, Chia-Hao; Liu, Chuan-Pu

2018-05-01

A facile method for fabricating blue light-emitting diodes (B-LEDs) with small embedded quantum dots (QDs) and enhanced light emission is demonstrated by tuning the temperature of the growing GaN capping layer to eliminate V-defects. As the growth temperature increases from 770 °C to 840 °C, not only does the density of the V-defects reduce from 4.12 ∗ 108 #/cm2 nm to zero on a smooth surface, but the QDs also get smaller. Therefore, the growth mechanism of smaller QDs assisted by elimination of V-defects is discussed. Photoluminescence and electroluminescence results show that smaller embedded QDs can improve recombination efficiency, and thus achieve higher peak intensity with smaller peak broadening. Accordingly, the external quantum efficiency of the B-LEDs with smaller QDs is enhanced, leading to a 6.8% increase in light output power in lamp-form package LEDs.

Quantum Monte Carlo studies of solvated systems

NASA Astrophysics Data System (ADS)

Schwarz, Kathleen; Letchworth Weaver, Kendra; Arias, T. A.; Hennig, Richard G.

2011-03-01

Solvation qualitatively alters the energetics of diverse processes from protein folding to reactions on catalytic surfaces. An explicit description of the solvent in quantum-mechanical calculations requires both a large number of electrons and exploration of a large number of configurations in the phase space of the solvent. These problems can be circumvented by including the effects of solvent through a rigorous classical density-functional description of the liquid environment, thereby yielding free energies and thermodynamic averages directly, while eliminating the need for explicit consideration of the solvent electrons. We have implemented and tested this approach within the CASINO Quantum Monte Carlo code. Our method is suitable for calculations in any basis within CASINO, including b-spline and plane wave trial wavefunctions, and is equally applicable to molecules, surfaces, and crystals. For our preliminary test calculations, we use a simplified description of the solvent in terms of an isodensity continuum dielectric solvation approach, though the method is fully compatible with more reliable descriptions of the solvent we shall employ in the future.

Simultaneous measurement of two noncommuting quantum variables: Solution of a dynamical model

NASA Astrophysics Data System (ADS)

Perarnau-Llobet, Martí; Nieuwenhuizen, Theodorus Maria

2017-05-01

The possibility of performing simultaneous measurements in quantum mechanics is investigated in the context of the Curie-Weiss model for a projective measurement. Concretely, we consider a spin-1/2 system simultaneously interacting with two magnets, which act as measuring apparatuses of two different spin components. We work out the dynamics of this process and determine the final state of the measuring apparatuses, from which we can find the probabilities of the four possible outcomes of the measurements. The measurement is found to be nonideal, as (i) the joint statistics do not coincide with the one obtained by separately measuring each spin component, and (ii) the density matrix of the spin does not collapse in either of the measured observables. However, we give an operational interpretation of the process as a generalized quantum measurement, and show that it is fully informative: The expected value of the measured spin components can be found with arbitrary precision for sufficiently many runs of the experiment.

Generalized hydrodynamics and non-equilibrium steady states in integrable many-body quantum systems

NASA Astrophysics Data System (ADS)

Vasseur, Romain; Bulchandani, Vir; Karrasch, Christoph; Moore, Joel

The long-time dynamics of thermalizing many-body quantum systems can typically be described in terms of a conventional hydrodynamics picture that results from the decay of all but a few slow modes associated with standard conservation laws (such as particle number, energy, or momentum). However, hydrodynamics is expected to fail for integrable systems that are characterized by an infinite number of conservation laws, leading to unconventional transport properties and to complex non-equilibrium states beyond the traditional dogma of statistical mechanics. In this talk, I will describe recent attempts to understand such stationary states far from equilibrium using a generalized hydrodynamics picture. I will discuss the consistency of ``Bethe-Boltzmann'' kinetic equations with linear response Drude weights and with density-matrix renormalization group calculations. This work was supported by the Department of Energy through the Quantum Materials program (R. V.), NSF DMR-1206515, AFOSR MURI and a Simons Investigatorship (J. E. M.), DFG through the Emmy Noether program KA 3360/2-1 (C. K.).

Phase space theory of evaporation in neon clusters: the role of quantum effects.

PubMed

Calvo, F; Parneix, P

2009-12-31

Unimolecular evaporation of neon clusters containing between 14 and 148 atoms is theoretically investigated in the framework of phase space theory. Quantum effects are incorporated in the vibrational densities of states, which include both zero-point and anharmonic contributions, and in the possible tunneling through the centrifugal barrier. The evaporation rates, kinetic energy released, and product angular momentum are calculated as a function of excess energy or temperature in the parent cluster and compared to the classical results. Quantum fluctuations are found to generally increase both the kinetic energy released and the angular momentum of the product, but the effects on the rate constants depend nontrivially on the excess energy. These results are interpreted as due to the very few vibrational states available in the product cluster when described quantum mechanically. Because delocalization also leads to much narrower thermal energy distributions, the variations of evaporation observables as a function of canonical temperature appear much less marked than in the microcanonical ensemble. While quantum effects tend to smooth the caloric curve in the product cluster, the melting phase change clearly keeps a signature on these observables. The microcanonical temperature extracted from fitting the kinetic energy released distribution using an improved Arrhenius form further suggests a backbending in the quantum Ne(13) cluster that is absent in the classical system. Finally, in contrast to delocalization effects, quantum tunneling through the centrifugal barrier does not play any appreciable role on the evaporation kinetics of these rather heavy clusters.

Coherent and conventional gravidynamic quantum 1/f noise

NASA Astrophysics Data System (ADS)

Handel, Peter H.; George, Thomas F.

2008-04-01

Quantum 1/f noise is a fundamental fluctuation of currents, physical cross sections or process rates, caused by infrared coupling of the current carriers to very low frequency (soft) quanta, also known as infraquanta. The latter are soft gravitons in the gravidynamic case with the coupling constant g= pGM2/Nch considered here -- soft photons in the electrodynamic case and soft transversal piezo-phonons in the lattice-dynamical case. Here p=3.14 and F=psi. Quantum 1/f noise is a new aspect of quantum mechanics expressed mainly through the coherent quantum 1/f effect 2g/pf derived here for large systems, and mainly through the conventional quantum 1/f effect for small systems or individual particles. Both effects are present in general, and their effects are superposed in a first approximation with the help of a coherence (weight) parameter s" that will be derived elsewhere for the gravitational case. The spectral density of fractional fluctuations S(dj/j,f) for j=e(hk/2pm)|F|2 is S(F2,f)/<|F|2> = S(j,f)/2 = [4ps"/(1+s")]GM2/pfNch = 4.4 10E9 M2/(pfNgram2). Here s" = 2N'GM/c2=N'rs, where N' is the number of particles of mass M per unit length of the current, rs their Schwarzschild radius, and s" is our coherence (weight) parameter giving the ratio of coherent to conventional quantum 1/f contributions.

Photonics of 2D gold nanolayers on sapphire surface

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

Muslimov, A. E., E-mail: amuslimov@mail.ru; Butashin, A. V.; Nabatov, B. V.

Gold layers with thicknesses of up to several nanometers, including ordered and disordered 2D nanostructures of gold particles, have been formed on sapphire substrates; their morphology is described; and optical investigations are carried out. The possibility of increasing the accuracy of predicting the optical properties of gold layers and 2D nanostructures using quantum-mechanical models based on functional density theory calculation techniques is considered. The application potential of the obtained materials in photonics is estimated.

Towards A Predictive First Principles Understanding Of Molecular Adsorption On Graphene

DTIC Science & Technology

2016-10-05

used and developed state-of-the-art quantum mechanical methods to make accurate predictions about the interaction strength and adsorption structure...density functional theory, ab initio methods 16.  SECURITY CLASSIFICATION OF: 17.  LIMITATION OF ABSTRACT SAR 18.  NUMBER OF PAGES   11   19a.  NAME OF...important physical properties for a whole class of systems with weak non-covalent interactions, for example those involving the binding between water

Designing New Materials for Converting Solar Energy to Fuels via Quantum Mechanics

DTIC Science & Technology

2014-07-11

dopants can also be exploited to increase charge carrier concentration without creating traps and hence improve the conductivity of these materials...e.g., Mn(II) in hematite for hole transport, Y(III) in MnO:ZnO for electron transport). • We discovered that dopants derived from covalent oxides...e.g., Si from silica, as a dopant in hematite) can also be used to increase charge carrier density without creating traps. Charge carriers stay

Efficient Multi-Dimensional Simulation of Quantum Confinement Effects in Advanced MOS Devices

NASA Technical Reports Server (NTRS)

Biegel, Bryan A.; Rafferty, Conor S.; Ancona, Mario G.; Yu, Zhi-Ping

2000-01-01

We investigate the density-gradient (DG) transport model for efficient multi-dimensional simulation of quantum confinement effects in advanced MOS devices. The formulation of the DG model is described as a quantum correction to the classical drift-diffusion model. Quantum confinement effects are shown to be significant in sub-100nm MOSFETs. In thin-oxide MOS capacitors, quantum effects may reduce gate capacitance by 25% or more. As a result, the inclusion or quantum effects in simulations dramatically improves the match between C-V simulations and measurements for oxide thickness down to 2 nm. Significant quantum corrections also occur in the I-V characteristics of short-channel (30 to 100 nm) n-MOSFETs, with current drive reduced by up to 70%. This effect is shown to result from reduced inversion charge due to quantum confinement of electrons in the channel. Also, subthreshold slope is degraded by 15 to 20 mV/decade with the inclusion of quantum effects via the density-gradient model, and short channel effects (in particular, drain-induced barrier lowering) are noticeably increased.

First-Principles Studies of Structure-Property Relationships: Enabling Design of Functional Materials

NASA Astrophysics Data System (ADS)

Zhou, Qunfei

First-principles calculations based on quantum mechanics have been proved to be powerful for accurately regenerating experimental results, uncovering underlying myths of experimental phenomena, and accelerating the design of innovative materials. This work has been motivated by the demand to design next-generation thermionic emitting cathodes and techniques to allow for synthesis of photo-responsive polymers on complex surfaces with controlled thickness and patterns. For Os-coated tungsten thermionic dispenser cathodes, we used first-principles methods to explore the bulk and surface properties of W-Os alloys in order to explain the previously observed experimental phenomena that thermionic emission varies significantly with W-Os alloy composition. Meanwhile, we have developed a new quantum mechanical approach to quantitatively predict the thermionic emission current density from materials perspective without any semi-empirical approximations or complicated analytical models, which leads to better understanding of thermionic emission mechanism. The methods from this work could be used to accelerate the design of next-generation thermionic cathodes. For photoresponsive materials, we designed a novel type of azobenzene-containing monomer for light-mediated ring-opening metathesis polymerization (ROMP) toward the fabrication of patterned, photo-responsive polymers by controlling ring strain energy (RSE) of the monomer that drives ROMP. This allows for unprecedented remote, noninvasive, instantaneous spatial and temporal control of photo-responsive polymer deposition on complex surfaces.This work on the above two different materials systems showed the power of quantum mechanical calculations on predicting, understanding and discovering the structures and properties of both known and unknown materials in a fast, efficient and reliable way.

Construction of exchange repulsion in terms of the wave functions at QM/MM boundary region

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

Takahashi, Hideaki, E-mail: hideaki@m.tohoku.ac.jp; Umino, Satoru; Morita, Akihiro

2015-08-28

We developed a simple method to calculate exchange repulsion between a quantum mechanical (QM) solute and a molecular mechanical (MM) molecule in the QM/MM approach. In our method, the size parameter in the Buckingham type potential for the QM solute is directly determined in terms of the one-electron wave functions of the solute. The point of the method lies in the introduction of the exchange core function (ECF) defined as a Slater function which mimics the behavior of the exterior electron density at the QM/MM boundary region. In the present paper, the ECF was constructed in terms of the Becke-Rousselmore » (BR) exchange hole function. It was demonstrated that the ECF yielded by the BR procedure can faithfully reproduce the radial behavior of the electron density of a QM solute. The size parameter of the solute as well as the exchange repulsion are, then, obtained using the overlap model without any fitting procedure. To examine the efficiency of the method, it was applied to calculation of the exchange repulsions for minimal QM/MM systems, hydrogen-bonded water dimer, and H{sub 3}O{sup +}–H{sub 2}O. We found that our approach is able to reproduce the potential energy curves for these systems showing reasonable agreements with those given by accurate full quantum chemical calculations.« less

Improving students' understanding of quantum mechanics

NASA Astrophysics Data System (ADS)

Zhu, Guangtian

2011-12-01

Learning physics is challenging at all levels. Students' difficulties in the introductory level physics courses have been widely studied and many instructional strategies have been developed to help students learn introductory physics. However, research shows that there is a large diversity in students' preparation and skills in the upper-level physics courses and it is necessary to provide scaffolding support to help students learn advanced physics. This thesis explores issues related to students' common difficulties in learning upper-level undergraduate quantum mechanics and how these difficulties can be reduced by research-based learning tutorials and peer instruction tools. We investigated students' difficulties in learning quantum mechanics by administering written tests and surveys to many classes and conducting individual interviews with a subset of students. Based on these investigations, we developed Quantum Interactive Learning Tutorials (QuILTs) and peer instruction tools to help students build a hierarchical knowledge structure of quantum mechanics through a guided approach. Preliminary assessments indicate that students' understanding of quantum mechanics is improved after using the research-based learning tools in the junior-senior level quantum mechanics courses. We also designed a standardized conceptual survey that can help instructors better probe students' understanding of quantum mechanics concepts in one spatial dimension. The validity and reliability of this quantum mechanics survey is discussed.

Quantum percolation phase transition and magnetoelectric dipole glass in hexagonal ferrites

NASA Astrophysics Data System (ADS)

Rowley, S. E.; Vojta, T.; Jones, A. T.; Guo, W.; Oliveira, J.; Morrison, F. D.; Lindfield, N.; Baggio Saitovitch, E.; Watts, B. E.; Scott, J. F.

2017-07-01

Hexagonal ferrites not only have enormous commercial impact (£2 billion/year in sales) due to applications that include ultrahigh-density memories, credit-card stripes, magnetic bar codes, small motors, and low-loss microwave devices, they also have fascinating magnetic and ferroelectric quantum properties at low temperatures. Here we report the results of tuning the magnetic ordering temperature in PbF e12 -xG axO19 to zero by chemical substitution x . The phase transition boundary is found to vary as TN˜(1-x /xc ) 2 /3 with xc very close to the calculated spin percolation threshold, which we determine by Monte Carlo simulations, indicating that the zero-temperature phase transition is geometrically driven. We find that this produces a form of compositionally tuned, insulating, ferrimagnetic quantum criticality. Close to the zero-temperature phase transition, we observe the emergence of an electric dipole glass induced by magnetoelectric coupling. The strong frequency behavior of the glass freezing temperature Tm has a Vogel-Fulcher dependence with Tm finite, or suppressed below zero in the zero-frequency limit, depending on composition x . These quantum-mechanical properties, along with the multiplicity of low-lying modes near the zero-temperature phase transition, are likely to greatly extend applications of hexaferrites into the realm of quantum and cryogenic technologies.

Tuning electronic properties in graphene quantum dots by chemical functionalization: Density functional theory calculations

NASA Astrophysics Data System (ADS)

Abdelsalam, Hazem; Elhaes, Hanan; Ibrahim, Medhat A.

2018-03-01

The energy gap and dipole moment of chemically functionalized graphene quantum dots are investigated by density functional theory. The energy gap can be tuned through edge passivation by different elements or groups. Edge passivation by oxygen considerably decreases the energy gap in hexagonal nanodots. Edge states in triangular quantum dots can also be manipulated by passivation with fluorine. The dipole moment depends on: (a) shape and edge termination of the quantum dot, (b) attached group, and (c) position to which the groups are attached. Depending on the position of attached groups, the total dipole can be increased, decreased, or eliminated.

Using hyperentanglement to enhance resolution, signal-to-noise ratio, and measurement time

NASA Astrophysics Data System (ADS)

Smith, James F.

2017-03-01

A hyperentanglement-based atmospheric imaging/detection system involving only a signal and an ancilla photon will be considered for optical and infrared frequencies. Only the signal photon will propagate in the atmosphere and its loss will be classical. The ancilla photon will remain within the sensor experiencing low loss. Closed form expressions for the wave function, normalization, density operator, reduced density operator, symmetrized logarithmic derivative, quantum Fisher information, quantum Cramer-Rao lower bound, coincidence probabilities, probability of detection, probability of false alarm, probability of error after M measurements, signal-to-noise ratio, quantum Chernoff bound, time-on-target expressions related to probability of error, and resolution will be provided. The effect of noise in every mode will be included as well as loss. The system will provide the basic design for an imaging/detection system functioning at optical or infrared frequencies that offers better than classical angular and range resolution. Optimization for enhanced resolution will be included. The signal-to-noise ratio will be increased by a factor equal to the number of modes employed during the hyperentanglement process. Likewise, the measurement time can be reduced by the same factor. The hyperentanglement generator will typically make use of entanglement in polarization, energy-time, orbital angular momentum and so on. Mathematical results will be provided describing the system's performance as a function of loss mechanisms and noise.

Quantum molecular dynamics simulations of dense matter

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

Collins, L.; Kress, J.; Troullier, N.

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,more » 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.« less

Quantum mechanics as classical statistical mechanics with an ontic extension and an epistemic restriction.

PubMed

Budiyono, Agung; Rohrlich, Daniel

2017-11-03

Where does quantum mechanics part ways with classical mechanics? How does quantum randomness differ fundamentally from classical randomness? We cannot fully explain how the theories differ until we can derive them within a single axiomatic framework, allowing an unambiguous account of how one theory is the limit of the other. Here we derive non-relativistic quantum mechanics and classical statistical mechanics within a common framework. The common axioms include conservation of average energy and conservation of probability current. But two axioms distinguish quantum mechanics from classical statistical mechanics: an "ontic extension" defines a nonseparable (global) random variable that generates physical correlations, and an "epistemic restriction" constrains allowed phase space distributions. The ontic extension and epistemic restriction, with strength on the order of Planck's constant, imply quantum entanglement and uncertainty relations. This framework suggests that the wave function is epistemic, yet it does not provide an ontic dynamics for individual systems.

A hybrid approach to simulation of electron transfer in complex molecular systems

PubMed Central

Kubař, Tomáš; Elstner, Marcus

2013-01-01

Electron transfer (ET) reactions in biomolecular systems represent an important class of processes at the interface of physics, chemistry and biology. The theoretical description of these reactions constitutes a huge challenge because extensive systems require a quantum-mechanical treatment and a broad range of time scales are involved. Thus, only small model systems may be investigated with the modern density functional theory techniques combined with non-adiabatic dynamics algorithms. On the other hand, model calculations based on Marcus's seminal theory describe the ET involving several assumptions that may not always be met. We review a multi-scale method that combines a non-adiabatic propagation scheme and a linear scaling quantum-chemical method with a molecular mechanics force field in such a way that an unbiased description of the dynamics of excess electron is achieved and the number of degrees of freedom is reduced effectively at the same time. ET reactions taking nanoseconds in systems with hundreds of quantum atoms can be simulated, bridging the gap between non-adiabatic ab initio simulations and model approaches such as the Marcus theory. A major recent application is hole transfer in DNA, which represents an archetypal ET reaction in a polarizable medium. Ongoing work focuses on hole transfer in proteins, peptides and organic semi-conductors. PMID:23883952

Quantum mechanical model for the anticarcinogenic effect of extremely-low-frequency electromagnetic fields on early chemical hepatocarcinogenesis

NASA Astrophysics Data System (ADS)

Godina-Nava, Juan José; Torres-Vega, Gabino; López-Riquelme, Germán Octavio; López-Sandoval, Eduardo; Samana, Arturo Rodolfo; García Velasco, Fermín; Hernández-Aguilar, Claudia; Domínguez-Pacheco, Arturo

2017-02-01

Using the conventional Haberkorn approach, it is evaluated the recombination of the radical pair (RP) singlet spin state to study theoretically the cytoprotective effect of an extremely-low-frequency electromagnetic field (ELF-EMF) on early stages of hepatic cancer chemically induced in rats. The proposal is that ELF-EMF modulates the interconversion rate of singlet and triplet spin states of the RP populations modifying the products from the metabolization of carcinogens. Previously, we found that the daily treatment with ELF-EMF 120 Hz inhibited the number and area of preneoplastic lesions in chemical carcinogenesis. The singlet spin population is evaluated diagonalizing the spin density matrix through the Lanczos method in a radical pair mechanism (RPM). Using four values of the interchange energy, we have studied the variations over the singlet population. The low magnetic field effect as a test of the influence over the enzymatic chemical reaction is evaluated calculating the quantum yield. Through a bootstrap technique the range is found for the singlet decay rate for the process. Applying the quantum measurements concept, we addressed the impact toward hepatic cells. The result contributes to improving our understanding of the chemical carcinogenesis process affected by charged particles that damage the DNA.

Influence of metal cofactors and water on the catalytic mechanism of creatininase-creatinine in aqueous solution from molecular dynamics simulation and quantum study

NASA Astrophysics Data System (ADS)

Lee, Vannajan Sanghiran; Kodchakorn, Kanchanok; Jitonnom, Jitrayut; Nimmanpipug, Piyarat; Kongtawelert, Prachya; Premanode, Bhusana

2010-10-01

The reaction mechanism of creatinine-creatininase binding to form creatine as a final product has been investigated by using a combined ab initio quantum mechanical/molecular mechanical approach and classical molecular dynamics (MD) simulations. In MD simulations, an X-ray crystal structure of the creatininase/creatinine was modified for creatininase/creatinine complexes and the MD simulations were run for free creatininase and creatinine in water. MD results reveal that two X-ray water molecules can be retained in the active site as catalytic water. The binding free energy from Molecular Mechanics Poisson-Boltzmann Surface Area calculation predicted the strong binding of creatinine with Zn2+, Asp45 and Glu183. Two step mechanisms via Mn2+/Zn2+ (as in X-ray structure) and Zn2+/Zn2+ were proposed for water adding step and ring opening step with two catalytic waters. The pathway using synchronous transit methods with local density approximations with PWC functional for the fragment in the active region were obtained. Preferable pathway Zn2+/Zn2+ was observed due to lower activation energy in water adding step. The calculated energy in the second step for both systems were comparable with the barrier of 26.03 and 24.44 kcal/mol for Mn2+/Zn2+ and Zn2+/Zn2+, respectively.

Impact of threading dislocation density on the lifetime of InAs quantum dot lasers on Si

NASA Astrophysics Data System (ADS)

Jung, Daehwan; Herrick, Robert; Norman, Justin; Turnlund, Katherine; Jan, Catherine; Feng, Kaiyin; Gossard, Arthur C.; Bowers, John E.

2018-04-01

We investigate the impact of threading dislocation density on the reliability of 1.3 μm InAs quantum dot lasers epitaxially grown on Si. A reduction in the threading dislocation density from 2.8 × 108 cm-2 to 7.3 × 106 cm-2 has improved the laser lifetime by about five orders of magnitude when aged continuous-wave near room temperature (35 °C). We have achieved extrapolated lifetimes (time to double initial threshold) more than 10 × 106 h. An accelerated laser aging test at an elevated temperature (60 °C) reveals that p-modulation doped quantum dot lasers on Si retain superior reliability over unintentionally doped ones. These results suggest that epitaxially grown quantum dot lasers could be a viable approach to realize a reliable, scalable, and efficient light source on Si.

Transmission and reflection of charge-density wave packets in a quantum Hall edge controlled by a metal gate

NASA Astrophysics Data System (ADS)

Matsuura, Masahiro; Mano, Takaaki; Noda, Takeshi; Shibata, Naokazu; Hotta, Masahiro; Yusa, Go

2018-02-01

Quantum energy teleportation (QET) is a proposed protocol related to quantum vacuum. The edge channels in a quantum Hall system are well suited for the experimental verification of QET. For this purpose, we examine a charge-density wave packet excited and detected by capacitively coupled front gate electrodes. We observe the waveform of the charge packet, which is proportional to the time derivative of the applied square voltage wave. Further, we study the transmission and reflection behaviors of the charge-density wave packet by applying a voltage to another front gate electrode to control the path of the edge state. We show that the threshold voltages where the dominant direction is switched in either transmission or reflection for dense and sparse wave packets are different from the threshold voltage where the current stops flowing in an equilibrium state.

Quantum time crystal by decoherence: Proposal with an incommensurate charge density wave ring

NASA Astrophysics Data System (ADS)

Nakatsugawa, K.; Fujii, T.; Tanda, S.

2017-09-01

We show that time translation symmetry of a ring system with a macroscopic quantum ground state is broken by decoherence. In particular, we consider a ring-shaped incommensurate charge density wave (ICDW ring) threaded by a fluctuating magnetic flux: the Caldeira-Leggett model is used to model the fluctuating flux as a bath of harmonic oscillators. We show that the charge density expectation value of a quantized ICDW ring coupled to its environment oscillates periodically. The Hamiltonians considered in this model are time independent unlike "Floquet time crystals" considered recently. Our model forms a metastable quantum time crystal with a finite length in space and in time.

Quantum quenches and work distributions in ultralow-density systems.

PubMed

Shchadilova, Yulia E; Ribeiro, Pedro; Haque, Masudul

2014-02-21

We present results on quantum quenches in lattice systems with a fixed number of particles in a much larger number of sites. Both local and global quenches in this limit generically have power-law work distributions ("edge singularities"). We show that this regime allows for large edge singularity exponents beyond that allowed by the constraints of the usual thermodynamic limit. This large-exponent singularity has observable consequences in the time evolution, leading to a distinct intermediate power-law regime in time. We demonstrate these results first using local quantum quenches in a low-density Kondo-like system, and additionally through global and local quenches in Bose-Hubbard, Aubry-Andre, and hard-core boson systems at low densities.

Generation of mechanical interference fringes by multi-photon counting

NASA Astrophysics Data System (ADS)

Ringbauer, M.; Weinhold, T. J.; Howard, L. A.; White, A. G.; Vanner, M. R.

2018-05-01

Exploring the quantum behaviour of macroscopic objects provides an intriguing avenue to study the foundations of physics and to develop a suite of quantum-enhanced technologies. One prominent path of study is provided by quantum optomechanics which utilizes the tools of quantum optics to control the motion of macroscopic mechanical resonators. Despite excellent recent progress, the preparation of mechanical quantum superposition states remains outstanding due to weak coupling and thermal decoherence. Here we present a novel optomechanical scheme that significantly relaxes these requirements allowing the preparation of quantum superposition states of motion of a mechanical resonator by exploiting the nonlinearity of multi-photon quantum measurements. Our method is capable of generating non-classical mechanical states without the need for strong single-photon coupling, is resilient against optical loss, and offers more favourable scaling against initial mechanical thermal occupation than existing schemes. Moreover, our approach allows the generation of larger superposition states by projecting the optical field onto NOON states. We experimentally demonstrate this multi-photon-counting technique on a mechanical thermal state in the classical limit and observe interference fringes in the mechanical position distribution that show phase super-resolution. This opens a feasible route to explore and exploit quantum phenomena at a macroscopic scale.

Support for the existence of invertible maps between electronic densities and non-analytic 1-body external potentials in non-relativistic time-dependent quantum mechanics

NASA Astrophysics Data System (ADS)

Mosquera, Martín A.

2017-10-01

Provided the initial state, the Runge-Gross theorem establishes that the time-dependent (TD) external potential of a system of non-relativistic electrons determines uniquely their TD electronic density, and vice versa (up to a constant in the potential). This theorem requires the TD external potential and density to be Taylor-expandable around the initial time of the propagation. This paper presents an extension without this restriction. Given the initial state of the system and evolution of the density due to some TD scalar potential, we show that a perturbative (not necessarily weak) TD potential that induces a non-zero divergence of the external force-density, inside a small spatial subset and immediately after the initial propagation time, will cause a change in the density within that subset, implying that the TD potential uniquely determines the TD density. In this proof, we assume unitary evolution of wavefunctions and first-order differentiability (which does not imply analyticity) in time of the internal and external force-densities, electronic density, current density, and their spatial derivatives over the small spatial subset and short time interval.

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

Kelly, Kevin J.; Parke, Stephen J.

Quantum mechanical interactions between neutrinos and matter along the path of propagation, the Wolfenstein matter effect, are of particular importance for the upcoming long-baseline neutrino oscillation experiments, specifically the Deep Underground Neutrino Experiment (DUNE). Here, we explore specifically what about the matter density profile can be measured by DUNE, considering both the shape and normalization of the profile between the neutrinos' origin and detection. Additionally, we explore the capability of a perturbative method for calculating neutrino oscillation probabilities and whether this method is suitable for DUNE. We also briefly quantitatively explore the ability of DUNE to measure the Earth's mattermore » density, and the impact of performing this measurement on measuring standard neutrino oscillation parameters.« less

Computation of the asymptotic states of modulated open quantum systems with a numerically exact realization of the quantum trajectory method

NASA Astrophysics Data System (ADS)

Volokitin, V.; Liniov, A.; Meyerov, I.; Hartmann, M.; Ivanchenko, M.; Hänggi, P.; Denisov, S.

2017-11-01

Quantum systems out of equilibrium are presently a subject of active research, both in theoretical and experimental domains. In this work, we consider time-periodically modulated quantum systems that are in contact with a stationary environment. Within the framework of a quantum master equation, the asymptotic states of such systems are described by time-periodic density operators. Resolution of these operators constitutes a nontrivial computational task. Approaches based on spectral and iterative methods are restricted to systems with the dimension of the hosting Hilbert space dim H =N ≲300 , while the direct long-time numerical integration of the master equation becomes increasingly problematic for N ≳400 , especially when the coupling to the environment is weak. To go beyond this limit, we use the quantum trajectory method, which unravels the master equation for the density operator into a set of stochastic processes for wave functions. The asymptotic density matrix is calculated by performing a statistical sampling over the ensemble of quantum trajectories, preceded by a long transient propagation. We follow the ideology of event-driven programming and construct a new algorithmic realization of the method. The algorithm is computationally efficient, allowing for long "leaps" forward in time. It is also numerically exact, in the sense that, being given the list of uniformly distributed (on the unit interval) random numbers, {η1,η2,...,ηn} , one could propagate a quantum trajectory (with ηi's as norm thresholds) in a numerically exact way. By using a scalable N -particle quantum model, we demonstrate that the algorithm allows us to resolve the asymptotic density operator of the model system with N =2000 states on a regular-size computer cluster, thus reaching the scale on which numerical studies of modulated Hamiltonian systems are currently performed.

Computation of the asymptotic states of modulated open quantum systems with a numerically exact realization of the quantum trajectory method.

PubMed

Volokitin, V; Liniov, A; Meyerov, I; Hartmann, M; Ivanchenko, M; Hänggi, P; Denisov, S

2017-11-01

Quantum systems out of equilibrium are presently a subject of active research, both in theoretical and experimental domains. In this work, we consider time-periodically modulated quantum systems that are in contact with a stationary environment. Within the framework of a quantum master equation, the asymptotic states of such systems are described by time-periodic density operators. Resolution of these operators constitutes a nontrivial computational task. Approaches based on spectral and iterative methods are restricted to systems with the dimension of the hosting Hilbert space dimH=N≲300, while the direct long-time numerical integration of the master equation becomes increasingly problematic for N≳400, especially when the coupling to the environment is weak. To go beyond this limit, we use the quantum trajectory method, which unravels the master equation for the density operator into a set of stochastic processes for wave functions. The asymptotic density matrix is calculated by performing a statistical sampling over the ensemble of quantum trajectories, preceded by a long transient propagation. We follow the ideology of event-driven programming and construct a new algorithmic realization of the method. The algorithm is computationally efficient, allowing for long "leaps" forward in time. It is also numerically exact, in the sense that, being given the list of uniformly distributed (on the unit interval) random numbers, {η_{1},η_{2},...,η_{n}}, one could propagate a quantum trajectory (with η_{i}'s as norm thresholds) in a numerically exact way. By using a scalable N-particle quantum model, we demonstrate that the algorithm allows us to resolve the asymptotic density operator of the model system with N=2000 states on a regular-size computer cluster, thus reaching the scale on which numerical studies of modulated Hamiltonian systems are currently performed.

Are quantum-mechanical-like models possible, or necessary, outside quantum physics?

NASA Astrophysics Data System (ADS)

Plotnitsky, Arkady

2014-12-01

This article examines some experimental conditions that invite and possibly require recourse to quantum-mechanical-like mathematical models (QMLMs), models based on the key mathematical features of quantum mechanics, in scientific fields outside physics, such as biology, cognitive psychology, or economics. In particular, I consider whether the following two correlative features of quantum phenomena that were decisive for establishing the mathematical formalism of quantum mechanics play similarly important roles in QMLMs elsewhere. The first is the individuality and discreteness of quantum phenomena, and the second is the irreducibly probabilistic nature of our predictions concerning them, coupled to the particular character of the probabilities involved, as different from the character of probabilities found in classical physics. I also argue that these features could be interpreted in terms of a particular form of epistemology that suspends and even precludes a causal and, in the first place, realist description of quantum objects and processes. This epistemology limits the descriptive capacity of quantum theory to the description, classical in nature, of the observed quantum phenomena manifested in measuring instruments. Quantum mechanics itself only provides descriptions, probabilistic in nature, concerning numerical data pertaining to such phenomena, without offering a physical description of quantum objects and processes. While QMLMs share their use of the quantum-mechanical or analogous mathematical formalism, they may differ by the roles, if any, the two features in question play in them and by different ways of interpreting the phenomena they considered and this formalism itself. This article will address those differences as well.

Holographic description of a quantum black hole on a computer

NASA Astrophysics Data System (ADS)

Hanada, Masanori; Hyakutake, Yoshifumi; Ishiki, Goro; Nishimura, Jun

2014-05-01

Black holes have been predicted to radiate particles and eventually evaporate, which has led to the information loss paradox and implies that the fundamental laws of quantum mechanics may be violated. Superstring theory, a consistent theory of quantum gravity, provides a possible solution to the paradox if evaporating black holes can actually be described in terms of standard quantum mechanical systems, as conjectured from the theory. Here, we test this conjecture by calculating the mass of a black hole in the corresponding quantum mechanical system numerically. Our results agree well with the prediction from gravity theory, including the leading quantum gravity correction. Our ability to simulate black holes offers the potential to further explore the yet mysterious nature of quantum gravity through well-established quantum mechanics.

Fundamental Study on Quantum Nanojets

DTIC Science & Technology

2004-08-01

Pergamon Press. Bell , J. S . 1966 On the problem of hidden variables in quantum mechanics. Rev. of Modern Phys., 38, 447. Berndl, K., Daumer, M...fluid dynamics based on two quantum mechanical perspectives; Schrödinger’s wave mechanics and quantum fluid dynamics based on Hamilton-Jacoby...References 8 2). Direct Problems a). Quantum fluid dynamics formalism based on Hamilton-Jacoby equation are adapted for the numerical

Increasing phytoplankton-available phosphorus and inhibition of macrophyte on phytoplankton bloom.

PubMed

Dai, Yanran; Wu, Juan; Ma, Xiaohang; Zhong, Fei; Cui, Naxin; Cheng, Shuiping

2017-02-01

We assembled mesocosms to address the coherent mechanisms that an increasing phosphorus (P) concentration in water columns coupled with the phytoplankton bloom and identify the performance gap of regulating phytoplankton growth between two macrophyte species, Ceratophyllum demersum L. and Vallisneria spiralis L. Intense alkaline phosphatase activities (APA) were observed in the unplanted control, with their predominant part, phytoplankton APA (accounting for up to 44.7% of the total APA), and another large share, bacterial APA. These correspond with the large average concentration of total phosphorus (TP), total dissolved phosphorus (TDP) and soluble reactive (SRP) as well as high phytoplankton density in the water column. The consistency among P concentrations, phytoplankton density and APA, together with the positive impact of phytoplankton density on total APA revealed by the structural equation modelling (SEM), indicates that facilitated APA levels in water is an essential strategy for phytoplankton to enhance the available P. Furthermore, a positive interaction between phytoplankton APA and bacteria APA was detected, suggesting a potential collaboration between phytoplankton and bacteria to boost available P content in the water column. Both macrophyte species had a prominent performance on regulating phytoplankton proliferation. The phytoplankton density and quantum yield in C. demersum systems were all significantly lower (33.8% and 24.0%) than those in V. spiralis systems. Additionally, a greater decoupling effect of C. demersum on the relationship between P, APA, phytoplankton density, bacteria dynamic and quantum yield was revealed by SEM. These results imply that the preferred tactic of different species could lead to the performance gap. Copyright © 2016 Elsevier B.V. All rights reserved.

Spin relaxation in n-type GaAs quantum wells from a fully microscopic approach

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

Zhou, J.; Wu, M. W.; Department of Physics, University of Science and Technology of China, Hefei, Anhui 230026

2007-01-15

We perform a full microscopic investigation on the spin relaxation in n-type (001) GaAs quantum wells with an Al{sub 0.4}Ga{sub 0.6}As barrier due to the D'yakonov-Perel' mechanism from nearly 20 K to room temperature by constructing and numerically solving the kinetic spin Bloch equations. We consider all the relevant scattering such as the electron-acoustic-phonon, the electron-longitudinal-optical-phonon, the electron-nonmagnetic-impurity, and the electron-electron Coulomb scattering to the spin relaxation. The spin relaxation times calculated from our theory with a fitting spin splitting parameter are in good agreement with the experimental data by Ohno et al. [Physica E (Amsterdam) 6, 817 (2000)] overmore » the whole temperature regime (from 20 to 300 K). The value of the fitted spin splitting parameter agrees with many experiments and theoretical calculations. We further show the temperature dependence of the spin relaxation time under various conditions such as electron density, impurity density, and well width. We predict a peak solely due to the Coulomb scattering in the spin relaxation time at low temperature (<50 K) in samples with low electron density (e.g., density less than 1x10{sup 11} cm{sup -2}) but high mobility. This peak disappears in samples with high electron density (e.g., 2x10{sup 11} cm{sup -2}) and/or low mobility. The hot-electron spin kinetics at low temperature is also addressed with many features quite different from the high-temperature case predicted.« less

Faithful conversion of propagating quantum information to mechanical motion

NASA Astrophysics Data System (ADS)

Reed, A. P.; Mayer, K. H.; Teufel, J. D.; Burkhart, L. D.; Pfaff, W.; Reagor, M.; Sletten, L.; Ma, X.; Schoelkopf, R. J.; Knill, E.; Lehnert, K. W.

2017-12-01

The motion of micrometre-sized mechanical resonators can now be controlled and measured at the fundamental limits imposed by quantum mechanics. These resonators have been prepared in their motional ground state or in squeezed states, measured with quantum-limited precision, and even entangled with microwave fields. Such advances make it possible to process quantum information using the motion of a macroscopic object. In particular, recent experiments have combined mechanical resonators with superconducting quantum circuits to frequency-convert, store and amplify propagating microwave fields. But these systems have not been used to manipulate states that encode quantum bits (qubits), which are required for quantum communication and modular quantum computation. Here we demonstrate the conversion of propagating qubits encoded as superpositions of zero and one photons to the motion of a micromechanical resonator with a fidelity in excess of the classical bound. This ability is necessary for mechanical resonators to convert quantum information between the microwave and optical domains or to act as storage elements in a modular quantum information processor. Additionally, these results are an important step towards testing speculative notions that quantum theory may not be valid for sufficiently massive systems.

Efficient Multi-Dimensional Simulation of Quantum Confinement Effects in Advanced MOS Devices

NASA Technical Reports Server (NTRS)

Biegel, Bryan A.; Ancona, Mario G.; Rafferty, Conor S.; Yu, Zhiping

2000-01-01

We investigate the density-gradient (DG) transport model for efficient multi-dimensional simulation of quantum confinement effects in advanced MOS devices. The formulation of the DG model is described as a quantum correction ot the classical drift-diffusion model. Quantum confinement effects are shown to be significant in sub-100nm MOSFETs. In thin-oxide MOS capacitors, quantum effects may reduce gate capacitance by 25% or more. As a result, the inclusion of quantum effects may reduce gate capacitance by 25% or more. As a result, the inclusion of quantum effects in simulations dramatically improves the match between C-V simulations and measurements for oxide thickness down to 2 nm. Significant quantum corrections also occur in the I-V characteristics of short-channel (30 to 100 nm) n-MOSFETs, with current drive reduced by up to 70%. This effect is shown to result from reduced inversion charge due to quantum confinement of electrons in the channel. Also, subthreshold slope is degraded by 15 to 20 mV/decade with the inclusion of quantum effects via the density-gradient model, and short channel effects (in particular, drain-induced barrier lowering) are noticeably increased.